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A0___PPT10 pp___PPT9n^,֋S#ޠ"PNG  IHDRF}sRGB PLTE3*ծ cmPPJCmp0712 7tRNS@f8IDATWc``d !$$<[UBS#B>\`Y{ff` R>&- {p_/̴>?" ddG |?" ddG  Z#" G n j[ n?" dd@   @@``PR  # G  j ` p>n[RR>n[RII B:(    Tk_/k_/ "9F  T Click to edit Master title style! !B  NTk_/k_/ "F-^  RClick to edit Master text styles Second level Third level Fourth level Fifth level!     S  Nk_/k_/ "`Tg  n*@ G ##G G jj  Nжk_/k_/ "`m0Tg   p*@ G ##G G jj  Nk_/k_/ "`U5FTg  p*@ G ##G G jjH  0U<܍ ? 3380___PPT10.Ovp Default DesignB^ ]] p @*](  l J 6Ԕ"`<kJ)[   ``C`CA ?"6@ NNN?N  ~  BA ??KH ~   BA ?? X  TgKgKff "`-G`XP___PPT92* ^ Natural Rubber Filled by Nanosilica: an ESR  Spin Probe Study Leki1, S. Vali1,2, A.P. Meera 3 and S. Thomas3 1 University of Rijeka, School of Medicine, Brae Branchetta 20, Rijeka, 51000, Croatia 2 Rudjer Boakovi Institute, Bijeni ka 54, Zagreb,10000, Croatia 3 Mahatma Gandhi University, School of Chemical Sciences, Kottayam, India - 686 560 Z0?3Y0;*?<, , , , , ,, , V ? R* !        D >T     B`S5G^" `-Am Q Objective (2 6   BS5G^" `V A" Q Materials (2 6   BTS5G^" `AFAH ZSample preparation(26   BT5G^" `- /m OMethods(26   B/S5G^" `) 1bAi" OResults(26    03S^D<4___PPT9 ]Investigation of the NR samples containg different amounts of the nanosilica particles and their influence on local chain dynamics. Influence of a coupling agent on the changes in matrix structure and chain dynamics.@! U! 8X  0@S<$ V& JTable 1. Samples of NR with different amounts of nanosilica"KC Kt nB*]D3 l  #"&<WVWV'aP0 $ TMS_ж_ж? 1]D3 `20 #G j # T4S_ж_ж?n1 D3 fRub.ns20   #G j " T^S_ж_ж? 0]1 `15 #G j ! TWS_ж_ж?n0 1 fRub.ns15   #G j   ToS_ж_ж? 6/]0 `10 #G j  TxS_ж_ж?n6/ 0 fRub.ns10   #G j  TS_ж_ж? -]6/ _0 #G j  T@S_ж_ж?n- 6/ fRub.ns00   #G j(   fS_ж_ж^d?"  B*]- |The amount of nanosilica / phr #G j   fXS_ж_ж5d?" nB* - e sample #G jZB ' s *> ?n6/]6/ZB ( s *> ?n0]0ZB ) s *> ?n1]1ZB , s *> ? B* D3ZB & s *> ?n-]-`B % 0> ?nB*]B*`B + 0> ?nB*nD3`B - 0> ?]B*]D3`B * 0> ?nD3]D3  0Si2 4 @The average diametar of the used nanosilica particles was 13 nm.A 2A A  0S5 A8 RTable 2. NR samples with different amounts of coupling agent (Si 69)"SK S p ^:@C j  #""a$93zA  TS_ж_ж?5 A@C _4 #G j  TS_ж_ж?^A5 @C h Rub.nscp04   #G j  TS_ж_ж?5 @A _2 #G j  TS_ж_ж?^@5 A h Rub.nscp02   #G j  TS_ж_ж?5 >@ _1 #G j  TS_ж_ж?^>5 @ h Rub.nscp01   #G j,   fS_ж_ж^d?" 5 :> "The amount of coupling agent / phr## ##G j   fS_ж_ж5d?" ^:5 > q sample& #G jZB   s *> ?^@@ZB   s *> ?^AAZB   s *> ?5 :5 @CZB   s *> ?^>>`B   0> ?^::`B   0> ?^:^@C`B   0> ?:@C`B   0> ?^@C@C  0T'J{c!QD<4___PPT9 Two-roll mixing folowed by compression moulding. Swelling in the toluene probe solution at the constant temperature (35C). Removing the solvent by evaporationand annealing at 60 C during tree days.6!  8X  0DT0- r.ESR  spin probe method   0T0-; )probe amount in the samples was 0.15 wt%,*# *4  # A ? sNv)sNZB &  s *> ? Ov)OZB '  s *> ? 'Qv)'QZB (  s *> ?&K&VZB )  s *> ? Mv)M`B *  0> ? Kv)K`B +  0> ? K V`B ,  0> ?v)Kv)V`B -  0> ? Vv)VZB 5  s *> ? 5Uv)5UZB :  s *> ? Sv)SZB @  s *> ? Rv)R I 0TDWO/Z \Table 3. The intensities ratio of narrow and wide component of ESR spectra measured at 10C.$] 2U ]  U 0TB E cThe amount of nanosilica in all samples containing the coupling agent was similar and equal 10 phr.d 2d d V 0TT31 BESR spectrometar : Varian E-109 Temperature unit Bruker ER 4111 VTCC Cx f  <A ??17@E#G x n  <A ??l5 #1E ) o 0lTM` e Z. Veksli, M Andreis, B. Rakvin, Prog Polym. Sci. 25 (2000) 949. G. Jeschke et al., Polymer Engineering and Science 44 (2004) 1112. 2 R p 0T_m Eh ESR spectra show a significant influence of nanosilica on the local chain dynamics. The increase in the nanosilica amount leads to the decrease in segmental motions. The coupling agent makes the role of nanosilica more pronounced. 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TWS_ж_ж?n0 1 fRub.ns15   #G j   ToS_ж_ж?  !"#$%&'()*+,-./0123456789:;<=>?@ABCDEFGHIJKLMNOPQRSTUVWXYZ[\]^_`abcdefghijklmnopqrstuvwxyz{|}~      !"#$%&'()*+,-./0123456789:;<=>?@ABCDEFGHIJKLMNOPQRSTUVWXYZ[\]^_`abcdefghijklmnopqrstuvwxyz{|}~      !"#$%&'()*+,-./0123456789:;<=>?@ABCDEFGHIJKLMNOPQRSTUVWXYZ[\]^_`abcdefghijklmnopqrstuvwxyz{|}~      !"#$%&'()*+,-./0123456789:;<=>?@ABCDEFGHIJKLMNOPQRSTUVWXYZ[\]^_`abcdefghijklmnopqrstuvwxyz{|}~      !"#$%&'()*+,-./0123456789:;<=>?@ABCDEFGHIJKLMNOPQRSTUVWXYZ[\]^_`abcdefghijklmnopqrstuvwxyz{|}~      !"#$%&'()*+,-./0123456789:;<=>?@ABCDEFGHIJKLMNOPQRSTUVWXYZ[\]^_`abcdefghijklmnopqrstuvwxyz{|}~      !"#$%&'()*+,-./0123456789:;<=>?@ABCDEFGHIJKLMNOPQRSTUVWXYZ[\]^_`abcdefghijklmnopqrstuvwxyz{|}~      !"#$%&'()*+,-./0123456789:;<=>?@ABCDEFGHIJKLMNOPQRSTUVWXYZ[\]^_`abcdefghijklmnopqrstuvwxyz{|}~      !"#$%&'()*+,-./0123456789:;<=>?@ABCDEFGHIJKLMNOPQRSTUVWXYZ[\]^_`abcdefghijklmnopqrstuvwxyz{|}~                           ! " # $ % & ' ( ) * + , - . / 0 1 2 3 4 5 6 7 8 9 : ; < = > ? @ A B C D E F G H I J K L M N O P Q R S T U V W X Y Z [ \ ] ^ _ ` a b c d e f g h i j k l m n o p q r s t u v w x y z { | } ~                            ! " # $ % & ' ( ) * + , - . / 0 1 2 3 4 5 6 7 8 9 : ; < = > ? @ A B C D E F G H I J K L M N O P Q R S T U V W X Y Z [ \ ] ^ _ ` a b c d e f g h i j k l m n o p q r s t u v w x y z { | } ~                            ! " # $ % & ' ( ) * + , - . / 0 1 2 3 4 5 6 7 8 9 : ; < = > ? @ A B C D E F G H I J K L M N O P Q R S T U V W X Y Z [ \ ] ^ _ ` a b c d e f g h i j k l m n o p q r s t u v w x y z { | } ~                            ! " # $ % & ' ( ) * + , - . / 0 1 2 3 4 5 6 7 8 9 : ; < = > ? @ A B C D E F G H I J K L M N O P Q R S T U V W X Y Z [ \ ] ^ _ ` a b c d e f g h i j k l m n o p q r s t u v w x y z { | } ~                            ! " # $ % & ' ( ) * + - . / 0 1 2 3 4 5 6 7 8 9 : ; < = > ? @ A B C D E F G H I J K L M N O P Q R S T U W X Y Z [ \ ] ^ _ ` a b c d e elDRAW 11.0 Graphic SPW 10.0 Graph 0SigmaPlotGraphicObject.90(SigmaPlot 10.0 Graph SPW 10.0 Graph 0SigmaPlotGraphicObject.90(SigmaPlot 10.0 GraphD/ 0|DArialhA RomanTT3ܖ 0ܖDTimes New RomanTT3ܖ 0ܖ DGaramond RomanTT3ܖ 0ܖ0DSymbold RomanTT3ܖ 0ܖ@DWP MathA RomanTT3ܖ 0ܖ@ . @n?" dd@  @@`` PowerPoint Document(DocumentSummaryInformation8XCorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 Graphic SPW 10.0 Graph 0SigmaPlotGraphicObject.90(SigmaPlot 10.0 Graph SPW 10.0 Graph 0SigmaPlotGraphicObject.90(SigmaPlot 10.0 GraphD/ 0|DArialhA .0z[ 0DTimes New Roman0z[ 0 DGaramond Roman0z[ 00DSymbold Roman0z[ 0@DWP MathA Roman0z[ 0@ . @n?" dd@  @@`` h`P v212$V0,Hw6"$gqN,WGְdEh36"$vHηΈ={>cUH 2$],ֽ4 P R$D<$*q 2$ _s8) \k= 2$Z&$(WkBAc  2$C^g¿pSK;&~ $2$fAζg6K/!m*52$i mD~s2$ : H=>X񭑹Wa $2$RլQ?ER@2$s IHRc 0AAP3@<ʚ;ʚ;g4dd z[ 0@p:@p<<4ddddL 0. A0___PPT10 pp___PPT9n^,֋S#ޠ"PNG  IHDRF}sRGB PLTE3*ծ cmPPJCmp0712 7tRNS@f8IDATWc``d !$$<[UBS#BT     B`S5G^" `-Am Q Objective (2 6   BS5G^" `V A" Q Materials (2 6   BTS5G^" `AFAH ZSample preparation(26   BT5G^" `QA3T OMethods(26   B/S5G^" `) 1bAi" OResults(26    03S^D<4___PPT9 ]Investigation of the NR samples containg different amounts of the nanosilica particles and their influence on local chain dynamics. Influence of a coupling agent on the changes in matrix structure and chain dynamics.@! U! 8X  0@S<$ V& JTable 1. Samples of NR with different amounts of nanosilica"KC Kt nB*]D3 l  #"&<WVWV'aP0 $ TMS_ж_ж? 1]D3 `20 #G j # T4S_ж_ж?n1 D3 fRub.ns20   #G j " T^S_ж_ж? 0]1 `15 #G j ! TWS_ж_ж?n0 1 fRub.ns15   #G j   ToS_ж_ж? 6/]0 `10 #G j  TxS_ж_ж?n6/ 0 fRub.ns10   #G j  TS_ж_ж? -]6/ _0 #G j  T@S_ж_ж?n- 6/ fRub.ns00   #G j(   fS_ж_ж^d?"  B*]- |The amount of nanosilica / phr #G j   fXS_ж_ж5d?" nB* - e sample #G jZB ' s *> ?n6/]6/ZB ( s *> ?n0]0ZB ) s *> ?n1]1ZB , s *> ? B* D3ZB & s *> ?n-]-`B % 0> ?nB*]B*`B + 0> ?nB*nD3`B - 0> ?]B*]D3`B * 0> ?nD3]D3  0Si2 4 @The average diametar of the used nanosilica particles was 13 nm.A 2A A  0S5 A8 RTable 2. NR samples with different amounts of coupling agent (Si 69)"SK S p ^:@C j  #""a$93zA  TS_ж_ж?5 A@C _4 #G j  TS_ж_ж?^A5 @C h Rub.nscp04   #G j  TS_ж_ж?5 @A _2 #G j  TS_ж_ж?^@5 A h Rub.nscp02   #G j  TS_ж_ж?5 >@ _1 #G j  TS_ж_ж?^>5 @ h Rub.nscp01   #G j,   fS_ж_ж^d?" 5 :> "The amount of coupling agent / phr## ##G j   fS_ж_ж5d?" ^:5 > q sample& #G jZB   s *> ?^@@ZB   s *> ?^AAZB   s *> ?5 :5 @CZB   s *> ?^>>`B   0> ?^::`B   0> ?^:^@C`B   0> ?:@C`B   0> ?^@C@C  0T'J{c!QD<4___PPT9 Two-roll mixing folowed by compression moulding. Swelling in the toluene probe solution at the constant temperature (35C). Removing the solvent by evaporationand annealing at 60 C during tree days.6!  8X  0DTV`W r.ESR  spin probe method   0TXV[ )probe amount in the samples was 0.15 wt%,*# *4  # AR%[  0("T[< ] ,4-hydroy-2,2,6,6-tetramethylpiperidin-1-oxyl- 2- # XB  0D)wkJw  B'T5G^" `\m 20/_ R Conclusion (2 6   B +T5G^" `\3UC^ S References  (2 6   0.Ti2<r44 \Figure 1. ESR spectra of samples containing different amount of nanosilica measured at 10C.$] 2 T ]  0(-T-o1Hg1 jFigure 3. Temperature dependence of the outer extrema (2Azz) of ESR spectra for Rub.ns10 (L) and Rub.nscp04 (%).Zr(2 0   r3  0\:TF<U5J Figure 2. ESR spectra of samples containing the same amount of nanosilica and various amounts of coupling agent measured at 10C.$ 2 y   08=TaH 6[IK mFigure 4. ESR spectra of the spin probe diffusing in the matrix of Rub.ns00 sample at different temperatures.$n 2 e nw  Kv)V   #"2&8,--,-,-K v)V A  TDT_ж_ж ?"`&'Qv)R b0.92 #G j ?  TST_ж_ж ?"` 'Q&R fRub.ns20   #G j ;  T]T_ж_ж?&Rv)S b0.29 #G j 9  TWT_ж_ж ?"` R&S h Rub.nscp01   #G j 6  ThoT_ж_ж?&Sv)5U b0.40 #G j 4  T|wT_ж_ж ?"` S&5U h Rub.nscp02   #G j 1  T\yT_ж_ж?&5Uv)V b0.31 #G j /  T\T_ж_ж ?"` 5U&V h Rub.nscp04   #G j   TT_ж_ж?&Ov)'Q b0.94 #G j   T T_ж_ж? O&'Q fRub.ns15   #G j   TT_ж_ж?&sNv)O b0.96 #G j   T̮T_ж_ж? sN&O fRub.ns10   #G j !  TT_ж_ж?&Mv)sN b1.75 #G j "  TT_ж_ж? M&sN fRub.ns00   #G jC #   fT_ж_ж^d?" &Kv)M In/IwN   #G j $   fhT_ж_ж5d?"  K&M dsample #G jZB %  s *> ? sNv)sNZB &  s *> ? Ov)OZB '  s *> ? 'Qv)'QZB (  s *> ?&K&VZB )  s *> ? Mv)M`B *  0> ? Kv)K`B +  0> ? K V`B ,  0> ?v)Kv)V`B -  0> ? Vv)VZB 5  s *> ? 5Uv)5UZB :  s *> ? Sv)SZB @  s *> ? Rv)R I 0TDWO/Z \Table 3. The intensities ratio of narrow and wide component of ESR spectra measured at 10C.$] 2U ]  U 0TB E cThe amount of nanosilica in all samples containing the coupling agent was similar and equal 10 phr.d 2d d V 0TTZ^` BESR spectrometar : Varian E-109 Temperature unit Bruker ER 4111 VTCC Cx f  <A ??17@E#G x n  <A ??l5 #1E ) o 0lTb0kJ?h Z. Veksli, M Andreis, B. Rakvin, Prog Polym. Sci. 25 (2000) 949. G. Jeschke et al., Polymer Engineering and Science 44 (2004) 1112. 2 R p 0T_m o?i ESR spectra show a significant influence of nanosilica on the local chain dynamics. The increase in the nanosilica amount leads to the decrease in segmental motions. The coupling agent makes the role of nanosilica more pronounced. Because of the better contact between the matrix chain segment and nanosilica particles, the restriction in local motions become more and more important as the amount of coupling agent increases.(2 X v 0A?/1<   A "`uL6!AQU   0T#U,HE}V 7a) without coupling agent b) with the coupling agent"8 27,  G  0DUW.HZ }Figure 5. Schematic presentation of rubber matrices with the same crosslink densities and the same amount of the nanosilica. &~(2 u g    0U*MBxHN : 2 68 A:NrBS  :NArBSf   6A ?A:NrBN<   # AA+RbBS<   # AAPqBP(  0p UMBIS @crosslink points nanosilica particles coupling agent particles "A 2?B     X  0A?"6&D"-f  C >A$logotip%20zaklade DB3I H  0U<܍ ? 3380___PPT10.@[rr? &   (kJmiw   ACorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 GraphicX$ 212$V0,Hw6"$gqN,WGְdEh36"$vHηΈ={>cUH 2$],ֽ4 P R$D<$*q 2$ _s8) \k= $2$C^g¿pSK;&~ r$߀M'$,,Gi 2՜.+,0(    CustomRG  ArialTimes New Roman GaramondSymbol WP MathADefault DesignCorelDRAW 11.0 GraphicSigmaPlot 10.0 GraphSlide 1  Fonts UsedDes$fAζg6K/!m*52$s%dgZ1RV f2$ : H=>X񭑹Wa  0AAP3@<ʚ;ʚ;g4dd<@ 06p:@p<<4dddd w 0Td3 6/]0 `10 #G j  TxS_ж_ж?n6/ 0 fRub.ns10   #G j  TS_ж_ж? -]6/ _0 #G j  T@S_ж_ж?n- 6/ fRub.ns00   #G j(   fS_ж_ж^d?"  B*]- |The amount of nanosilica / phr #G j   fXS_ж_ж5d?" nB* - e sample #G jZB ' s *> ?n6/]6/ZB ( s *> ?n0]0ZB ) s *> ?n1]1ZB , s *> ? B* D3ZB & s *> ?n-]-`B % 0> ?nB*]B*`B + 0> ?nB*nD3`B - 0> ?]B*]D3`B * 0> ?nD3]D3  0Si2 4 @The average diametar of the used nanosilica particles was 13 nm.A 2A A  0S5 A8 RTable 2. NR samples with different amounts of coupling agent (Si 69)"SK S p ^:@C j  #""a$93zA  TS_ж_ж?5 A@C _4 #G j  TS_ж_ж?^A5 @C h Rub.nscp04   #G j  TS_ж_ж?5 @A _2 #G j  TS_ж_ж?^@5 A h Rub.nscp02   #G j  TS_ж_ж?5 >@ _1 #G j  TS_ж_ж?^>5 @ h Rub.nscp01   #G j,   fS_ж_ж^d?" 5 :> "The amount of coupling agent / phr## ##G j   fS_ж_ж5d?" ^:5 > q sample& #G jZB   s *> ?^@@ZB   s *> ?^AAZB   s *> ?5 :5 @CZB   s *> ?^>>`B   0> ?^::`B   0> ?^:^@C`B   0> ?:@C`B   0> ?^@C@C  0T'J{c!QD<4___PPT9 Two-roll mixing folowed by compression moulding. Swelling in the toluene probe solution at the constant temperature (35C). Removing the solvent by evaporationand annealing at 60 C during tree days.6!  8X  0DTV`W r.ESR  spin probe method   0TXV[ )probe amount in the samples was 0.15 wt%,*# *4  # AR%[  0("T[< ] ,4-hydroy-2,2,6,6-tetramethylpiperidin-1-oxyl- 2- # XB  0D)wkJw  B'T5G^" `V/FX R Conclusion (2 6   B +T5G^" `X7GZ S References  (2 6   0.T)1H, \Figure 1. ESR spectra of samples containing different amount of nanosilica measured at 10C.$] 2 T ]  0(-T7o1H; jFigure 3. Temperature dependence of the outer extrema (2Azz) of ESR spectra for Rub.ns10 (L) and Rub.nscp04 (%).Zr(2 0   r3  0\:TxA<U5E Figure 2. ESR spectra of samples containing the same amount of nanosilica and various amounts of coupling agent measured at 10C.$ 2 y   08=T+L1/ mFigure 4. ESR spectra of the spin probe diffusing in the matrix of Rub.ns00 sample at different temperatures.$n 2 e nw  Kv)V   #"2&8,--,-,-E )P A  TDT_ж_ж ?"`&'Qv)R b0.92 #G j ?  TST_ж_ж ?"` 'Q&R fRub.ns20   #G j ;  T]T_ж_ж?&Rv)S b0.29 #G j 9  TWT_ж_ж ?"` R&S h Rub.nscp01   #G j 6  ThoT_ж_ж?&Sv)5U b0.40 #G j 4  T|wT_ж_ж ?"` S&5U h Rub.nscp02   #G j 1  T\yT_ж_ж?&5Uv)V b0.31 #G j /  T\T_ж_ж ?"` 5U&V h Rub.nscp04   #G j   TT_ж_ж?&Ov)'Q b0.94 #G j   T T_ж_ж? O&'Q fRub.ns15   #G j   TT_ж_ж?&sNv)O b0.96 #G j   T̮T_ж_ж? sN&O fRub.ns10   #G j !  TT_ж_ж?&Mv)sN b1.75 #G j "  TT_ж_ж? M&sN fRub.ns00   #G jC #   fT_ж_ж^d?" &Kv)M In/IwN   #G j $   fhT_ж_ж5d?"  K&M dsample #G jZB %  s *> ? sNv)sNZB &  s *> ? Ov)OZB '  s *> ? 'Qv)'QZB (  s *> ?&K&VZB )  s *> ? Mv)M`B *  0> ? Kv)K`B +  0> ? K V`B ,  0> ?v)Kv)V`B -  0> ? Vv)VZB 5  s *> ? 5Uv)5UZB :  s *> ? Sv)SZB @  s *> ? Rv)R I 0TQ<-2U \Table 3. The intensities ratio of narrow and wide component of ESR spectra measured at 10C.$] 2U ]  U 0TB E cThe amount of nanosilica in all samples containing the coupling agent was similar and equal 10 phr.d 2d d V 0TTZ^` BESR spectrometar : Varian E-109 Temperature unit Bruker ER 4111 VTCC Cx f  <A ??- -* x n  <A ??0z/:@ ) o 0lT\v7H,c Z. Veksli, M Andreis, B. Rakvin, Prog Polym. Sci. 25 (2000) 949. G. Jeschke et al., Polymer Engineering and Science 44 (2004) 1112. 2 R p 0TZ<6e ESR spectra show a significant influence of nanosilica on the local chain dynamics. The increase in the nanosilica amount leads to the decrease in segmental motions. The coupling agent makes the role of nanosilica more pronounced. Because of the better contact between the matrix chain segment and nanosilica particles, the restriction in local motions become more and more important as the amount of coupling agent increases.(2 X v 0A?z5F(<   A "`E6{AM   0TN\-EJP 7a) without coupling agent b) with the coupling agent"8 27,  G  0DU=Q-gGT }Figure 5. Schematic presentation of rubber matrices with the same crosslink densities and the same amount of the nanosilica. &~(2 u g    0U*MBxHN : 2 68 A:NrBS  C4AAHf   6A ?A:NrBN<   # AA+RbBS<   # AAPqBP(  0p U>CDB-ITI @crosslink points nanosilica particles coupling agent particles "A 2?B     X  0A?,7Di7f  C >A$logotip%20zaklade DB3I H  0U<܍ ? 3380___PPT10.@[r& 2 ? & Ґ   (kJmiw   ACorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 GraphicCorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 Graphic SPW 10.0 Graph 0SigmaPlotGraphicObject.90(SigmaPlot 10.0 Graph SPW 10.0 Graph 0SigmaPlotGraphicObject.90(SigmaPlot 10.0 GraphD/ 0|DArialhA .0z[ 0DTimes New Roman0z[ 0 DGaramond Roman0z[ 00DSymbold Roman0z[ 0@DWP MathA Roman0z[ 0@ . @n?" dd@  @@`` h`P 212$V0,Hw6"$gqN,WGְdEh36"$vHηΈ={>cUH 2$],ֽ4 P R$D<$*q 2$ _s8) \k= 2$Z&$(WkBAc  2$C^g¿pSK;&~ r$߀M'$,,Gi 2$fAζg6K/!m*52$i mD~s2$ : H=>X񭑹Wa $2$RլQ?ER@2$s IHRc 0AAP3@<ʚ;ʚ;g4!d!d z[ 0p:@p<<4ddddL 0. A0___PPT10 pp___PPT9n^,֋S#ޠ"PNG  IHDRF}sRGB PLTE3*ծ cmPPJCmp0712 7tRNS@f8IDATWc``d !$$<[UBS#BT     B`S5G^" `-Am Q Objective (2 6   BS5G^" `V A" Q Materials (2 6   BTS5G^" `AFAH ZSample preparation(26   BT5G^" `QA3T OMethods(26   B/S5G^" `4C? OResults(26    03S^D<4___PPT9 ]Investigation of the NR samples containg different amounts of the nanosilica particles and their influence on local chain dynamics. Influence of a coupling agent on the changes in matrix structure and chain dynamics.@! U! 8X  0@S<$ V& JTable 1. Samples of NR with different amounts of nanosilica"KC Kt nB*]D3 l  #"&<WVWV'aP0 $ TMS_ж_ж? 1]D3 `20 #G j # T4S_ж_ж?n1 D3 fRub.ns20   #G j " T^S_ж_ж? 0]1 `15 #G j ! TWS_ж_ж?n0 1 fRub.ns15   #G j   ToS_ж_ж? 6/]0 `10 #G j  TxS_ж_ж?n6/ 0 fRub.ns10   #G j  TS_ж_ж? -]6/ _0 #G j  T@S_ж_ж?n- 6/ fRub.ns00   #G j(   fS_ж_ж^d?"  B*]- |The amount of nanosilica / phr #G j   fXS_ж_ж5d?" nB* - e sample #G jZB ' s *> ?n6/]6/ZB ( s *> ?n0]0ZB ) s *> ?n1]1ZB , s *> ? B* D3ZB & s *> ?n-]-`B % 0> ?nB*]B*`B + 0> ?nB*nD3`B - 0> ?]B*]D3`B * 0> ?nD3]D3  0Si2 4 @The average diametar of the used nanosilica particles was 13 nm.A 2A A  0S5 A8 RTable 2. NR samples with different amounts of coupling agent (Si 69)"SK S p ^:@C j  #""a$93zA  TS_ж_ж?5 A@C _4 #G j  TS_ж_ж?^A5 @C h Rub.nscp04   #G j  TS_ж_ж?5 @A _2 #G j  TS_ж_ж?^@5 A h Rub.nscp02   #G j  TS_ж_жA0___PPT10 pp___PPT9n^,֋S#ޠ"PNG  IHDRF}sRGB PLTE3*ծ cmPPJCmp0712 7tRNS@f8IDATWc``d !$$<[UBS#B@ _1 #G j  TS_ж_ж?^>5 @ h Rub.nscp01   #G j,   fS_ж_ж^d?" 5 :> "The amount of coupling agent / phr## ##G j   fS_ж_ж5d?" ^:5 > q sample& #G jZB   s *> ?^@@ZB   s *> ?^AAZB   s *> ?5 :5 @CZB   s *> ?^>>`B   0> ?^::`B   0> ?^:^@C`B   0> ?:@C`B   0> ?^@C@C  0T'J{c!QD<4___PPT9 Two-roll mixing folowed by compression moulding. Swelling in the toluene probe solution at the constant temperature (35C). Removing the solvent by evaporationand annealing at 60 C during tree days.6!  8X(  0DTWZ<\ ESR  spin probe method probe amount in the samples was 0.15 wt% CC C4  # A#U~ ^  0("TZ^{6_ ,4-hydroy-2,2,6,6-tetramethylpiperidin-1-oxyl- 2- # XB  0D)wkJw  B'T5G^" `W|/Y R Conclusion (2 6   B +T5G^" `W7hG Z S References  (2 6   0.T%+3KH?- \Figure 2. ESR spectra of samples containing different amount of nanosilica measured at 10C.$] 2 T ]  0(-T:5F= jFigure 4. Temperature dependence of the outer extrema (2Azz) of ESR spectra for Rub.ns10 (L) and Rub.nscp04 (%).Zr(2 0   r3  0\:TA_0(D Figure 3. ESR spectra of samples containing the same amount of nanosilica and various amounts of coupling agent measured at 10C.$ 2 y !  08=T+L1. mFigure 1. ESR spectra of the spin probe diffusing in the matrix of Rub.ns00 sample at different temperatures.&n(2 e nw  Kv)V   #"2&8,--,-,-DI; DT A  TDT_ж_ж ?"`&'Qv)R b0.92 #G j ?  TST_ж_ж ?"` 'Q&R fRub.ns20   #G j ;  T]T_ж_ж?&Rv)S b0.29 #G j 9  TWT_ж_ж ?"` R&S h Rub.nscp01   #G j 6  ThoT_ж_ж?&Sv)5U b0.40 #G j 4  T|wT_ж_ж ?"` S&5U h Rub.nscp02   #G j 1  T\yT_ж_ж?&5Uv)V b0.31 #G j /  T\T_ж_ж ?"` 5U&V h Rub.nscp04   #G j   TT_ж_ж?&Ov)'Q b0.94 #G j   T T_ж_ж? O&'Q fRub.ns15   #G j   TT_ж_ж?&sNv)O b0.96 #G j   T̮T_ж_ж? sN&O fRub.ns10   #G j !  TT_ж_ж?&Mv)sN b1.75 #G j "  TT_ж_ж? M&sN fRub.ns00   #G jC #   fT_ж_ж^d?" &Kv)M In/IwN   #G j $   fhT_ж_ж5d?"  K&M dsample #G jZB %  s *> ? sNv)sNZB &  s *> ? Ov)OZB '  s *> ? 'Qv)'QZB (  s *> ?&K&VZB )  s *> ? Mv)M`B *  0> ? Kv)K`B +  0> ? K V`B ,  0> ?v)Kv)V`B -  0> ? Vv)VZB 5  s *> ? 5Uv)5UZB :  s *> ? Sv)SZB @  s *> ? Rv)R I 0TND9FXG \Table 3. The intensities ratio of narrow and wide component of ESR spectra measured at 10C.$] 2U ]  U 0TB E cThe amount of nanosilica in all samples containing the coupling agent was similar and equal 10 phr.d 2d d V 0TT]a&c BESR spectrometar : Varian E-109 Temperature unit Bruker ER 4111 VTCC Cx f  <A ??- -* x n  <A ??0z/:@ ) o 0lT[8JHb Z. Veksli, M Andreis, B. Rakvin, Prog Polym. Sci. 25 (2000) 949. G. Jeschke et al., Polymer Engineering and Science 44 (2004) 1112. 2 R p 0TZ<6e ESR spectra show a significant influence of nanosilica on the local chain dynamics. The increase in the nanosilica amount leads to the decrease in segmental motions. The coupling agent makes the role of nanosilica more pronounced. Because of the better contact between the matrix chain segment and nanosilica particles, the restriction in local motions become more and more important as the amount of coupling agent increases.(2 X v 0A?]U5}F)<   A "`D)3M   0ThNL6O ;a) without coupling agent b) with the coupling agent"< 2;,  G  0DUP1S }Figure 5. Schematic presentation of rubber matrices with the same crosslink densities and the same amount of the nanosilica. &~(2 u g    0U*MBxHN : 2 68 A:NrBS  C23Hf   6A ?A:NrBN<   # AA+RbBS<   # AAPqBP(  0p UC39H @crosslink points nanosilica particles coupling agent particles "A 2?B     X  0A?f/H7D9f  C >A$logotip%20zaklade Q@F0Z  ) #q   #" DL(M n =w  3 #"  ) #qB   B&CDE|F45%Yv*FFHVfXv8VV&*Z(t8@          "`) KO    B CDEFh5%FFT H XhThhD4:X$ ` ` $ Zb<D,$      v  * @ 8 t V$ 8p4ff8(DrhtZhJ814@                       "` _   tBCz DEFP5%44 { ZN <  < x2 ,    @ * N X  z t\ (> T  ^ rP  F` ~ $ v4XDrtTF6DD8b*vV *  h fx%(@                 "`U ="   B C DE$Fl5%IIB ` p~  &` $ 6prB TP T    P 4` 4bf V n  & P 4 |    8 * 0     ~ :` B , ` x$ p<h(t:XHvX:8VtJxV<<34@                        "`s w>   BC DE0Fp5%LLuV( t8 f ,x:<H<xV,VV8  Hh <Ht< (F (HF6Df:D,HB   n  V  P    ` $ U 58@                         3"`    dBCDEFL5%11;vZX Z  vX::*Xv 8**F TXTTJZ<Tb<xRp:Hp8tTU#$@                "`Y #   B(CDEXF(5%uZf<<8xt, 8H Hth(@       3"` aMV2   C "` V2   C "`L?V2   C "`UdHHV2   C "`&rWV2   C "`K0V2   C "`V2   C "`V2   C "`~pV2   C "`>F1(V2   C "`th   c LA (1Small checker board"`lk   c LA (1Small checker board"`ED   c LA (1Small checker board"`]\   c LA (1Small checker board"`   c LA (1Small checker board"`{%z$   c LA (1Small checker board"`ON   c LA (1Small checker board"`UT   c LA (1Small checker board"`!"   c LA (1Small checker board"`   c LA (1Small checker board"`   c LA (1Small checker board"`  H  0U<܍ ? 3380___PPT10.@[r  ?     (kJmiw   ACorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 GraphicCorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 Graphic SPW 10.0 Graph 0SigmaPlotGraphicObject.90(SigmaPlot 10.0 Graph SPW 10.0 Graph 0SigmaPlotGraphicObject.90(SigmaPlot 10.0 GraphD/ 0|DArialhA .0z[ 0DTimes New Roman0z[ 0 DGaramond Roman0z[ 00DSymbold Roman0z[ 0@DWP MathA Roman0z[ 0@ . @n?" dd@  @@`` h`P 212$V0,Hw6"$gqN,WGְdEh36"$vHηΈ={>cUH 2$],ֽ4 P R$D<$*q 2$ _s8) \k= 2$Z&$(WkBAc  2$C^g¿pSK;&~ r$߀M'$,,Gi 2$fAζg6K/!m*52$i mD~s2$ : H=>X񭑹Wa $2$RլQ?ER@2$s IHRc 0AAP3@<ʚ;ʚ;g4!d!d z[ 0F p:@p<<4ddddL 0. A0___PPT10 pp___PPT9n^,֋S#ޠ"PNG  IHDRF}sRGB PLTE3*ծ cmPPJCmp0712 7tRNS@f8IDATWc``d !$$<[UBS#BT     B`S5G^" `-Am Q Objective (2 6   BS5G^" `V A" Q Materials (2 6   BTS5G^" `AFAH ZSample preparation(26   BT5G^" `QA3T OMethods(26   B/S5G^" `4C? OResults(26    03S^D<4___PPT9 ]Investigation of the NR samples containg different amounts of the nanosilica particles and their influence on local chain dynamics. Influence of a coupling agent on the changes in matrix structure and chain dynamics.@! U! 8X  0@S<$ V& JTable 1. Samples of NR with different amounts of nanosilica"KC Kt nB*]D3 l  #"&<WVWV'aP0 $ TMS_ж_ж? 1]D3 `20 #G j # T4S_ж_ж?n1 D3 fRub.ns20   #G j " T^S_ж_ж? 0]1 `15 #G j ! TWS_ж_ж?n0 1 fRub.ns15   #G j   ToS_ж_ж? 6/]0 `10 #G j  TxS_ж_ж?n6/ 0 fRub.ns10   #G j  TS_ж_ж? -]6/ _0 #G j  T@S_ж_ж?n- 6/ fRub.ns00   #G j(   fS_ж_ж^d?"  B*]- |The amount of nanosilica / phr #G j   fXS_ж_ж5d?" nB* - e sample #G jZB ' s *> ?n6/]6/ZB ( s *> ?n0]0ZB ) s *> ?n1]1ZB , s *> ? B* D3ZB & s *> ?n-]-`B % 0> ?nB*]B*`B + 0> ?nB*nD3`B - 0> ?]B*]D3`B * 0> ?nD3]D3  0Si2 4 @The average diametar of the used nanosilica particles was 13 nm.A 2A A  0S5 A8 RTable 2. NR samples with different amounts of coupling agent (Si 69)"SK S p ^:@C j  #""a$93zA  TS_ж_ж?5 A@C _4 #G j  TS_ж_ж?^A5 @C h Rub.nscp04   #G j  TS_ж_ж?5 @A _2 #G j  TS_ж_ж?^@5 A h Rub.nscp02   #G j  TS_ж_ж?5 >@ _1 #G j  TS_ж_ж?^>5 @ h Rub.nscp01   #G j,   fS_ж_ж^d?" 5 :> "The amount of coupling agent / phr## ##G j   fS_ж_ж5d?" ^:5 > q sample& #G jZB   s *> ?^@@ZB   s *> ?^AAZB   s *> ?5 :5 @CZB   s *> ?^>>`B   0> ?^::`B   0> ?^:^@C`B   0> ?:@C`B   0> ?^@C@C  0T'J{c!QD<4___PPT9 Two-roll mixing folowed by compression moulding. Swelling in the toluene probe solution at the constant temperature (35C). Removing the solvent by evaporationand annealing at 60 C during tree days.6!  8X(  0DTWZ<\ ESR  spin probe method probe amount in the samples was 0.15 wt% CC C4  # A#U~ ^  0("TZ^{6_ ,4-hydroy-2,2,6,6-tetramethylpiperidin-1-oxyl- 2- # XB  0D)wkJw  B'T5G^" `W|/Y R Conclusion (2 6   B +T5G^" `W7hG Z S References  (2 6   0.T%+3KH?- \Figure 2. ESR spectra of samples containing different amount of nanosilica measured at 10C.$] 2 T ]  0(-T;5F> jFigure 4. Temperature dependence of the outer extrema (2Azz) of ESR spectra for Rub.ns10 (L) and Rub.nscp04 (%).Zr(2 0   r3  0\:TA_0(D Figure 3. ESR spectra of samples containing the same amount of nanosilica and various amounts of coupling agent measured at 10C.$ 2 y !  08=T+L1. mFigure 1. ESR spectra of the spin probe diffusing in the matrix of Rub.ns00 sample at different temperatures.&n(2 e nw  Kv)V   #"2&8,--,-,-DI; DT A  TDT_ж_ж ?"`&'Qv)R b0.92 #G j ?  TST_ж_ж ?"` 'Q&R fRub.ns20   #G j ;  T]T_ж_ж?&Rv)S b0.29 #G j 9  TWT_ж_ж ?"` R&S h Rub.nscp01   #G j 6  ThoT_ж_ж?&Sv)5U b0.40 #G j 4  T|wT_ж_ж ?"` S&5U h Rub.nscp02   #G j 1  T\yT_ж_ж?&5Uv)V b0.31 #G j /  T\T_ж_ж ?"` 5U&V h Rub.nscp04   #G j   TT_ж_ж?&Ov)'Q b0.94 #G j   T T_ж_ж? O&'Q fRub.ns15   #G j   TT_ж_ж?&sNv)O b0.96 #G j   T̮T_ж_ж? sN&O fRub.ns10   #G j !  TT_ж_ж?&Mv)sN b1.75 #G j "  TT_ж_ж? M&sN fRub.ns00   #G jC #   fT_ж_ж^d?" &Kv)M In/IwN   #G j $   fhT_ж_ж5d?"  K&M dsample #G jZB %  s *> ? sNv)sNZB &  s *> ? Ov)OZB '  s *> ? 'Qv)'QZB (  s *> ?&K&VZB )  s *> ? Mv)M`B *  0> ? Kv)K`B +  0> ? K V`B ,  0> ?v)Kv)V`B -  0> ? Vv)VZB 5  s *> ? 5Uv)5UZB :  s *> ? Sv)SZB @  s *> ? Rv)R I 0TND9FXG \Table 3. The intensities ratio of narrow and wide component of ESR spectra measured at 10C.$] 2U ]  U 0TB E cThe amount of nanosilica in all samples containing the coupling agent was similar and equal 10 phr.d 2d d V 0TT]a&c BESR spectrometar : Varian E-109 Temperature unit Bruker ER 4111 VTCC C f  <A ??"`- -* x n  <A ??0z/:@ ) o 0lT[8JHb Z. Veksli, M Andreis, B. Rakvin, Prog Polym. Sci. 25 (2000) 949. G. Jeschke et al., Polymer Engineering and Science 44 (2004) 1112. 2 R p 0TZ<6e ESR spectra show a significant influence of nanosilica on the local chain dynamics. The increase in the nanosilica amount leads to the decrease in segmental motions. The coupling agent makes the role of nanosilica more pronounced. Because of the better contact between the matrix chain segment and nanosilica particles, the restriction in local motions become more and more important as the amount of coupling agent increases.(2 f v 0A?"`]U5}F)<   A "`D)3M   0ThNL6O ;a) without coupling agent b) with the coupling agent"< 2;,  G  0DUP1S }Figure 5. Schematic presentation of rubber matrices with the same crosslink densities and the same amount of the nanosilica. &~(2 u g    0U*MBxHN : 2 68 A:NrBS  C23Hf   6A ?A:NrBN<   # AA+RbBS<   # AAPqBP(  0p UC39H @crosslink points nanosilica particles coupling agent particles "A 2?B     X  0A?f/H7D9f  C >A$logotip%20zaklade Q@F0Z  ) #q   #" DL(M n =w  3 #"  ) #qB   B&CDE|F45%Yv*FFHVfXv8VV&*Z(t8@          "`) KO    B CDEFh5%FFT H XhThhD4:X$ ` ` $ Zb<D,$      v  * @ 8 t V$ 8p4ff8(DrhtZhJ814@                       "` _   tBCz DEFP5%44 { ZN <  < x2 ,    @ * N X  z t\ (> T  ^ rP  F` ~ $ v4XDrtTF6DD8b*vV *  h fx%(@                 "`U ="   B C DE$Fl5%IIB ` p~  &` $ 6prB TP T    P 4` 4bf V n  & P 4 |    8 * 0     ~ :` B , ` x$ p<h(t:XHvX:8VtJxV<<34@                        "`s w>   BC DE0Fp5%LLuV( t8 f ,x:<H<xV,VV8  Hh <Ht< (F (HF6Df:D,HB   n  V  P    ` $ U 58@                         3"`    dBCDEFL5%11;vZX Z  vX::*Xv 8**F TXTTJZ<Tb<xRp:Hp8tTU#$@                "`Y #   B(CDEXF(5%uZf<<8xt, 8H Hth(@       3"` aMV2   C "` V2   C "`L?V2   C "`UdHHV2   C "`&rWV2   C "`K0V2   C "`V2   C "`V2   C "`~pV2   C "`>F1(V2   C "`th   c LA (1Small checker board"`lk   c LA (1Small checker board"`ED   c LA (1Small checker board"`]\   c LA (1Small checker board"`   c LA (1Small checker board"`{%z$   c LA (1Small checker board"`ON   c LA (1Small checker board"`UT   c LA (1Small checker board"`!"   c LA (1Small checker board"`   c LA (1Small checker board"`   c LA (1Small checker board"`  H  0U<܍ ? 3380___PPT10.@[r s ?    (kJmiw   ACorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 GraphicCorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 Graphic SPW 10.0 Graph 0SigmaPlotGraphicObject.90(SigmaPlot 10.0 Graph SPW 10.0 Graph 0SigmaPlotGraphicObject.90(SigmaPlot 10.0 GraphD/ 0|DArialhA .0z[ 0DTimes New Roman0z[ 0 DGaramond Roman0z[ 00DSymbold Roman0z[ 0@DWP MathA Roman0z[ 0@ . @n?" dd@  @@`` h`P 212$V0,Hw6"$gqN,WGְdEh36"$vHηΈ={>cUH 2$],ֽ4 P R$D<$*q 2$ _s8) \k= 2$Z&$(WkBAc  2$C^g¿pSK;&~ r$߀M'$,,Gi 2$fAζg6K/!m*52$i mD~s2$ : H=>X񭑹Wa $2$RլQ?ER@2$s IHRc 0AAP3@<ʚ;ʚ;g4!d!d z[ 0p:@p<<4ddddL 0. A0___PPT10 pp___PPT9n^,֋S#ޠ"PNG  IHDRF}sRGB PLTE3*ծ cmPPJCmp0712 7tRNS@f8IDATWc``d !$$<[UBS#BT     B`S5G^" `-Am Q Objective (2 6   BS5G^" `V A" Q Materials (2 6   BTS5G^" `AFAH ZSample preparation(26   BT5G^" `QA3T OMethods(26   B/S5G^" `4C? OResults(26    03S^D<4___PPT9 ]Investigation of the NR samples containg different amounts of the nanosilica particles and their influence on local chain dynamics. Influence of a coupling agent on the changes in matrix structure and chain dynamics.@! U! 8X  0@S<$ V& JTable 1. Samples of NR with different amounts of nanosilica"KC Kt nB*]D3 l  #"&<WVWV'aP0 $ TMS_ж_ж? 1]D3 `20 #G j # T4S_ж_ж?n1 D3 fRub.ns20   #G j " T^S_ж_ж? 0]1 `15 #G j ! TWS_ж_ж?n0 1 fRub.ns15   #G j   ToS_ж_ж? 6/]0 `10 #G j  TxS_ж_ж?n6/ 0 fRub.ns10   #G j  TS_ж_ж? -]6/ _0 #G j  T@S_ж_ж?n- 6/ fRub.ns00   #G j(   fS_ж_ж^d?"  B*]- |The amount of nanosilica / phr #G j   fXS_ж_ж5d?" nB* - e sample #G jZB ' s *> ?n6/]6/ZB ( s *> ?n0]0ZB ) s *> ?n1]1ZB , s *> ? B* D3ZB & s *> ?n-]-`B % 0> ?nB*]B*`B + 0> ?nB*nD3`B - 0> ?]B*]D3`B * 0> ?nD3]D3  0Si2 4 @The average diametar of the used nanosilica particles was 13 nm.A 2A A  0S5 A8 RTable 2. NR samples with different amounts of coupling agent (Si 69)"SK S p ^:@C j  #""a$93zA  TS_ж_ж?5 A@C _4 #G j  TS_ж_ж?^A5 @C h Rub.nscp04   #G j  TS_ж_ж?5 @A _2 #G j  TS_ж_ж?^@5 A h Rub.nscp02   #G j  TS_ж_ж?5 > l J 6Ԕ"`<kJ~U   ``C`CA ?"6@ NNN?N  ~  BA ??TG: ~   @ _1 #G j  TS_ж_ж?^>5 @ h Rub.nscp01   #G j,   fS_ж_ж^d?" 5 :> "The amount of coupling agent / phr## ##G j   fS_ж_ж5d?" ^:5 > q sample& #G jZB   s *> ?^@@ZB   s *> ?^AAZB   s *> ?5 :5 @CZB   s *> ?^>>`B   0> ?^::`B   0> ?^:^@C`B   0> ?:@C`B   0> ?^@C@C  0T'J{c!QD<4___PPT9 Two-roll mixing folowed by compression moulding. Swelling in the toluene probe solution at the constant temperature (35C). Removing the solvent by evaporationand annealing at 60 C during tree days.6!  8X(  0DTWZ<\ ESR  spin probe method probe amount in the samples was 0.15 wt% CC C4  # A#U~ ^  0("TZ^{6_ ,4-hydroy-2,2,6,6-tetramethylpiperidin-1-oxyl- 2- # XB  0D)wkJw  B'T5G^" `W|/Y R Conclusion (2 6   B +T5G^" `W7hGY S References  (2 6   0.T%+3KH?- \Figure 2. ESR spectra of samples containing different amount of nanosilica measured at 10C.$] 2 T ]  0(-T;5F> jFigure 4. Temperature dependence of the outer extrema (2Azz) of ESR spectra for Rub.ns10 (L) and Rub.nscp04 (%).Zr(2 0   r3  0\:TA_0(D Figure 3. ESR spectra of samples containing the same amount of nanosilica and various amounts of coupling agent measured at 10C.$ 2 y !  08=T+L1. mFigure 1. ESR spectra of the spin probe diffusing in the matrix of Rub.ns00 sample at different temperatures.&n(2 e nw  Kv)V   #"2&8,--,-,-DI; DT A  TDT_ж_ж ?"`&'Qv)R b0.92 #G j ?  TST_ж_ж ?"` 'Q&R fRub.ns20   #G j ;  T]T_ж_ж?&Rv)S b0.29 #G j 9  TWT_ж_ж ?"` R&S h Rub.nscp01   #G j 6  ThoT_ж_ж?&Sv)5U b0.40 #G j 4  T|wT_ж_ж ?"` S&5U h Rub.nscp02   #G j 1  T\yT_ж_ж?&5Uv)V b0.31 #G j /  T\T_ж_ж ?"` 5U&V h Rub.nscp04   #G j   TT_ж_ж?&Ov)'Q b0.94 #G j   T T_ж_ж? O&'Q fRub.ns15   #G j   TT_ж_ж?&sNv)O b0.96 #G j   T̮T_ж_ж? sN&O fRub.ns10   #G j !  TT_ж_ж?&Mv)sN b1.75 #G j "  TT_ж_ж? M&sN fRub.ns00   #G jC #   fT_ж_ж^d?" &Kv)M In/IwN   #G j $   fhT_ж_ж5d?"  K&M dsample #G jZB %  s *> ? sNv)sNZB &  s *> ? Ov)OZB '  s *> ? 'Qv)'QZB (  s *> ?&K&VZB )  s *> ? Mv)M`B *  0> ? Kv)K`B +  0> ? K V`B ,  0> ?v)Kv)V`B -  0> ? Vv)VZB 5  s *> ? 5Uv)5UZB :  s *> ? Sv)SZB @  s *> ? Rv)R I 0TND9FXG \Table 3. The intensities ratio of narrow and wide component of ESR spectra measured at 10C.$] 2U ]  U 0TB E cThe amount of nanosilica in all samples containing the coupling agent was similar and equal 10 phr.d 2d d V 0TT]a&c BESR spectrometar : Varian E-109 Temperature unit Bruker ER 4111 VTCC C f  <A ??"`- -* x n  <A ??0z/:@ ) o 0lTZ8JH9a Z. Veksli, M Andreis, B. Rakvin, Prog Polym. Sci. 25 (2000) 949. G. Jeschke et al., Polymer Engineering and Science 44 (2004) 1112. 2 R p 0TZ<6e ESR spectra show a significant influence of nanosilica on the local chain dynamics. The increase in the nanosilica amount leads to the decrease in segmental motions. The coupling agent makes the role of nanosilica more pronounced. Because of the better contact between the matrix chain segment and nanosilica particles, the restriction in local motions become more and more important as the amount of coupling agent increases.(2 f v 0A?"`]U5}F)<   A "`D)3M   0ThNL6O ;a) without coupling agent b) with the coupling agent"< 2;,  G  0DUP1S }Figure 5. Schematic presentation of rubber matrices with the same crosslink densities and the same amount of the nanosilica. &~(2 u g    0U*MBxHN : 2 68 A:NrBS  C23Hf   6A ?A:NrBN<   # AA+RbBS<   # AAPqBP(  0p UC39H @crosslink points nanosilica particles coupling agent particles "A 2?B     X  0A?f/H7D9f  C >A$logotip%20zaklade Q@F0Z  ) #q   #" DL(M n =w  3 #"  ) #qB   B&CDE|F45%Yv*FFHVfXv8VV&*Z(t8@          "`) KO    B CDEFh5%FFT H XhThhD4:X$ ` ` $ Zb<D,$      v  * @ 8 t V$ 8p4ff8(DrhtZhJ814@                       "` _   tBCz DEFP5%44 { ZN <  < x2 ,    @ * N X  z t\ (> T  ^ rP  F` ~ $ v4XDrtTF6DD8b*vV *  h fx%(@                 "`U ="   B C DE$Fl5%IIB ` p~  &` $ 6prB TP T    P 4` 4bf V n  & P 4 |    8 * 0     ~ :` B , ` x$ p<h(t:XHvX:8VtJxV<<34@                        "`s w>   BC DE0Fp5%LLuV( t8 f ,x:<H<xV,VV8  Hh <Ht< (F (HF6Df:D,HB   n  V  P    ` $ U 58@                         3"`    dBCDEFL5%11;vZX Z  vX::*Xv 8**F TXTTJZ<Tb<xRp:Hp8tTU#$@                "`Y #   B(CDEXF(5%uZf<<8xt, 8H Hth(@       3"` aMV2   C "` V2   C "`L?V2   C "`UdHHV2   C "`&rWV2   C "`K0V2   C "`V2   C "`V2   C "`~pV2   C "`>F1(V2   C "`th   c LA (1Small checker board"`lk   c LA (1Small checker board"`ED   c LA (1Small checker board"`]\   c LA (1Small checker board"`   c LA (1Small checker board"`{%z$   c LA (1Small checker board"`ON   c LA (1Small checker board"`UT   c LA (1Small checker board"`!"   c LA (1Small checker board"`   c LA (1Small checker board"`   c LA (1Small checker board"`  H  0U<܍ ? 3380___PPT10.@[rԒ d ?     (kJmiw   ACorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 GraphicCorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 Graphic SPW 10.0 Graph 0SigmaPlotGraphicObject.90(SigmaPlot 10.0 Graph SPW 10.0 Graph 0SigmaPlotGraphicObject.90(SigmaPlot 10.0 GraphD/ 0|DArialhA .0z[ 0DTimes New Roman0z[ 0 DGaramond Roman0z[ 00DSymbold Roman0z[ 0@DWP MathA Roman0z[ 0@ . @n?" dd@  @@`` P 212$V0,Hw6"$gqN,WGְdEh36"$vHηΈ={>cUH 2$],ֽ4 P R$D<$*q 2$ _s8) \k= 2$Z&$(WkBAc  2$C^g¿pSK;&~ r$߀M'$,,Gi 2$fAζg6K/!m*5$2$ : H=>X񭑹Wa  0AAP3@<ʚ;ʚ;g4!d!d z[ 0>p:@p<<4ddddL 0. A0___PPT10 pp___PPT9n^,֋S#ޠ"PNG  IHDRF}sRGB PLTE3*ծ cmPPJCmp0712 7tRNS@f8IDATWc``d !$$<[UBS#BT     B`S5G^" `-Am Q Objective (2 6   BS5G^" `V A" Q Materials (2 6   BTS5G^" `AFAH ZSample preparation(26   BT5G^" `QA3T OMethods(26   B/S5G^" `4C? OResults(26    03S^D<4___PPT9 ]Investigation of the NR samples containg different amounts of the nanosilica particles and their influence on local chain dynamics. Influence of a coupling agent on the changes in matrix structure and chain dynamics.@! U! 8X  0@S<$ V& JTable 1. Samples of NR with different amounts of nanosilica"KC Kt nB*]D3 l  #"&<WVWV'aP0 $ TMS_ж_ж? 1]D3 `20 #G j # T4S_ж_ж?n1 D3 fRub.ns20   #G j " T^S_ж_ж? 0]1 `15 #G j ! TWS_ж_ж?n0 1 fRub.ns15   #G j   ToS_ж_ж? 6/]0 `10 #G j  TxS_ж_ж?n6/ 0 fRub.ns10   #G j  TS_ж_ж? -]6/ _0 #G j  T@S_ж_ж?n- 6/ fRub.ns00   #G j(   fS_ж_ж^d?"  B*]- |The amount of nanosilica / phr #G j   fXS_ж_ж5d?" nB* - e sample #G jZB ' s *> ?n6/]6/ZB ( s *> ?n0]0ZB ) s *> ?n1]1ZB , s *> ? B* D3ZB & s *> ?n-]-`B % 0> ?nB*]B*`B + 0> ?nB*nD3`B - 0> ?]B*]D3`B * 0> ?nD3]D3  0Si2 4 @The average diametar of the used nanosilica particles was 13 nm.A 2A A  0S5 A8 RTable 2. NR samples with different amounts of coupling agent (Si 69)"SK S p ^:@C j  #""a$93zA  TS_ж_ж?5 A@C _4 #G j  TS_ж_ж?^A5 @C h Rub.nscp04   #G j  TS_ж_ж?5 @A _2 #G j  TS_ж_ж?^@5 A h Rub.nscp02   #G j  TS_ж_ж?5 >@ _1 #G j  TS_ж_ж?^>5 @ h Rub.nscp01   #G j,   fS_ж_ж^d?" 5 :> "The amount of coupling agent / phr## ##G j   fS_ж_ж5d?" ^:5 > q sample& #G jZB   s *> ?^@@ZB   s *> ?^AAZB   s *> ?5 :5 @CZB   s *> ?^>>`B   0> ?^::`B   0> ?^:^@C`B   0> ?:@C`B   0> ?^@C@C  0T'J{c!QD<4___PPT9 Two-roll mixing folowed by compression moulding. Swelling in the toluene probe solution at the constant temperature (35C). Removing the solvent by evaporationand annealing at 60 C during tree days.6!  8X(  0DTWZ<\ ESR  spin probe method probe amount in the samples was 0.15 wt% CC C4  # A#U~ ^  0("TZ^{6_ ,4-hydroy-2,2,6,6-tetramethylpiperidin-1-oxyl- 2- # XB  0D)wkJw  B'T5G^" `W|/Y R Conclusion (2 6   B +T5G^" `W7hGY S References  (2 6   0.T%+3KH?- \Figure 2. ESR spectra of samples containing different amount of nanosilica measured at 10C.$] 2 T ]  0(-T;5F> jFigure 4. Temperature dependence of the outer extrema (2Azz) of ESR spectra for Rub.ns10 (L) and Rub.nscp04 (%).Zr(2 0   r3  0\:TA_0(D Figure 3. ESR spectra of samples containing the same amount of nanosilica and various amounts of coupling agent measured at 10C.$ 2 y !  08=T+L1. mFigure 1. ESR spectra of the spin probe diffusing in the matrix of Rub.ns00 sample at different temperatures.&n(2 e nw  Kv)V   #"2&8,--,-,-DI; DT A  TDT_ж_ж ?"`&'Qv)R b0.92 #G j ?  TST_ж_ж ?"` 'Q&R fRub.ns20   #G j ;  T]T_ж_ж?&Rv)S b0.29 #G j 9  TWT_ж_ж ?"` R&S h Rub.nscp01   #G j 6  ThoT_ж_ж?&Sv)5U b0.40 #G j 4  T|wT_ж_ж ?"` S&5U h Rub.nscp02   #G j 1  T\yT_ж_ж?&5Uv)V b0.31 #G j /  T\T_ж_ж ?"` 5U&V h Rub.nscp04   #G j   TT_ж_ж?&Ov)'Q b0.94 #G j   T T_ж_ж? O&'Q fRub.ns15   #G j   TT_ж_ж?&sNv)O b0.96 #G j   T̮T_ж_ж? sN&O fRub.ns10   #G j !  TT_ж_ж?&Mv)sN b1.75 #G j "  TT_ж_ж? M&sN fRub.ns00   #G jC #   fT_ж_ж^d?" &Kv)M In/IwN   #G j $   fhT_ж_ж5d?"  K&M dsample #G jZB %  s *> ? sNv)sNZB &  s *> ? Ov)OZB '  s *> ? 'Qv)'QZB (  s *> ?&K&VZB )  s *> ? Mv)M`B *  0> ? Kv)K`B +  0> ? K V`B ,  0> ?v)Kv)V`B -  0> ? Vv)VZB 5  s *> ? 5Uv)5UZB :  s *> ? Sv)SZB @  s *> ? Rv)R I 0TND9FXG \Table 3. The intensities ratio of narrow and wide component of ESR spectra measured at 10C.$] 2U ]  U 0TB E cThe amount of nanosilica in all samples containing the coupling agent was similar and equal 10 phr.d 2d d V 0TT]a&c BESR spectrometar : Varian E-109 Temperature unit Bruker ER 4111 VTCC C f  <A ??"`- -* x n  <A ??0z/:@ ) o 0lTZ8JH9a Z. Veksli, M Andreis, B. Rakvin, Prog Polym. Sci. 25 (2000) 949. G. Jeschke et al., Polymer Engineering and Science 44 (2004) 1112. 2 R p 0TZ<6e ESR spectra show a significant influence of nanosilica on the local chain dynamics. The increase in the nanosilica amount leads to the decrease in segmental motions. The coupling agent makes the role of nanosilica more pronounced. Because of the better contact between the matrix chain segment and nanosilica particles, the restriction in local motions become more and more important as the amount of coupling agent increases.(2 f v 0A?"`]U5}F)<   A "`1E\-8N  0TN8O Ia) without coupling agent b) with the coupling agent"J 2I,  G  0DUQ"4T }Figure 5. Schematic presentation of rubber matrices with the same crosslink densities and the same amount of the nanosilica. &~(2 u g    0U*MBxHN : 2 X  0A?f/H7D9f  C >A$logotip%20zaklade Q@F0Z  ) #q   #" 1E ,N n =w  3 #"  ) #qB   B&CDE|F45%Yv*FFHVfXv8VV&*Z(t8@          "`) KO    B CDEFh5%FFT H XhThhD4:X$ ` ` $ Zb<D,$      v  * @ 8 t V$ 8p4ff8(DrhtZhJ814@                       "` _   tBCz DEFP5%44 { ZN <  < x2 ,    @ * N X  z t\ (> T  ^ rP  F` ~ $ v4XDrtTF6DD8b*vV *  h fx%(@                 "`U ="   B C DE$Fl5%IIB ` p~  &` $ 6prB TP T    P 4` 4bf V n  & P 4 |    8 * 0     ~ :` B , ` x$ p<h(t:XHvX:8VtJxV<<34@                        "`s w>   BC DE0Fp5%LLuV( t8 f ,x:<H<xV,VV8  Hh <Ht< (F (HF6Df:D,HB   n  V  P    ` $ U 58@                         3"`    dBCDEFL5%11;vZX Z  vX::*Xv 8**F TXTTJZ<Tb<xRp:Hp8tTU#$@                "`Y #   B(CDEXF(5%uZf<<8xt, 8H Hth(@       3"` aMV2   C "` V2   C "`L?V2   C "`UdHHV2   C "`&rWV2   C "`K0V2   C "`V2   C "`V2   C "`~pV2   C "`>F1(V2   C "`th   c LA (1Small checker board"`lk   c LA (1Small checker board"`ED   c LA (1Small checker board"`]\   c LA (1Small checker board"`   c LA (1Small checker board"`{%z$   c LA (1Small checker board"`ON   c LA (1Small checker board"`UT   c LA (1Small checker board"`!"   c LA (1Small checker board"`   c LA (1Small checker board"`   c LA (1Small checker board"`  H  0U<܍ ? 3380___PPT10.@[r  ?    (kJmiw   ACorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 GraphicCorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 Graphic SPW 10.0 Graph 0SigmaPlotGraphicObject.90(SigmaPlot 10.0 Graph SPW 10.0 Graph 0SigmaPlotGraphicObject.90(SigmaPlot 10.0 GraphD/ 0|DArialhA .0z[ 0DTimes New Roman0z[ 0 DGaramond Roman0z[ 00DSymbold Roman0z[ 0@DWP MathA Roman0z[ 0@ . @n?" dd@  @@`` P 212$V0,Hw6"$gqN,WGְdEh36"$vHηΈ={>cUH 2$],ֽ4 P R$D<$*q 2$ _s8) \k= 2$Z&$(WkBAc  2$C^g¿pSK;&~ r$߀M'$,,Gi 2$fAζg6K/!m*5$2$ : H=>X񭑹Wa  0AAP3@<ʚ;ʚ;g4!d!d z[ 0Rp:@p<<4ddddL 0. A0___PPT10 pp___PPT9n^,֋S#ޠ"PNG  IHDRF}sRGB PLTE3*ծ cmPPJCmp0712 7tRNS@f8IDATWc``d !$$<[UBS#BT     B`S5G^" `-Am Q Objective (2 6   BS5G^" `V A" Q Materials (2 6   BTS5G^" `AFAH ZSample preparation(26   BT5G^" `QA3T OMethods(26   B/S5G^" `4C? OResults(26    03S^D<4___PPT9 ]Investigation of the NR samples containg different amounts of the nanosilica particles and their influence on local chain dynamics. Influence of a coupling agent on the changes in matrix structure and chain dynamics.@! U! 8X  0@S<$ V& JTable 1. Samples of NR with different amounts of nanosilica"KC Kt nB*]D3 l  #"&<WVWV'aP0 $ TMS_ж_ж? 1]D3 `20 #G j # T4S_ж_ж?n1 D3 fRub.ns20   #G j " T^S_ж_ж? 0]1 `15 #G j ! TWS_ж_ж?n0 1 fRub.ns15   #G j   ToS_ж_ж? 6/]0 `10 #G j  TxS_ж_ж?n6/ 0 fRub.ns10   #G j  TS_ж_ж? -]6/ _0 #G j  T@S_ж_ж?n- 6/ fRub.ns00   #G j(   fS_ж_ж^d?"  B*]- |The amount of nanosilica / phr #G j   fXS_ж_ж5d?" nB* - e sample #G jZB ' s *> ?n6/]6/ZB ( s *> ?n0]0ZB ) s *> ?n1]1ZB , s *> ? B* D3ZB & s *> ?n-]-`B % 0> ?nB*]B*`B + 0> ?nB*nD3`B - 0> ?]B*]D3`B * 0> ?nD3]D3  0Si2 4 @The average diametar of the used nanosilica particles was 13 nm.A 2A A  0S5 A8 RTable 2. NR samples with different amounts of coupling agent (Si 69)"SK S p ^:@C j  #""a$93zA  TS_ж_ж?5 A@C _4 #G j  TS_ж_ж?^A5 @C h Rub.nscp04   #G j  TS_ж_ж?5 @A _2 #G j  TS_ж_ж?^@5 A h Rub.nscp02   #G j BA ??T' h  T8gKgKff "`-G`XP___PPT92* n Natural Rubber Filled by Nanosilica: an ESR  Spin Probe Stud  TS_ж_ж?5 >@ _1 #G j  TS_ж_ж?^>5 @ h Rub.nscp01   #G j,   fS_ж_ж^d?" 5 :> "The amount of coupling agent / phr## ##G j   fS_ж_ж5d?" ^:5 > q sample& #G jZB   s *> ?^@@ZB   s *> ?^AAZB   s *> ?5 :5 @CZB   s *> ?^>>`B   0> ?^::`B   0> ?^:^@C`B   0> ?:@C`B   0> ?^@C@C  0T'J{c!QD<4___PPT9 Two-roll mixing folowed by compression moulding. Swelling in the toluene probe solution at the constant temperature (35C). Removing the solvent by evaporationand annealing at 60 C during tree days.6!  8X(  0DTWZ<\ ESR  spin probe method probe amount in the samples was 0.15 wt% CC C4  # A#U~ ^  0("TZ^{6_ ,4-hydroy-2,2,6,6-tetramethylpiperidin-1-oxyl- 2- # XB  0D)wkJw  B'T5G^" `W|/Y R Conclusion (2 6   B +T5G^" `W7hGY S References  (2 6   0.T%+3KH?- \Figure 2. ESR spectra of samples containing different amount of nanosilica measured at 10C.$] 2 T ]  0(-T;5F> jFigure 4. Temperature dependence of the outer extrema (2Azz) of ESR spectra for Rub.ns10 (L) and Rub.nscp04 (%).Zr(2 0   r3  0\:TA_0(D Figure 3. ESR spectra of samples containing the same amount of nanosilica and various amounts of coupling agent measured at 10C.$ 2 y !  08=T+L1. mFigure 1. ESR spectra of the spin probe diffusing in the matrix of Rub.ns00 sample at different temperatures.&n(2 e nw  Kv)V   #"2&F;eDS A  TDT_ж_ж ?"`&'Qv)R b0.92 #G j ?  TST_ж_ж ?"` 'Q&R fRub.ns20   #G j ;  T]T_ж_ж?&Rv)S b0.29 #G j 9  TWT_ж_ж ?"` R&S h Rub.nscp01   #G j 6  ThoT_ж_ж?&Sv)5U b0.40 #G j 4  T|wT_ж_ж ?"` S&5U h Rub.nscp02   #G j 1  T\yT_ж_ж?&5Uv)V b0.31 #G j /  T\T_ж_ж ?"` 5U&V h Rub.nscp04   #G j   TT_ж_ж?&Ov)'Q b0.94 #G j   T T_ж_ж? O&'Q fRub.ns15   #G j   TT_ж_ж?&sNv)O b0.96 #G j   T̮T_ж_ж? sN&O fRub.ns10   #G j !  TT_ж_ж?&Mv)sN b1.75 #G j "  TT_ж_ж? M&sN fRub.ns00   #G jC #   fT_ж_ж^d?" &Kv)M In/IwN   #G j $   fhT_ж_ж5d?"  K&M dsample #G jZB %  s *> ? sNv)sNZB &  s *> ? Ov)OZB '  s *> ? 'Qv)'QZB (  s *> ?&K&VZB )  s *> ? Mv)M`B *  0> ? Kv)K`B +  0> ? K V`B ,  0> ?v)Kv)V`B -  0> ? Vv)VZB 5  s *> ? 5Uv)5UZB :  s *> ? Sv)SZB @  s *> ? Rv)R I 0T.B9F8E \Table 3. The intensities ratio of narrow and wide component of ESR spectra measured at 10C.$] 2U ]  U 0TB E cThe amount of nanosilica in all samples containing the coupling agent was similar and equal 10 phr.d 2d d V 0TT]a&c BESR spectrometar : Varian E-109 Temperature unit Bruker ER 4111 VTCC C f  <A ??"`- -* x n  <A ??0z/:@ ) o 0lTZ8JH9a Z. Veksli, M Andreis, B. Rakvin, Prog Polym. Sci. 25 (2000) 949. G. Jeschke et al., Polymer Engineering and Science 44 (2004) 1112. 2 R p 0TZ<6e ESR spectra show a significant influence of nanosilica on the local chain dynamics. The increase in the nanosilica amount leads to the decrease in segmental motions. The coupling agent makes the role of nanosilica more pronounced. Because of the better contact between the matrix chain segment and nanosilica particles, the restriction in local motions become more and more important as the amount of coupling agent increases.(2 f v 0A?"`]U5}F)<   A "`1E\-8N  0TN8O Ia) without coupling agent b) with the coupling agent"J 2I,  G  0DUQ"4T }Figure 5. Schematic presentation of rubber matrices with the same crosslink densities and the same amount of the nanosilica. &~(2 u g    0U*MBxHN : 2 X  0A?f/H7D9f  C >A$logotip%20zaklade Q@F0Z  ) #q   #" 1E ,N n =w  3 #"  ) #qB   B&CDE|F45%Yv*FFHVfXv8VV&*Z(t8@          "`) KO    B CDEFh5%FFT H XhThhD4:X$ ` ` $ Zb<D,$      v  * @ 8 t V$ 8p4ff8(DrhtZhJ814@                       "` _   tBCz DEFP5%44 { ZN <  < x2 ,    @ * N X  z t\ (> T  ^ rP  F` ~ $ v4XDrtTF6DD8b*vV *  h fx%(@                 "`U ="   B C DE$Fl5%IIB ` p~  &` $ 6prB TP T    P 4` 4bf V n  & P 4 |    8 * 0     ~ :` B , ` x$ p<h(t:XHvX:8VtJxV<<34@                        "`s w>   BC DE0Fp5%LLuV( t8 f ,x:<H<xV,VV8  Hh <Ht< (F (HF6Df:D,HB   n  V  P    ` $ U 58@                         3"`    dBCDEFL5%11;vZX Z  vX::*Xv 8**F TXTTJZ<Tb<xRp:Hp8tTU#$@                "`Y #   B(CDEXF(5%uZf<<8xt, 8H Hth(@       3"` aMV2   C "` V2   C "`L?V2   C "`UdHHV2   C "`&rWV2   C "`K0V2   C "`V2   C "`V2   C "`~pV2   C "`>F1(V2   C "`th   c LA (1Small checker board"`lk   c LA (1Small checker board"`ED   c LA (1Small checker board"`]\   c LA (1Small checker board"`   c LA (1Small checker board"`{%z$   c LA (1Small checker board"`ON   c LA (1Small checker board"`UT   c LA (1Small checker board"`!"   c LA (1Small checker board"`   c LA (1Small checker board"`   c LA (1Small checker board"`  H  0U<܍ ? 3380___PPT10.@[r֑  ?     (kJmiw   ACorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 GraphicCorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 Graphic SPW 10.0 Graph 0SigmaPlotGraphicObject.90(SigmaPlot 10.0 Graph SPW 10.0 Graph 0SigmaPlotGraphicObject.90(SigmaPlot 10.0 GraphD/ 0|DArialhA .0z[ 0DTimes New Roman0z[ 0 DGaramond Roman0z[ 00DSymbold Roman0z[ 0@DWP MathA Roman0z[ 0@ . @n?" dd@  @@`` P 212$V0,Hw6"$gqN,WGְdEh36"$vHηΈ={>cUH 2$],ֽ4 P R$D<$*q 2$ _s8) \k= 2$Z&$(WkBAc  2$C^g¿pSK;&~ r$߀M'$,,Gi 2$fAζg6K/!m*5$2$ : H=>X񭑹Wa  0AAP3@<ʚ;ʚ;g4!d!d z[ 0p:@p<<4ddddL 0. A0___PPT10 pp___PPT9n^,֋S#ޠ"PNG  IHDRF}sRGB PLTE3*ծ cmPPJCmp0712 7tRNS@f8IDATWc``d !$$<[UBS#BT     B`S5G^" `-Am Q Objective (2 6   BS5G^" `V A" Q Materials (2 6   BTS5G^" `AFAH ZSample preparation(26   BT5G^" `QA3T OMethods(26   B/S5G^" `4C? OResults(26    03S^D<4___PPT9 ]Investigation of the NR samples containg different amounts of the nanosilica particles and their influence on local chain dynamics. Influence of a coupling agent on the changes in matrix structure and chain dynamics.@! U! 8X  0@S<$ V& JTable 1. Samples of NR with different amounts of nanosilica"KC Kt nB*]D3 l  #"&<WVWV'aP0 $ TMS_ж_ж? 1]D3 `20 #G j # T4S_ж_ж?n1 D3 fRub.ns20   #G j " T^S_ж_ж? 0]1 `15 #G j ! TWS_ж_ж?n0 1 fRub.ns15   #G j   ToS_ж_ж? 6/]0 `10 #G j  TxS_ж_ж?n6/ 0 fRub.ns10   #G j  TS_ж_ж? -]6/ _0 #G j  T@S_ж_ж?n- 6/ fRub.ns00   #G j(   fS_ж_ж^d?"  B*]- |The amount of nanosilica / phr #G j   fXS_ж_ж5d?" nB* - e sample #G jZB ' s *> ?n6/]6/ZB ( s *> ?n0]0ZB ) s *> ?n1]1ZB , s *> ? B* D3ZB & s *> ?n-]-`B % 0> ?nB*]B*`B + 0> ?nB*nD3`B - 0> ?]B*]D3`B * 0> ?nD3]D3  0Si2 4 @The average diametar of the used nanosilica particles was 13 nm.A 2A A  0S5 A8 RTable 2. NR samples with different amounts of coupling agent (Si 69)"SK S p ^:@C j  #""a$93zA  TS_ж_ж?5 A@C _4 #G j  TS_ж_ж?^A5 @C h Rub.nscp04   #G j  TS_ж_ж?5 @A _2 #G j  TS_ж_ж?^@5 A h Rub.nscp02   #G j  TS_ж_ж?5 >@ _1 #G j  TS_ж_ж?^>5 @ h Rub.nscp01   #G j,   fS_ж_ж^d?" 5 :> "The amount of coupling agent / phr## ##G j   fS_ж_ж5d?" ^:5 > q sample& #G jZB   s *> ?^@@ZB   s *> ?^AAZB   s *> ?5 :5 @CZB   s *> ?^>>`B   0> ?^::`B   0> ?^:^@C`B   0> ?:@C`B   0> ?^@C@C  0T'J{c!QD<4___PPT9 Two-roll mixing folowed by compression moulding. Swelling in the toluene probe solution at the constant temperature (35C). Removing the solvent by evaporationand annealing at 60 C during tree days.6!  8X*  0DTWZ] ESR  spin probe method probe amount in the samples was 0.15 wt% DD D4  # A#U~ ^  0("TZ^{6_ ,4-hydroy-2,2,6,6-tetramethylpiperidin-1-oxyl- 2- # XB  0D)wkJw  B'T5G^" `W|/Y R Conclusion (2 6   B +T5G^" `W7hGY S References  (2 6   0.T%+3KH?- \Figure 2. ESR spectra of samples containing different amount of nanosilica measured at 10C.$] 2 T ]  0(-T;5F> jFigure 4. Temperature dependence of the outer extrema (2Azz) of ESR spectra for Rub.ns10 (L) and Rub.nscp04 (%).Zr(2 0   r3  0\:TA_0(D Figure 3. ESR spectra of samples containing the same amount of nanosilica and various amounts of coupling agent measured at 10C.$ 2 y !  08=T+L1. mFigure 1. ESR spectra of the spin probe diffusing in the matrix of Rub.ns00 sample at different temperatures.&n(2 e nw  Kv)V   #"2&F;eDS A  TDT_ж_ж ?"`&'Qv)R b0.92 #G j ?  TST_ж_ж ?"` 'Q&R fRub.ns20   #G j ;  T]T_ж_ж?&Rv)S b0.29 #G j 9  TWT_ж_ж ?"` R&S h Rub.nscp01   #G j 6  ThoT_ж_ж?&Sv)5U b0.40 #G j 4  T|wT_ж_ж ?"` S&5U h Rub.nscp02   #G j 1  T\yT_ж_ж?&5Uv)V b0.31 #G j /  T\T_ж_ж ?"` 5U&V h Rub.nscp04   #G j   TT_ж_ж?&Ov)'Q b0.94 #G j   T T_ж_ж? O&'Q fRub.ns15   #G j   TT_ж_ж?&sNv)O b0.96 #G j   T̮T_ж_ж? sN&O fRub.ns10   #G j !  TT_ж_ж?&Mv)sN b1.75 #G j "  TT_ж_ж? M&sN fRub.ns00   #G jC #   fT_ж_ж^d?" &Kv)M In/IwN   #G j $   fhT_ж_ж5d?"  K&M dsample #G jZB %  s *> ? sNv)sNZB &  s *> ? Ov)OZB '  s *> ? 'Qv)'QZB (  s *> ?&K&VZB )  s *> ? Mv)M`B *  0> ? Kv)K`B +  0> ? K V`B ,  0> ?v)Kv)V`B -  0> ? Vv)VZB 5  s *> ? 5Uv)5UZB :  s *> ? Sv)SZB @  s *> ? Rv)R I 0T.B9F8E \Table 3. The intensities ratio of narrow and wide component of ESR spectra measured at 10C.$] 2U ]  U 0TB E cThe amount of nanosilica in all samples containing the coupling agent was similar and equal 10 phr.d 2d d V 0TT]a&c BESR spectrometar : Varian E-109 Temperature unit Bruker ER 4111 VTCC C f  <A ??"`- -* x n  <A ??0z/:@ ) o 0lTZ8JH9a Z. Veksli, M Andreis, B. Rakvin, Prog Polym. Sci. 25 (2000) 949. G. Jeschke et al., Polymer Engineering and Science 44 (2004) 1112. 2 R p 0TZ<6e ESR spectra show a significant influence of nanosilica on the local chain dynamics. The increase in the nanosilica amount leads to the decrease in segmental motions. The coupling agent makes the role of nanosilica more pronounced. Because of the better contact between the matrix chain segment and nanosilica particles, the restriction in local motions become more and more important as the amount of coupling agent increases.(2 f v 0A?"`]U5}F)<   A "`1E\-8N  0TN8O Ia) without coupling agent b) with the coupling agent"J 2I,  G  0DUQ"4T }Figure 5. Schematic presentation of rubber matrices with the same crosslink densities and the same amount of the nanosilica. &~(2 u g    0U*MBxHN : 2 X  0A?f/H7D9f  C >A$logotip%20zaklade Q@F0Z  ) #q   #" 1E ,N n =w  3 #"  ) #qB   B&CDE|F45%Yv*FFHVfXv8VV&*Z(t8@          "`) KO    B CDEFh5%FFT H XhThhD4:X$ ` ` $ Zb<D,$      v  * @ 8 t V$ 8p4ff8(DrhtZhJ814@                       "` _   tBCz DEFP5%44 { ZN <  < x2 ,    @ * N X  z t\ (> T  ^ rP  F` ~ $ v4XDrtTF6DD8b*vV *  h fx%(@                 "`U ="   B C DE$Fl5%IIB ` p~  &` $ 6prB TP T    P 4` 4bf V n  & P 4 |    8 * 0     ~ :` B , ` x$ p<h(t:XHvX:8VtJxV<<34@                        "`s w>   BC DE0Fp5%LLuV( t8 f ,x:<H<xV,VV8  Hh <Ht< (F (HF6Df:D,HB   n  V  P    ` $ U 58@                         3"`    dBCDEFL5%11;vZX Z  vX::*Xv 8**F TXTTJZ<Tb<xRp:Hp8tTU#$@                "`Y #   B(CDEXF(5%uZf<<8xt, 8H Hth(@       3"` aMV2   C "` V2   C "`L?V2   C "`UdHHV2   C "`&rWV2   C "`K0V2   C "`V2   C "`V2   C "`~pV2   C "`>F1(V2   C "`th   c LA (1Small checker board"`lk   c LA (1Small checker board"`ED   c LA (1Small checker board"`]\   c LA (1Small checker board"`   c LA (1Small checker board"`{%z$   c LA (1Small checker board"`ON   c LA (1Small checker board"`UT   c LA (1Small checker board"`!"   c LA (1Small checker board"`   c LA (1Small checker board"`   c LA (1Small checker board"`  H  0U<܍ ? 3380___PPT10.@[r  ?    (kJmiw   ACorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 GraphicCorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 Graphic SPW 10.0 Graph 0SigmaPlotGraphicObject.90(SigmaPlot 10.0 Graph SPW 10.0 Graph 0SigmaPlotGraphicObject.90(SigmaPlot 10.0 GraphD/ 0|DArialhA .0z[ 0DTimes New Roman0z[ 0 DGaramond Roman0z[ 00DSymbold Roman0z[ 0@DWP MathA Roman0z[ 0@ . @n?" dd@  @@`` P 212$V0,Hw6"$gqN,WGְdEh36"$vHηΈ={>cUH 2$],ֽ4 P R$D<$*q 2$ _s8) \k= 2$Z&$(WkBAc  2$C^g¿pSK;&~ r$߀M'$,,Gi 2$fAζg6K/!m*5$2$ : H=>X񭑹Wa  0AAP3@<ʚ;ʚ;g4!d!d z[ 0"p:@p<<4ddddL 0. A0___PPT10 pp___PPT9n^,֋S#ޠ"PNG  IHDRF}sRGB PLTE3*ծ cmPPJCmp0712 7tRNS@f8IDATWc``d !$$<[UBS#BT     B`S5G^" `-Am Q Objective (2 6   BS5G^" `V A" Q Materials (2 6   BTS5G^" `AFAH ZSample preparation(26   BT5G^" `QA3T OMethods(26   B/S5G^" `4C? OResults(26    03S^D<4___PPT9 ]Investigation of the NR samples containg different amounts of the nanosilica particles and their influence on local chain dynamics. Influence of a coupling agent on the changes in matrix structure and chain dynamics.@! U! 8X  0@S<$ V& JTable 1. Samples of NR with different amounts of nanosilica"KC Kt nB*]D3 l  #"&<WVWV'aP0 $ TMS_ж_ж? 1]D3 `20 #G j # T4S_ж_ж?n1 D3 fRub.ns20   #G j " T^S_ж_ж? 0]1 `15 #G j ! TWS_ж_ж?n0 1 fRub.ns15   #G j   ToS_ж_ж? 6/]0 `10 #G j  TxS_ж_ж?n6/ 0 fRub.ns10   #G j  TS_ж_ж? -]6/ _0 #G j  T@S_ж_ж?n- 6/ fRub.ns00   #G j(   fS_ж_ж^d?"  B*]- |The amount of nanosilica / phr #G j   fXS_ж_ж5d?" nB* - e sample #G jZB ' s *> ?n6/]6/ZB ( s *> ?n0]0ZB ) s *> ?n1]1ZB , s *> ? B* D3ZB & s *> ?n-]-`B % 0> ?nB*]B*`B + 0> ?nB*nD3`B - 0> ?]B*]D3`B * 0> ?nD3]D3  0Si2 4 @The average diametar of the used nanosilica particles was 13 nm.A 2A A  0S5 A8 RTable 2. NR samples with different amounts of coupling agent (Si 69)"SK S p ^:@C j  #""a$93zA  TS_ж_ж?5 A@C _4 #G j  TS_ж_ж?^A5 @C h Rub.nscp04   #G j  TS_ж_ж?5 @A _2 #G j  TS_ж_ж?^@5 A h Rub.nscp02   y Leki1, S. Vali1,2, A.P. Meera3 and S. Thomas3 1 University of Rijeka, School of Medicine, Brae Branchetta 20, Rijeka, 51000, Croatia 2 Rudjer Boakovi Institute, Bijeni ka 54, Zagreb,10000, Croatia 3 Mahatma Gandhi University, School of Chemical Sc#G j  TS_ж_ж?5 >@ _1 #G j  TS_ж_ж?^>5 @ h Rub.nscp01   #G j,   fS_ж_ж^d?" 5 :> "The amount of coupling agent / phr## ##G j   fS_ж_ж5d?" ^:5 > q sample& #G jZB   s *> ?^@@ZB   s *> ?^AAZB   s *> ?5 :5 @CZB   s *> ?^>>`B   0> ?^::`B   0> ?^:^@C`B   0> ?:@C`B   0> ?^@C@C  0T'J{c!QD<4___PPT9 Two-roll mixing folowed by compression moulding. Swelling in the toluene probe solution at the constant temperature (35C). Removing the solvent by evaporationand annealing at 60 C during tree days.6!  8X*  0DTWZ] ESR  spin probe method probe amount in the samples was 0.15 wt% DD D4  # A#U~ ^  0("TZ^{6_ ,4-hydroy-2,2,6,6-tetramethylpiperidin-1-oxyl- 2- # XB  0D)wkJw  B'T5G^" `W|/Y R Conclusion (2 6   B +T5G^" `W7hGY S References  (2 6   0.T%+3KH?- \Figure 2. ESR spectra of samples containing different amount of nanosilica measured at 10C.$] 2 T ]  0(-T;5F> jFigure 4. Temperature dependence of the outer extrema (2Azz) of ESR spectra for Rub.ns10 (L) and Rub.nscp04 (%).Zr(2 0   r3  0\:TA_0(D Figure 3. ESR spectra of samples containing the same amount of nanosilica and various amounts of coupling agent measured at 10C.$ 2 y !  08=T+L1. mFigure 1. ESR spectra of the spin probe diffusing in the matrix of Rub.ns00 sample at different temperatures.&n(2 e nw  Kv)V   #"2&F;eDS A  TDT_ж_ж ?"`&'Qv)R b0.92 #G j ?  TST_ж_ж ?"` 'Q&R fRub.ns20   #G j ;  T]T_ж_ж?&Rv)S b0.29 #G j 9  TWT_ж_ж ?"` R&S h Rub.nscp01   #G j 6  ThoT_ж_ж?&Sv)5U b0.40 #G j 4  T|wT_ж_ж ?"` S&5U h Rub.nscp02   #G j 1  T\yT_ж_ж?&5Uv)V b0.31 #G j /  T\T_ж_ж ?"` 5U&V h Rub.nscp04   #G j   TT_ж_ж?&Ov)'Q b0.94 #G j   T T_ж_ж? O&'Q fRub.ns15   #G j   TT_ж_ж?&sNv)O b0.96 #G j   T̮T_ж_ж? sN&O fRub.ns10   #G j !  TT_ж_ж?&Mv)sN b1.75 #G j "  TT_ж_ж? M&sN fRub.ns00   #G jC #   fT_ж_ж^d?" &Kv)M In/IwN   #G j $   fhT_ж_ж5d?"  K&M dsample #G jZB %  s *> ? sNv)sNZB &  s *> ? Ov)OZB '  s *> ? 'Qv)'QZB (  s *> ?&K&VZB )  s *> ? Mv)M`B *  0> ? Kv)K`B +  0> ? K V`B ,  0> ?v)Kv)V`B -  0> ? Vv)VZB 5  s *> ? 5Uv)5UZB :  s *> ? Sv)SZB @  s *> ? Rv)R I 0T.B9F8E \Table 3. The intensities ratio of narrow and wide component of ESR spectra measured at 10C.$] 2U ]  U 0TB E cThe amount of nanosilica in all samples containing the coupling agent was similar and equal 10 phr.d 2d d V 0TT]a&c BESR spectrometar : Varian E-109 Temperature unit Bruker ER 4111 VTCC C f  <A ??"`- -* x n  <A ??0z/:@ ) o 0lTZ8JH9a Z. Veksli, M Andreis, B. Rakvin, Prog Polym. Sci. 25 (2000) 949. G. Jeschke et al., Polymer Engineering and Science 44 (2004) 1112. 2 R p 0TZ<6e ESR spectra show a significant influence of nanosilica on the local chain dynamics. The increase in the nanosilica amount leads to the decrease in segmental motions. The coupling agent makes the role of nanosilica more pronounced. Because of the better contact between the matrix chain segment and nanosilica particles, the restriction in local motions become more and more important as the amount of coupling agent increases.(2 f v 0A?"`]U5}F)<   A "`1E\-8N  0TN8O Ia) without coupling agent b) with the coupling agent"J 2I,  G  0DUQ"4T }Figure 5. Schematic presentation of rubber matrices with the same crosslink densities and the same amount of the nanosilica. &~(2 u g    0U*MBxHN : 2 X  0A?f/H7D9f  C >A$logotip%20zaklade Q@F0Z  ) #q   #" 1E ,N n =w  3 #"  ) #qB   B&CDE|F45%Yv*FFHVfXv8VV&*Z(t8@          "`) KO    B CDEFh5%FFT H XhThhD4:X$ ` ` $ Zb<D,$      v  * @ 8 t V$ 8p4ff8(DrhtZhJ814@                       "` _   tBCz DEFP5%44 { ZN <  < x2 ,    @ * N X  z t\ (> T  ^ rP  F` ~ $ v4XDrtTF6DD8b*vV *  h fx%(@                 "`U ="   B C DE$Fl5%IIB ` p~  &` $ 6prB TP T    P 4` 4bf V n  & P 4 |    8 * 0     ~ :` B , ` x$ p<h(t:XHvX:8VtJxV<<34@                        "`s w>   BC DE0Fp5%LLuV( t8 f ,x:<H<xV,VV8  Hh <Ht< (F (HF6Df:D,HB   n  V  P    ` $ U 58@                         3"`    dBCDEFL5%11;vZX Z  vX::*Xv 8**F TXTTJZ<Tb<xRp:Hp8tTU#$@                "`Y #   B(CDEXF(5%uZf<<8xt, 8H Hth(@       3"` aMV2   C "` V2   C "`L?V2   C "`UdHHV2   C "`&rWV2   C "`K0V2   C "`V2   C "`V2   C "`~pV2   C "`>F1(V2   C "`th   c LA (1Small checker board"`lk   c LA (1Small checker board"`ED   c LA (1Small checker board"`]\   c LA (1Small checker board"`   c LA (1Small checker board"`{%z$   c LA (1Small checker board"`ON   c LA (1Small checker board"`UT   c LA (1Small checker board"`!"   c LA (1Small checker board"`   c LA (1Small checker board"`   c LA (1Small checker board"`  H  0U<܍ ? 3380___PPT10.@[r  ? ֍   (kJmiw   ACorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 GraphicCorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 Graphic SPW 10.0 Graph 0SigmaPlotGraphicObject.90(SigmaPlot 10.0 Graph SPW 10.0 Graph 0SigmaPlotGraphicObject.90(SigmaPlot 10.0 GraphD/ 0|DArialhA .0z[ 0DTimes New Roman0z[ 0 DGaramond Roman0z[ 00DSymbold Roman0z[ 0@DWP MathA Roman0z[ 0@ . @n?" dd@  @@`` P 212$V0,Hw6"$gqN,WGְdEh36"$vHηΈ={>cUH 2$],ֽ4 P R$D<$*q 2$ _s8) \k= 2$Z&$(WkBAc  2$C^g¿pSK;&~ r$߀M'$,,Gi 2$fAζg6K/!m*5$2$ : H=>X񭑹Wa  0AAP3@<ʚ;ʚ;g4dddd z[ 06/p:@p<<4ddddL 0. A0___PPT10 pp___PPT9n^,֋S#ޠ"PNG  IHDRF}sRGB PLTE3*ծ cmPPJCmp0712 7tRNS@f8IDATWc``d !$$<[UBS#BT     B`S5G^" `-Am Q Objective (2 6   BS5G^" `V A" Q Materials (2 6   BTS5G^" `AFAH ZSample preparation(26   BT5G^" `QA3T OMethods(26   B/S5G^" `4C? OResults(26    03S^D<4___PPT9 ]Investigation of the NR samples containg different amounts of the nanosilica particles and their influence on local chain dynamics. Influence of a coupling agent on the changes in matrix structure and chain dynamics.@! U! 8X  0@S<$ V& JTable 1. Samples of NR with different amounts of nanosilica"KC Kt nB*]D3 l  #"&<WVWV'aP0 $ TMS_ж_ж? 1]D3 `20 #G j # T4S_ж_ж?n1 D3 fRub.ns20   #G j " T^S_ж_ж? 0]1 `15 #G j ! TWS_ж_ж?n0 1 fRub.ns15   #G j   ToS_ж_ж? 6/]0 `10 #G j  TxS_ж_ж?n6/ 0 fRub.ns10   #G j  TS_ж_ж? -]6/ _0 #G j  T@S_ж_ж?n- 6/ fRub.ns00   #G j(   fS_ж_ж^d?"  B*]- |The amount of nanosilica / phr #G j   fXS_ж_ж5d?" nB* - e sample #G jZB ' s *> ?n6/]6/ZB ( s *> ?n0]0ZB ) s *> ?n1]1ZB , s *> ? B* D3ZB & s *> ?n-]-`B % 0> ?nB*]B*`B + 0> ?nB*nD3`B - 0> ?]B*]D3`B * 0> ?nD3]D3  0Si2 4 @The average diametar of the used nanosilica particles was 13 nm.A 2A A  0S5 A8 RTable 2. NR samples with different amounts of coupling agent (Si 69)"SK S p ^:@C j  #""a$93zA  TS_ж_ж?5 A@C _4 #G j  TS_ж_ж?^A5 @C h Rub.nscp04   #G j  TS_ж_ж?5 @A _2 #G j  TS_ж_ж?^@5 A h Rub.nscp02   #G j  TS_ж_ж?5 >@ _1 #G j  TS_ж_ж?^>5 @ h Rub.nscp01   #G j,   fS_ж_ж^d?" 5 :> "The amount of coupling agent / phr## ##G j   fS_ж_ж5d?" ^:5 > q sample& #G jZB   s *> ?^@@ZB   s *> ?^AAZB   s *> ?5 :5 @CZB   s *> ?^>>`B   0> ?^::`B   0> ?^:^@C`B   0> ?:@C`B   0> ?^@C@C  0T'J{c!QD<4___PPT9 Two-roll mixing folowed by compression moulding. Swelling in the toluene probe solution at the constant temperature (35C). Removing the solvent by evaporationand annealing at 60 C during tree days.6!  8X*  0DTWZ] ESR  spin probe method probe amount in the samples was 0.15 wt% DD D4  # A#U~ ^  0("TZ^{6_ ,4-hydroy-2,2,6,6-tetramethylpiperidin-1-oxyl- 2- # XB  0D)wkJw  B'T5G^" `W|/Y R Conclusion (2 6   B +T5G^" `W7hGY S References  (2 6   0.T%+3KH?- \Figure 2. ESR spectra of samples containing different amount of nanosilica measured at 10C.$] 2 T ]  0(-T;5F> jFigure 4. Temperature dependence of the outer extrema (2Azz) of ESR spectra for Rub.ns10 (L) and Rub.nscp04 (%).Zr(2 0   r3  0\:TA_0(D Figure 3. ESR spectra of samples containing the same amount of nanosilica and various amounts of coupling agent measured at 10C.$ 2 y !  08=T+L1. mFigure 1. ESR spectra of the spin probe diffusing in the matrix of Rub.ns00 sample at different temperatures.&n(2 e nw  Kv)V   #"2&F;eDS A  TDT_ж_ж ?"`&'Qv)R b0.92 #G j ?  TST_ж_ж ?"` 'Q&R fRub.ns20   #G j ;  T]T_ж_ж?&Rv)S b0.29 #G j 9  TWT_ж_ж ?"` R&S h Rub.nscp01   #G j 6  ThoT_ж_ж?&Sv)5U b0.40 #G j 4  T|wT_ж_ж ?"` S&5U h Rub.nscp02   #G j 1  T\yT_ж_ж?&5Uv)V b0.31 #G j /  T\T_ж_ж ?"` 5U&V h Rub.nscp04   #G j   TT_ж_ж?&Ov)'Q b0.94 #G j   T T_ж_ж? O&'Q fRub.ns15   #G j   TT_ж_ж?&sNv)O b0.96 #G j   T̮T_ж_ж? sN&O fRub.ns10   #G j !  TT_ж_ж?&Mv)sN b1.75 #G j "  TT_ж_ж? M&sN fRub.ns00   #G jC #   fT_ж_ж^d?" &Kv)M In/IwN   #G j $   fhT_ж_ж5d?"  K&M dsample #G jZB %  s *> ? sNv)sNZB &  s *> ? Ov)OZB '  s *> ? 'Qv)'QZB (  s *> ?&K&VZB )  s *> ? Mv)M`B *  0> ? Kv)K`B +  0> ? K V`B ,  0> ?v)Kv)V`B -  0> ? Vv)VZB 5  s *> ? 5Uv)5UZB :  s *> ? Sv)SZB @  s *> ? Rv)R I 0T.B9F8E \Table 3. The intensities ratio of narrow and wide component of ESR spectra measured at 10C.$] 2U ]  U 0TB E cThe amount of nanosilica in all samples containing the coupling agent was similar and equal 10 phr.d 2d d V 0TT]a&c BESR spectrometar : Varian E-109 Temperature unit Bruker ER 4111 VTCC C f  <A ??"`- -* x n  <A ??0z/:@ ) o 0lTZ8JH9a Z. Veksli, M Andreis, B. Rakvin, Prog Polym. Sci. 25 (2000) 949. G. Jeschke et al., Polymer Engineering and Science 44 (2004) 1112. 2 R p 0TZ<6e ESR spectra show a significant influence of nanosilica on the local chain dynamics. The increase in the nanosilica amount leads to the decrease in segmental motions. The coupling agent makes the role of nanosilica more pronounced. Because of the better contact between the matrix chain segment and nanosilica particles, the restriction in local motions become more and more important as the amount of coupling agent increases.(2 f v 0A?"`]U5}F)<   A "`1E\-8N  0TN8O Ia) without coupling agent b) with the coupling agent"J 2I,  G  0DUQ"4T }Figure 5. Schematic presentation of rubber matrices with the same crosslink densities and the same amount of the nanosilica. &~(2 u g    0U*MBxHN : 2 X  0A?f/H7D9f  C >A$logotip%20zaklade Q@F0Z  ) #q   #" 1E ,N n =w  3 #"  ) #qB   B&CDE|F45%Yv*FFHVfXv8VV&*Z(t8@          "`) KO    B CDEFh5%FFT H XhThhD4:X$ ` ` $ Zb<D,$      v  * @ 8 t V$ 8p4ff8(DrhtZhJ814@                       "` _   tBCz DEFP5%44 { ZN <  < x2 ,    @ * N X  z t\ (> T  ^ rP  F` ~ $ v4XDrtTF6DD8b*vV *  h fx%(@                 "`U ="   B C DE$Fl5%IIB ` p~  &` $ 6prB TP T    P 4` 4bf V n  & P 4 |    8 * 0     ~ :` B , ` x$ p<h(t:XHvX:8VtJxV<<34@                        "`s w>   BC DE0Fp5%LLuV( t8 f ,x:<H<xV,VV8  Hh <Ht< (F (HF6Df:D,HB   n  V  P    ` $ U 58@                         3"`    dBCDEFL5%11;vZX Z  vX::*Xv 8**F TXTTJZ<Tb<xRp:Hp8tTU#$@                "`Y #   B(CDEXF(5%uZf<<8xt, 8H Hth(@       3"` aMV2   C "` V2   C "`L?V2   C "`UdHHV2   C "`&rWV2   C "`K0V2   C "`V2   C "`V2   C "`~pV2   C "`>F1(V2   C "`th   c LA (1Small checker board"`lk   c LA (1Small checker board"`ED   c LA (1Small checker board"`]\   c LA (1Small checker board"`   c LA (1Small checker board"`{%z$   c LA (1Small checker board"`ON   c LA (1Small checker board"`UT   c LA (1Small checker board"`!"   c LA (1Small checker board"`   c LA (1Small checker board"`   c LA (1Small checker board"`  H  0U<܍ ? 3380___PPT10.@[r  ?    (kJmiw   ECorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 GraphicCorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 Graphic9wֻ,F̝sfv"`]:\\Bˍ-M!&G6"п<KyOZ7ymYmN(,{MBJLU}ZB5+&AKRw/4"кRϊ秶Z*^4lK(~QOd>2Ozrӷ0Xl&n;6ƬKR_gڞu[G;RU]d_UGڪe#>Kc67hdi=q].k4鲶jh_E~XJgpyeD915"iW4)#aihNwD+)[*,!{*nm~N}oUғ/ VL\VM C׿??}vLWXcTicG<0F66ƨ:1u\{D̯'ՒU #3avF\g6TSyM*yz^sSHe7gԔ+*ANyX 'D&s%$Ԓ$ԒHjIWjI$ + $ZҕZIB-JRKIgu3K+, 9dڦvg #Sp'WzLCRA3|iܾRDFHWh_~#y6ֽgCӬt;cݱio9>vJ= ь&^ь& &iF:Vlhk!/9 cݱ'OBVmyb]OgcyѮ8{;$87ciTqL␸QiS,Il6yU_q=VzƴK9uۯnrM{>n#sWgy{ݩn^\,#'gkޓ$}s4vW3A<7S=N{θ',{r9Qd+O+OꨭQa/O{Ux{9nGya޳٨q'LGsӸLGs![zkըV5?Ar$3H׺&Su̯ C]_+((S.)kZM^`!Q~x<lǒd4t9q.i𭕯,k>ߖsz֩(߫Wm"/gѿc8G(X%GlN P :#F(VF[E: p?R'@at!O(b[FyG'@ak}쒼Ǜ%Z7~}y+}&PpĮ0z6f}#: 1*R0tFp5Gz^'@a49"GY P\J/'+ kW"#4⨁pAFLw.#Nl*f#";Ev AFd? hTi<O2W 'TiKNhgD;#>3E ҈e"O` F2S% J@x #0+Q*hpyFgD@ԸJ#peF\fD@zqK@,Kq7|բSg9O -b3#63bfD5#$!2Bdĥ9cQF{ Fa" Ɉ"4/!@H4-haDX͈Ռ2190:m N1#6[OٌR( 2O\kX_bˈXl 1b#8( /0#3bU+ID P88D 9 (:v8A"JhSo0㈧HJ/ #rĿHD P!E".LW-wa/0*211F|qD^|yDϔDQLjqIPHD PA"Jhr&[AaTm f1b#D9NQFcqDў`#v0Zh 0b#F#QD"JV 0Q]ǿ]NcUH 2$],ֽ4 P R$D<$*q 2$ _s8) \k= $2$C^g¿pSK;&~ r$߀M'$,,Gi 2$fAζg6K/!m*52$s%dgZ1RV f2$ : H=>X񭑹Wa  0AAP3@<ʚ;ʚ;g4!d!d z[ 0X p:@p<<4ddddL 0. A0___PPT10 pp___PPT9n^,֋S#ޠ"PNG  IHDRF}sRGB PLTE3*ծ cmPPJCmp0712 7tRNS@f8IDATWc``d !$$<[UBS#BT     BLS5G^" `-Am Q Objective (2 6   BS5G^" `V A" Q Materials (2 6   BS5G^" `AFAH ZSample preparation(26   Bp#S5G^" `QA3T OMethods(26   BS5G^" `4C? OResults(26    0$5S^D<4___PPT9 ]Investigation of the NR samples containg different amounts of the nanosilica particles and their influence on local chain dynamics. Influence of a coupling agent on the changes in matrix structure and chain dynamics.@! U! 8X  0(AS<$ V& JTable 1. Samples of NR with different amounts of nanosilica"KC Kt nB*]D3 l  #"&<WVWV'aP0 $ T_ж_ж? 1]D3 `20 #G j # TxVS_ж_ж?n1 D3 fRub.ns20   #G j " THS_ж_ж? 0]1 `15 #G j ! ThS_ж_ж?n0 1 fRub.ns15   #G j   TYS_ж_ж? 6/]0 `10 #G j  T ?n6/]6/ZB ( s *> ?n0]0ZB ) s *> ?n1]1ZB , s *> ? B* D3ZB & s *> ?n-]-`B % 0> ?nB*]B*`B + 0> ?nB*nD3`B - 0> ?]B*]D3`B * 0> ?nD3]D3  0Si2 4 @The average diametar of the used nanosilica particles was 13 nm.A 2A A  0S5 A8 RTable 2. NR samples with different amounts of coupling agent (Si 69)"SK S p ^:@C j  #""a$93zA  T,S_ж_ж?5 A@C _4 #G j  TS_ж_ж?^A5 @C h Rub.nscp04   #G j  TS_ж_ж?5 @A _2 #G j  TS_ж_ж?^@5 A h Rub.nscp02   #G j  T\S_ж_ж?5 >@ _1 #G j  T5 @ h Rub.nscp01       !"#$%&'()*+,-./0123456789:;<=>?@ABCDEFGHIJKLMNOPQRSTUVWXYZ[\]^_`abcdefghijklmnopqrstuvwxyz{|~  #G j,   fS_ж_ж^d?" 5 :> "The amount of coupling agent / phr## ##G j   f4S_ж_ж5d?" ^:5 > q sample& #G jZB   s *> ?^@@ZB   s *> ?^AAZB   s *> ?5 :5 @CZB   s *> ?^>>`B   0> ?^::`B   0> ?^:^@C`B   0> ?:@C`B   0> ?^@C@C  0T'J{c!QD<4___PPT9 Two-roll mixing folowed by compression moulding. Swelling in the toluene probe solution at the constant temperature (35C). Removing the solvent by evaporationand annealing at 60 C during tree days.6!  8X*  0 TWZ] ESR  spin probe method probe amount in the samples was 0.15 wt% DD D4  # A#U~ ^  0SZ^{6_ ,4-hydroy-2,2,6,6-tetramethylpiperidin-1-oxyl- 2- # XB  0D)wkJw  BT5G^" `W|/Y R Conclusion (2 6   B T5G^" `W7hGY S References  (2 6   0 T%+3KH?- \Figure 2. ESR spectra of samples containing different amount of nanosilica measured at 10C.$] 2 T ]  0T;5F> jFigure 4. Temperature dependence of the outer extrema (2Azz) of ESR spectra for Rub.ns10 (L) and Rub.nscp04 (%).Zr(2 0   r3  0$TA_0(D Figure 3. ESR spectra of samples containing the same amount of nanosilica and various amounts of coupling agent measured at 10C.$ 2 y !  0*T+L1. mFigure 1. ESR spectra of the spin probe diffusing in the matrix of Rub.ns00 sample at different temperatures.&n(2 e nw  Kv)V   #"2&F;eDS A  T<T_ж_ж ?"`&'Qv)R b0.92 #G j ?  T?T_ж_ж ?"` 'Q&R fRub.ns20   #G j ;  TTGT_ж_ж?&Rv)S b0.29 #G j 9  TPT_ж_ж ?"` R&S h Rub.nscp01   #G j 6  TYT_ж_ж?&Sv)5U b0.40 #G j 4  TbT_ж_ж ?"` S&5U h Rub.nscp02   #G j 1  TlT_ж_ж?&5Uv)V b0.31 #G j /  TtuT_ж_ж ?"` 5U&V h Rub.nscp04   #G j   T~T_ж_ж?&Ov)'Q b0.94 #G j   TT_ж_ж? O&'Q fRub.ns15   #G j   T T_ж_ж?&sNv)O b0.96 #G j   TdT_ж_ж? sN&O fRub.ns10   #G j !  TT_ж_ж?&Mv)sN b1.75 #G j "  TܬT_ж_ж? M&sN fRub.ns00   #G jC #   fĸT_ж_ж^d?" &Kv)M In/IwN   #G j $   f0T_ж_ж5d?"  K&M dsample #G jZB %  s *> ? sNv)sNZB &  s *> ? Ov)OZB '  s *> ? 'Qv)'QZB (  s *> ?&K&VZB )  s *> ? Mv)M`B *  0> ? Kv)K`B +  0> ? K V`B ,  0> ?v)Kv)V`B -  0> ? Vv)VZB 5  s *> ? 5Uv)5UZB :  s *> ? Sv)SZB @  s *> ? Rv)R I 0pT.B9F8E \Table 3. The intensities ratio of narrow and wide component of ESR spectra measured at 10C.$] 2U ]  U 0LTB E cThe amount of nanosilica in all samples containing the coupling agent was similar and equal 10 phr.d 2d d V 0T]a&c BESR spectrometar : Varian E-109 Temperature unit Bruker ER 4111 VTCC C f  <A ??"`- -* x n  <A ??0z/:@ ) o 0(TZ8JH9a Z. Veksli, M Andreis, B. Rakvin, Prog Polym. Sci. 25 (2000) 949. G. Jeschke et al., Polymer Engineering and Science 44 (2004) 1112. 2 R p 0TZ<6e ESR spectra show a significant influence of nanosilica on the local chain dynamics. The increase in the nanosilica amount leads to the decrease in segmental motions. The coupling agent makes the role of nanosilica more pronounced. Because of the better contact between the matrix chain segment and nanosilica particles, the restriction in local motions become more and more important as the amount of coupling agent increases.(2 f v 0A?"`]U5}F)<   A "`1E\-8N  0TN8O Ia) without coupling agent b) with the coupling agent"J 2I,  G  0|TQ"4T }Figure 5. 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(kJmiw   ICorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 GraphicCorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 Graphic SPW 10.0 Graph 0SigmaPlotGraphicObject.90(SigmaPlot 10.0 Graph SPW 10.0 Graph 0SigmaPlotGraphicObject.90(SigmaPlot 10.0 GraphD/ 0|DArialhA  /0z[ 0DTimes New Roman0z[ 0 DGaramond Roman0z[ 00DSymbold Roman0z[ 0@DWP MathA Roman0z[ 0@ . @n?" dd@  @@`` P 212$V0,Hw6"$gqN,WGְdEh36"$vHηΈ={>cUH 2$],ֽ4 P R$D<$*q 2$ _s8) \k= $2$C^g¿pSK;&~ r$߀M'$,,Gi 2$fAζg6K/!m*52$s%dgZ1RV f2$ : H=>X񭑹Wa  0AAP3@<ʚ;ʚ;g4!d!d z[ 0p:@p<<4ddddL 0. A0___PPT10 pp___PPT9n^,֋S#ޠ"PNG  IHDRF}sRGB PLTE3*ծ cmPPJCmp0712 7tRNS@f8IDATWc``d !$$<[UBS#BT     BLT5G^" `-Am Q Objective (2 6   BT5G^" `V A" Q Materials (2 6   BT5G^" `AFAH ZSample preparation(26   Bp#T5G^" `QA3T OMethods(26   BT5G^" `4C? OResults(26    0$5T^D<4___PPT9 ]Investigation of the NR samples containg different amounts of the nanosilica particles and their influence on local chain dynamics. Influence of a coupling agent on the changes in matrix structure and chain dynamics.@! U! 8X  0`AT<$ V& JTable 1. Samples of NR with different amounts of nanosilica"KC Kt nB*]D3 l  #"&<WVWV'aP0 $ T_ж_ж? 1]D3 `20 #G j # T`VT_ж_ж?n1 D3 fRub.ns20   #G j " THT_ж_ж? 0]1 `15 #G j ! ThT_ж_ж?n0 1 fRub.ns15   #G j   TYT_ж_ж? 6/]0 `10 #G j  T yT_ж_ж?n6/ 0 fRub.ns10   #G j  TT_ж_ж? -]6/ _0 #G j  T(T_ж_ж?n- 6/ fRub.ns00   #G j(   f0T_ж_ж^d?"  B*]- |The amount of nanosilica / phr #G j   fT_ж_ж5d?" nB* - e sample #G jZB ' s *> ?n6/]6/ZB ( s *> ?n0]0ZB ) s *> ?n1]1ZB , s *> ? B* D3ZB & s *> ?n-]-`B % 0> ?nB*]B*`B + 0> ?nB*nD3`B - 0> ?]B*]D3`B * 0> ?nD3]D3  0Ti2 4 @The average diametar of the used nanosilica particles was 13 nm.A 2A A  0T5 A8 RTable 2. NR samples with different amounts of coupling agent (Si 69)"SK S p ^:@C j  #""a$93zA  TIJT_ж_ж?5 A@C _4 #G j  TT_ж_ж?^A5 @C h Rub.nscp04   #G j  TT_ж_ж?5 @A _2 #G j  TT_ж_ж?^@5 A h Rub.nscp02   #G j  TTT_ж_ж?5 >@ _1 #G j  TT_ж_ж?^>5 @ h Rub.nscp01   #G j,   f T_ж_ж^d?" 5 :> "The amount of coupling agent / phr## ##G j   fdT_ж_ж5d?" ^:5 > q sample& #G jZB   s *> ?^@@ZB   s *> ?^AAZB   s *> ?5 :5 @CZB   s *> ?^>>`B   0> ?^::`B   0> ?^:^@C`B   0> ?:@C`B   0> ?^@C@C  0U'J{c!QD<4___PPT9 Two-roll mixing folowed by compression moulding. Swelling in the toluene probe solution at the constant temperature (35C). Removing the solvent by evaporationand annealing at 60 C during tree days.6!  8X*  0 UWZ] ESR  spin probe method probe amount in the samples was 0.15 wt% DD D4  # A#U~ ^  0TZ^{6_ ,4-hydroy-2,2,6,6-tetramethylpiperidin-1-oxyl- 2- # XB  0D)wkJw  BU5G^" `W|/Y R Conclusion (2 6   B U5G^" `W7hGY S References  (2 6   0 U%+3KH?- \Figure 2. ESR spectra of samples containing different amount of nanosilica measured at 10C.$] 2 T ]  0U;5F> jFigure 4. Temperature dependence of the outer extrema (2Azz) of ESR spectra for Rub.ns10 (L) and Rub.nscp04 (%).Zr(2 0   r3  0$UA_0(D Figure 3. ESR spectra of samples containing the same amount of nanosilica and various amounts of coupling agent measured at 10C.$ 2 y !  0*U+L1. mFigure 1. ESR spectra of the spin probe diffusing in the matrix of Rub.ns00 sample at different temperatures.&n(2 e nw  Kv)V   #"2&F;eDS A  T<U_ж_ж ?"`&'Qv)R b0.92 #G j ?  T?U_ж_ж ?"` 'Q&R fRub.ns20   #G j ;  TTGU_ж_ж?&Rv)S b0.29 #G j 9  TOU_ж_ж ?"` R&S h Rub.nscp01   #G j 6  TYU_ж_ж?&Sv)5U b0.40 #G j 4  TpbU_ж_ж ?"` S&5U h Rub.nscp02   #G j 1  TkU_ж_ж?&5Uv)V b0.31 #G j /  TtU_ж_ж ?"` 5U&V h Rub.nscp04   #G j   T~U_ж_ж?&Ov)'Q b0.94 #G j   T`U_ж_ж? O&'Q fRub.ns15   #G j   TU_ж_ж?&sNv)O b0.96 #G j   TؙU_ж_ж? sN&O fRub.ns10   #G j !  TU_ж_ж?&Mv)sN b1.75 #G j "  TPU_ж_ж? M&sN fRub.ns00   #G jC #   f8U_ж_ж^d?" &Kv)M In/IwN   #G j $   fU_ж_ж5d?"  K&M dsample #G jZB %  s *> ? sNv)sNZB &  s *> ? Ov)OZB '  s *> ? 'Qv)'QZB (  s *> ?&K&VZB )  s *> ? Mv)M`B *  0> ? Kv)K`B +  0> ? K V`B ,  0> ?v)Kv)V`B -  0> ? Vv)VZB 5  s *> ? 5Uv)5UZB :  s *> ? Sv)SZB @  s *> ? Rv)R I 0U.B9F8E \Table 3. The intensities ratio of narrow and wide component of ESR spectra measured at 10C.$] 2U ]  U 0UB E cThe amount of nanosilica in all samples containing the coupling agent was similar and equal 10 phr.d 2d d V 0LU]a{c BESR spectrometar : Varian E-109 Temperature unit Bruker ER 4111 VTCC C f  <A ??"`- -* x n  <A ??0z/:@ ) o 0UZ8JH9a Z. Veksli, M Andreis, B. Rakvin, Prog Polym. Sci. 25 (2000) 949. G. Jeschke et al., Polymer Engineering and Science 44 (2004) 1112. 2 R p 0DUZ<6e ESR spectra show a significant influence of nanosilica on the local chain dynamics. The increase in the nanosilica amount leads to the decrease in segmental motions. The coupling agent makes the role of nanosilica more pronounced. Because of the better contact between the matrix chain segment and nanosilica particles, the restriction in local motions become more and more important as the amount of coupling agent increases.(2 f v 0A?"`]U5}F)<   A "`1E\-8N  0UN8O Ia) without coupling agent b) with the coupling agent"J 2I,  G  0UQ"4T }Figure 5. Schematic presentation of rubber matrices with the same crosslink densities and the same amount of the nanosilica. &~(2 u g    0U*MBxHN : 2 f  C >A$logotip%20zaklade Q@F0Z  ) #q   #" 1E ,N n =w  3 #"  ) #qB   B&CDE|F45%Yv*FFHVfXv8VV&*Z(t8@          "`) KO    B CDEFh5%FFT H XhThhD4:X$ ` ` $ Zb<D,$      v  * @ 8 t V$ 8p4ff8(DrhtZhJ814@                       "` _   tBCz DEFP5%44 { ZN <  < x2 ,    @ * N X  z t\ (> T  ^ rP  F` ~ $ v4XDrtTF6DD8b*vV *  h fx%(@                 "`U ="   B C DE$Fl5%IIB ` p~  &` $ 6prB TP T    P 4` 4bf V n  & P 4 |    8 * 0     ~ :` B , ` x$ p<h(t:XHvX:8VtJxV<<34@                        "`s w>   BC DE0Fp5%LLuV( t8 f ,x:<H<xV,VV8  Hh <Ht< (F (HF6Df:D,HB   n  V  P    ` $ U 58@                         3"`    dBCDEFL5%11;vZX Z  vX::*Xv 8**F TXTTJZ<Tb<xRp:Hp8tTU#$@                "`Y #   B(CDEXF(5%uZf<<8xt, 8H Hth(@       3"` aMV2   C "` V2   C "`L?V2   C "`UdHHV2   C "`&rWV2   C "`K0V2   C "`V2   C "`V2   C "`~pV2   C "`>F1(V2   C "`th   c LA (1Small checker board"`lk   c LA (1Small checker board"`ED   c LA (1Small checker board"`]\   c LA (1Small checker board"`   c LA (1Small checker board"`{%z$   c LA (1Small checker board"`ON   c LA (1Small checker board"`UT   c LA (1Small checker board"`!"   c LA (1Small checker board"`   c LA (1Small checker board"`   c LA (1Small checker board"`  X  0A ?/7D>:H  0U<܍ ? 3380___PPT10.@[r3??    (kJmiw   ICorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 GraphicCorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 Graphic SPW 10.0 Graph 0SigmaPlotGraphicObject.90(SigmaPlot 10.0 Graph SPW 10.0 Graph 0SigmaPlotGraphicObject.90(SigmaPlot 10.0 GraphD/ 0|DArialhA  /0z[ 0DTimes New Roman0z[ 0 DGaramond Roman0z[ 00DSymbold Roman0z[ 0@DWP MathA Roman0z[ 0@ . @n?" dd@  @@`` P 212$V0,Hw6"$gqN,WGְdEh36"$vHηΈ={>cUH 2$],ֽ4 P R$D<$*q 2$ _s8) \k= $2$C^g¿pSK;&~ r$߀M'$,,Gi 2$fAζg6K/!m*52$s%dgZ1RV f2$ : H=>X񭑹Wa  0AAP3@<ʚ;ʚ;g4!d!d z[ 0p:@p<<4ddddL 0. A0___PPT10 pp___PPT9n^,֋S#ޠ"PNG  IHDRF}sRGB PLTE3*ծ cmPPJCmp0712 7tRNS@f8IDATWc``d !$$<[UBS#BcUH 2$],ֽ4 P R$D<$*q 2$ _s8) \k= $2$C^g¿pSK;&~ r$߀M'$,,Gi 2$fAζg6K/!m*52$s%dgZ1RV f2$ : H=>X񭑹Wa  0AAP3@<ʚ;ʚ;g4dd z[ 0Zp:@p<<4ddddL 0( A0___PPT10 pp___PPT9n^,֋S#ޠ"PNG  IHDRF}sRGB PLTE3*ծ cmPPJCmp0712 7tRNS@f8IDATWc``d !$$<[UBS#BT     B5G^" `-Am Q Objective (2 6   B5G^" `V A" Q Materials (2 6   Bd5G^" `AFAH ZSample preparation(26   B5G^" `QA3T OMethods(26   B5G^" `4C? OResults(26    0^D<4___PPT9 ]Investigation of the NR samples containg different amounts of the nanosilica particles and their influence on local chain dynamics. Influence of a coupling agent on the changes in matrix structure and chain dynamics.@! U! 8X  0<$ V& JTable 1. Samples of NR with different amounts of nanosilica"KC Kt nB*]D3 l  #"&<WVWV'aP0 $ T=_ж_ж? 1]D3 `20 #G j # TL_ж_ж?n1 D3 fRub.ns20   #G j " TT_ж_ж? 0]1 `15 #G j ! T_ж_ж?n0 1 fRub.ns15   #G j   Te_ж_жiences, Kottayam, India - 686 560 Z0?2Y0;*?<, , , , , ,, , V ? R*  !    ? 6/]0 `10 #G j  Tg_ж_ж?n6/ 0 fRub.ns10   #G j  T`_ж_ж? -]6/ _0 #G j  T|_ж_ж?n- 6/ fRub.ns00   #G j(   f_ж_ж^d?"  B*]- |The amount of nanosilica / phr #G j   f4_ж_ж5d?" nB* - e sample #G jZB ' s *> ?n6/]6/ZB ( s *> ?n0]0ZB ) s *> ?n1]1ZB , s *> ? B* D3ZB & s *> ?n-]-`B % 0> ?nB*]B*`B + 0> ?nB*nD3`B - 0> ?]B*]D3`B * 0> ?nD3]D3  0 i2 4 @The average diametar of the used nanosilica particles was 13 nm.A 2A A  0̛5 A8 RTable 2. NR samples with different amounts of coupling agent (Si 69)"SK S p ^:@C j  #""a$93zA  T_ж_ж?5 A@C _4 #G j  T_ж_ж?^A5 @C h Rub.nscp04   #G j  TL_ж_ж?5 @A _2 #G j  Tp_ж_ж?^@5 A h Rub.nscp02   #G j  T_ж_ж?5 >@ _1 #G j  T<_ж_ж?^>5 @ h Rub.nscp01   #G j,   f_ж_ж^d?" 5 :> "The amount of coupling agent / phr## ##G j   fh_ж_ж5d?" ^:5 > q sample& #G jZB   s *> ?^@@ZB   s *> ?^AAZB   s *> ?5 :5 @CZB   s *> ?^>>`B   0> ?^::`B   0> ?^:^@C`B   0> ?:@C`B   0> ?^@C@C  0'J{c!QD<4___PPT9 Two-roll mixing folowed by compression moulding. Swelling in the toluene probe solution at the constant temperature (35C). Removing the solvent by evaporationand annealing at 60 C during tree days.6!  8X*  0WZ] ESR  spin probe method probe amount in the samples was 0.15 wt% DD D4  # A#U~ ^  0Z^{6_ ,4-hydroy-2,2,6,6-tetramethylpiperidin-1-oxyl- 2- # XB  0D)wkJw  Bl5G^" `W|/Y R Conclusion (2 6   Bl 5G^" `W7hGY S References  (2 6   0 %+3KH?- \Figure 2. ESR spectra of samples containing different amount of nanosilica measured at 10C.$] 2 T ]  0;5F> jFigure 4. Temperature dependence of the outer extrema (2Azz) of ESR spectra for Rub.ns10 (L) and Rub.nscp04 (%).Zr(2 0   r3  0 A_0(D Figure 3. ESR spectra of samples containing the same amount of nanosilica and various amounts of coupling agent measured at 10C.$ 2 y !  0+L1. mFigure 1. ESR spectra of the spin probe diffusing in the matrix of Rub.ns00 sample at different temperatures.&n(2 e nw  Kv)V   #"2&F;eDS A  T,_ж_ж ?"`&'Qv)R b0.92 #G j ?  Td6_ж_ж ?"` 'Q&R fRub.ns20   #G j ;  T|'_ж_ж?&Rv)S b0.29 #G j 9  TH_ж_ж ?"` R&S h Rub.nscp01   #G j 6  T9_ж_ж?&Sv)5U b0.40 #G j 4  TdZ_ж_ж ?"` S&5U h Rub.nscp02   #G j 1  T\c_ж_ж?&5Uv)V b0.31 #G j /  Tl_ж_ж ?"` 5U&V h Rub.nscp04   #G j   Tu_ж_ж?&Ov)'Q b0.94 #G j   Tw_ж_ж? O&'Q fRub.ns15   #G j   T_ж_ж?&sNv)O b0.96 #G j   T<_ж_ж? sN&O fRub.ns10   #G j !  T _ж_ж?&Mv)sN b1.75 #G j "  T<_ж_ж? M&sN fRub.ns00   #G jC #   f_ж_ж^d?" &Kv)M In/IwN   #G j $   f_ж_ж5d?"  K&M dsample #G jZB %  s *> ? sNv)sNZB &  s *> ? Ov)OZB '  s *> ? 'Qv)'QZB (  s *> ?&K&VZB )  s *> ? Mv)M`B *  0> ? Kv)K`B +  0> ? K V`B ,  0> ?v)Kv)V`B -  0> ? Vv)VZB 5  s *> ? 5Uv)5UZB :  s *> ? Sv)SZB @  s *> ? Rv)R I 0.B9F8E \Table 3. The intensities ratio of narrow and wide component of ESR spectra measured at 10C.$] 2U ]  U 0B E cThe amount of nanosilica in all samples containing the coupling agent was similar and equal 10 phr.d 2d d V 0]a{c BESR spectrometar : Varian E-109 Temperature unit Bruker ER 4111 VTCC C f  <A ??"`- -* x n  <A ??0z/:@ ) o 0Z8JH9a Z. Veksli, M Andreis, B. Rakvin, Prog Polym. Sci. 25 (2000) 949. G. Jeschke et al., Polymer Engineering and Science 44 (2004) 1112. 2 R p 0Z<6e ESR spectra show a significant influence of nanosilica on the local chain dynamics. The increase in the nanosilica amount leads to the decrease in segmental motions. The coupling agent makes the role of nanosilica more pronounced. Because of the better contact between the matrix chain segment and nanosilica particles, the restriction in local motions become more and more important as the amount of coupling agent increases.(2 f v 0A?"`]U5}F)<   A "`1E\-8N  0N8O Ia) without coupling agent b) with the coupling agent"J 2I,  G  0PQ"4T }Figure 5. Schematic presentation of rubber matrices with the same crosslink densities and the same amount of the nanosilica. &~(2 u g    0*MBxHN : 2 f  C >A$logotip%20zaklade Q@F0Z  ) #q   #" 1E ,N n =w  3 #"  ) #qB   B&CDE|F45%Yv*FFHVfXv8VV&*Z(t8@          "`) KO    B CDEFh5%FFT H XhThhD4:X$ ` ` $ Zb<D,$      v  * @ 8 t V$ 8p4ff8(DrhtZhJ814@                       "` _   tBCz DEFP5%44 { ZN <  < x2 ,    @ * N X  z t\ (> T  ^ rP  F` ~ $ v4XDrtTF6DD8b*vV *  h fx%(@                 "`U ="   B C DE$Fl5%IIB ` p~  &` $ 6prB TP T    P 4` 4bf V n  & P 4 |    8 * 0     ~ :` B , ` x$ p<h(t:XHvX:8VtJxV<<34@                        "`s w>   BC DE0Fp5%LLuV( t8 f ,x:<H<xV,VV8  Hh <Ht< (F (HF6Df:D,HB   n  V  P    ` $ U 58@                         3"`    dBCDEFL5%11;vZX Z  vX::*Xv 8**F TXTTJZ<Tb<xRp:Hp8tTU#$@                "`Y #   B(CDEXF(5%uZf<<8xt, 8H Hth(@       3"` aMV2   C "` V2   C "`L?V2   C "`UdHHV2   C "`&rWV2   C "`K0V2   C "`V2   C "`V2   C "`~pV2   C "`>F1(V2   C "`th   c LA (1Small checker board"`lk   c LA (1Small checker board"`ED   c LA (1Small checker board"`]\   c LA (1Small checker board"`   c LA (1Small checker board"`{%z$   c LA (1Small checker board"`ON   c LA (1Small checker board"`UT   c LA (1Small checker board"`!"   c LA (1Small checker board"`   c LA (1Small checker board"`   c LA (1Small checker board"`  X  0A ?/7D>:H  0U<܍ ? 3380___PPT10.@[r? bq  (kJmiw   MCorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 GraphicCorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 Graphic SPW 10.0 Graph 0SigmaPlotGraphicObject.90(SigmaPlot 10.0 Graph SPW 10.0 Graph 0SigmaPlotGraphicObject.90(SigmaPlot 10.0 GraphD/ 0|DArialhA (0z[ 0"DTimes New Roman0z[ 0 DGaramond Roman0z[ 00DSymbold Roman0z[ 0@DWP MathA Roman0z[ 0@ . @n?" dd@  @@`` X$ 212$V0,Hw6"$gqN,WGְdEh36"$vHηΈ={>cUH 2$],ֽ4 P R$D<$*q 2$ _s8) \k= $2$C^g¿pSK;&~ r$߀M'$,,Gi 2$fAζg6K/!m*52$s%dgZ1RV f2$ : H=>X񭑹Wa  0AAP3@<ʚ;ʚ;g4dd z[ 0p:@p<<4ddddL 0( A0___PPT10 pp___PPT9n^,֋S#ޠ"PNG  IHDRF}sRGB PLTE3*ծ cmPPJCmp0712 7tRNS@f8IDATWc``d !$$<[UBS#BT     B5G^" `-Am Q Objective (2 6   B5G^" `V A" Q Materials (2 6   Bd5G^" `AFAH ZSample preparation(26   B5G^" `QA3T OMethods(26   B5G^" `4C? OResults(26    0^D<4___PPT9 ]Investigation of the NR samples containg different amounts of the nanosilica particles and their influence on local chain dynamics. Influence of a coupling agent on the changes in matrix structure and chain dynamics.@! U! 8X  0<$ V& JTable 1. Samples of NR with different amounts of nanosilica"KC Kt nB*]D3 l  #"&<WVWV'aP0 $ T=_ж_ж? 1]D3 `20 #G j # TL_ж_ж?n1 D3 fRub.ns20   #G j " TT_ж_ж? 0]1 `15 #G j ! T_ж_ж?n0 1 fRub.ns15   #G j   Te_ж_ж? 6/]0 `10 #G j  Tg_ж_ж?n6/ 0 fRub.ns10   #G j  T`_ж_ж? -]6/ _0 #G j  T|_ж_ж?n- 6/ fRub.ns00   #G j(   f_ж_ж^d?"  B*]- |The amount of nanosilica / phr #G j   f4_ж_ж5d?" nB* - e sample #G jZB ' s *> ?n6/]6/ZB ( s *> ?n0]0ZB ) s *> ?n1]1ZB , s *> ? B* D3ZB & s *> ?n-]-`B % 0> ?nB*]B*`B + 0> ?nB*nD3`B - 0> ?]B*]D3`B * 0> ?nD3]D3  0 i2 4 @The average diametar of the used nanosilica particles was 13 nm.A 2A A  0̛5 A8 RTable 2. NR samples with different amounts of coupling agent (Si 69)"SK S p ^:@C j  #""a$93zA  T_ж_ж?5 A@C _4 #G j  T_ж_ж?^A5 @C h Rub.nscp04   #G j  TL_ж_ж?5 @A _2 #G j  Tp_ж_ж?^@5 A h Rub.nscp02   #G j  T_ж_ж?5 >@ _1 #G j  T<_ж_ж?^>5 @ h Rub.nscp01   #G j,   f_ж_ж^d?" 5 :> "The amount of coupling agent / phr## ##G j   fh_ж_ж5d?" ^:5 > q sample& #G jZB   s *> ?^@@ZB   s *> ?^AAZB   s *> ?5 :5 @CZB   s *> ?^>>`B   0> ?^::`B   0> ?^:^@C`B   0> ?:@C`B   0> ?^@C@C  0'J{c!QD<4___PPT9 Two-roll mixing folowed by compression moulding. Swelling in the toluene probe solution at the constant temperature (35C). Removing the solvent by evaporationand annealing at 60 C during tree days.6!  8X*  0WZ] ESR  spin probe method probe amount in the samples was 0.15 wt% DD D4  # A#U~ ^  0Z^{6_ -4-hydroy-2,2,6,6-tetramethylpiperidine-1-oxyl. 2.8   XB  0D)wkJw  Bl5G^" `W|/Y R Conclusion (2 6   Bl 5G^" `W7hGY S References  (2 6   0 %+3KH?- \Figure 2. ESR spectra of samples containing different amount of nanosilica measured at 10C.$] 2 T ]  0;5F> jFigure 4. Temperature dependence of the outer extrema (2Azz) of ESR spectra for Rub.ns10 (L) and Rub.nscp04 (%).Zr(2 0   r3  0 A_0(D Figure 3. ESR spectra of samples containing the same amount of nanosilica and various amounts of coupling agent measured at 10C.$ 2 y !  0+L1. mFigure 1. ESR spectra of the spin probe diffusing in the matrix of Rub.ns00 sample at different temperatures.&n(2 e nw  Kv)V   #"2&F;eDS A  T,_ж_ж ?"`&'Qv)R b0.92 #G j ?  Td6_ж_ж ?"` 'Q&R fRub.ns20   #G j ;  T|'_ж_ж?&Rv)S b0.29 #G j 9  TH_ж_ж ?"` R&S h Rub.nscp01   #G j 6  T9_ж_ж?&Sv)5U b0.40 #G j 4  TdZ_ж_ж ?"` S&5U h Rub.nscp02   #G j 1  T\c_ж_ж?&5Uv)V b0.31 #G j /  Tl_ж_ж ?"` 5U&V h Rub.nscp04   #G j   Tu_ж_ж?&Ov)'Q b0.94 #G j   Tw_ж_ж? O&'Q fRub.ns15   #G j   T_ж_ж?&sNv)O b0.96 #G j   T<_ж_ж? sN&O fRub.ns10   #G j !  T _ж_ж?&Mv)sN b1.75 #G j "  T<_ж_ж? M&sN fRub.ns00   #G jC #   f_ж_ж^d?" &Kv)M In/IwN   #G j $   f_ж_ж5d?"  K&M dsample #G jZB %  s *> ? sNv)sNZB &  s *> ? Ov)OZB '  s *> ? 'Qv)'QZB (  s *> ?&K&VZB )  s *> ? Mv)M`B *  0> ? Kv)K`B +  0> ? K V`B ,  0> ?v)Kv)V`B -  0> ? Vv)VZB 5  s *> ? 5Uv)5UZB :  s *> ? Sv)SZB @  s *> ? Rv)R I 0.B9F8E \Table 3. The intensities ratio of narrow and wide component of ESR spectra measured at 10C.$] 2U ]  U 0B E cThe amount of nanosilica in all samples containing the coupling agent was similar and equal 10 phr.d 2d d V 0]a{c BESR spectrometar : Varian E-109 Temperature unit Bruker ER 4111 VTCC C f  <A ??"`- -* x n  <A ??0z/:@ ) o 0Z8JH9a Z. Veksli, M Andreis, B. Rakvin, Prog Polym. Sci. 25 (2000) 949. G. Jeschke et al., Polymer Engineering and Science 44 (2004) 1112. 2 R p 0Z<6e ESR spectra show a significant influence of nanosilica on the local chain dynamics. The increase in the nanosilica amount leads to the decrease in segmental motions. The coupling agent makes the role of nanosilica more pronounced. Because of the better contact between the matrix chain segment and nanosilica particles, the restriction in local motions become more and more important as the amount of coupling agent increases.(2 f v 0A?"`]U5}F)<   A "`1E\-8N  0N8O Ia) without coupling agent b) with the coupling agent"J 2I,  G  0PQ"4T }Figure 5. Schematic presentation of rubber matrices with the same crosslink densities and the same amount of the nanosilica. &~(2 u g    0*MBxHN : 2 f  C >A$logotip%20zaklade Q@F0Z  ) #q   #" 1E ,N n =w  3 #"  ) #qB   B&CDE|F45%Yv*FFHVfXv8VV&*Z(t8@          "`) KO    B CDEFh5%FFT H XhThhD4:X$ ` ` $ Zb<D,$      v  * @ 8 t V$ 8p4ff8(DrhtZhJ814@                       "` _   tBCz DEFP5%44 { ZN <  < x2 ,    @ * N X  z t\ (> T  ^ rP  F` ~ $ v4XDrtTF6DD8b*vV *  h fx%(@                 "`U ="   B C DE$Fl5%IIB ` p~  &` $ 6prB TP T    P 4` 4bf V n  & P 4 |    8 * 0     ~ :` B , ` x$ p<h(t:XHvX:8VtJxV<<34@                        "`s w>   BC DE0Fp5%LLuV( t8 f ,x:<H<xV,VV8  Hh <Ht< (F (HF6Df:D,HB   n  V  P    ` $ U 58@                         3"`    dBCDEFL5%11;vZX Z  vX::*Xv 8**F TXTTJZ<Tb<xRp:Hp8tTU#$@                "`Y #   B(CDEXF(5%uZf<<8xt, 8H Hth(@       3"` aMV2   C "` V2   C "`L?V2   C "`UdHHV2   C "`&rWV2   C "`K0V2   C "`V2   C "`V2   C "`~pV2   C "`>F1(V2   C "`th   c LA (1Small checker board"`lk   c LA (1Small checker board"`ED   c LA (1Small checker board"`]\   c LA (1Small checker board"`   c LA (1Small checker board"`{%z$   c LA (1Small checker board"`ON   c LA (1Small checker board"`UT   c LA (1Small checker board"`!"   c LA (1Small checker board"`   c LA (1Small checker board"`   c LA (1Small checker board"`  X  0A ?/7D>:H  0U<܍ ? 3380___PPT10.@[r?  / (kJmiw   MCorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 GraphicCorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 Graphic SPW 10.0 Graph 0SigmaPlotGraphicObject.90(SigmaPlot 10.0 Graph SPW 10.0 Graph 0SigmaPlotGraphicObject.90(SigmaPlot 10.0 GraphD/ 0|DArialhA (0z[ 0"DTimes New Roman0z[ 0 DGaramond Roman0z[ 00DSymbold Roman0z[ 0@DWP MathA Roman0z[ 0@ . @n?" dd@  @@`` X$ 212$V0,Hw6"$gqN,WGְdEh36"$vHηΈ={>cUH 2$],ֽ4 P R$D<$*q 2$ _s8) \k= $2$C^g¿pSK;&~ r$߀M'$,,Gi 2$fAζg6K/!m*52$s%dgZ1RV f2$ : H=>X񭑹Wa  0AAP3@<ʚ;ʚ;g4dd z[ 0p:@p<<4ddddL 0( A0___PPT10 pp___PPT9n^,֋S#ޠ"PNG  IHDRF}sRGB PLTE3*ծ cmPPJCmp0712 7tRNS@f8IDATWc``d !$$<[UBS#BcUH 2$],ֽ4 P R$D<$*q 2$ _s8) \k= $2$C^g¿pSK;&~ r$߀M'$,,Gi 2$fAζg6K/!m*52$s%dgZ1RV f2$ : H=>X񭑹Wa  0AAP3@<ʚ;ʚ;g4dd z[ 0p:@p<<4ddddL 0e A0___PPT10 pp___PPT9n^,֋S#ޠ"PNG  IHDRF}sRGB PLTE3*ծ cmPPJCmp0712 7tRNS@f8IDATWc``d !$$<[UBS#B?@ABCDEFGHIJKLMNOPQRSTUVWXYZ[\]^_`abcdefghijklmnopqrstuvwxyz|}~      !"#$%&'()*+,-./0123456789:;<=>?@ABCDEFGHIJKLMNOPQRSTUVWXYZ[\]^_`abcdefghijklmnopqrstuvwxy{{|}~z      !"#$%&'()*+,-./0123456789:;<=>?@ABCDEFGHIJKLMNOPQRSTUVWXYZ[\]^_`abcdefghijklmnopqrstuvwxyz|}~ V  {  ign TemplateEmbedded OLE Servers Slide Titles_SigmaSigmaical     D  T     Bt;85G^" `-Am Y Objective (2 6   Bh*85G^" `V A" Y Materials (2 6   B(85G^" `AFAH tSample preparation(26$   B4,85G^" `QA3T WMethods(26  B 5G^" `4C? WResults(26  0L8^D<4___PPT9 'Investigation of the NR samples containg different amounts of the nanosilica particles and their influence on local chain dynamics. Influence of a coupling agent on the changes in matrix structure and chain dynamics.@! U!       8Xv  0(F8<$ V& JTable 1. Samples of NR with different amounts of nanosilica"KC    t nB*]D3 l  #"&<WVWV'aP0 $ THV8_ж_ж? 1]D3 N20#G j # T_8_ж_ж?n1 D3 TRub.ns20  #G j " Tg8_ж_ж? 0]1 N15#G j ! Tp8_ж_ж?n0 1 TRub.ns15  #G j   Ty8_ж_ж? 6/]0 N10#G j  T8_ж_ж?n6/ 0 TRub.ns10  #G j  T8_ж_ж? -]6/ M0#G j  TĔ8_ж_ж?n- 6/ TRub.ns00  #G jx   f8_ж_ж^d?"  B*]- The amount of nanosilica / phrZ #G j!   fX8_ж_ж5d?" nB* - u sample#G jZB ' s *> ?n6/]6/ZB ( s *> ?n0]0ZB ) s *> ?n1]1ZB , s *> ? B* D3ZB & s *> ?n-]-`B % 0> ?nB*]B*`B + 0> ?nB*nD3`B - 0> ?]B*]D3`B * 0> ?nD3]D3~  08i2 4 @The average diametar of the used nanosilica particles was 13 nm.A 2A  l  0085 A8 RTable 2. NR samples with different amounts of coupling agent (Si 69)"SKt   p ^:@C j  #""a$93zA  T8_ж_ж?5 A@C M4#G j  T 8_ж_ж?^A5 @C V Rub.nscp04  #G j  Tt8_ж_ж?5 @A M2#G j  T8_ж_ж?^@5 A V Rub.nscp02  #G j  TP8_ж_ж?5 >@ M1#G j  T8_ж_ж?^>5 @ V Rub.nscp01  #G j|   f8_ж_ж^d?" 5 :> "The amount of coupling agent / phr##Z #G j-   fD9_ж_ж5d?" ^:5 >  sample&#G jZB   s *> ?^@@ZB   s *> ?^AAZB   s *> ?5 :5 @CZB   s *> ?^>>`B   0> ?^::`B   0> ?^:^@C`B   0> ?:@C`B   0> ?^@C@C\  09'J{c!QD<4___PPT9 Two-roll mixing folowed by compression moulding. Swelling in the toluene probe solution at the constant temperature (35C). Removing the solvent by evaporationand annealing at 60 C during tree days.6!   8X  09WZ] XESR  spin probe method probe amount in the samples was 0.15 wt% DD 4  # A#U~ ^   0l9Z^{F_ .4-hydroxy-2,2,6,6-tetramethylpiperidine-1-oxyl/ 2/B  XB  0D)wkJw  B,95G^" `W|/Y Z Conclusion (2 6   Bp95G^" `W7hGY [ References  (2 6   0l#9%+3KH?- N\Figure 2. ESR spectra of samples containing different amount of nanosilica measured at 10C.$] 2 T    j  0,)9;5F> Figure 4. Temperature dependence of the outer extrema (2Azz) of ESR spectra for Rub.ns10 (L) and Rub.nscp04 (%).Zr(2 0   -  0D19A_0(D Figure 3. ESR spectra of samples containing the same amount of nanosilica and various amounts of coupling agent measured at 10C.$ 2 y     069+L1. mFigure 1. ESR spectra of the spin probe diffusing in the matrix of Rub.ns00 sample at different temperatures.&n(2 e      Kv)V   #"2&F;eDS A  TC9_ж_ж ?"`&'Qv)R P0.92#G j ?  TDM9_ж_ж ?"` 'Q&R TRub.ns20  #G j ;  TLO9_ж_ж?&Rv)S P0.29#G j 9  Tl_9_ж_ж ?"` R&S V Rub.nscp01  #G j 6  Txh9_ж_ж?&Sv)5U P0.40#G j 4  Tdq9_ж_ж ?"` S&5U V Rub.nscp02  #G j 1  Tz9_ж_ж?&5Uv)V P0.31#G j /  T9_ж_ж ?"` 5U&V V Rub.nscp04  #G j   T$9_ж_ж?&Ov)'Q P0.94#G j   T9_ж_ж? O&'Q TRub.ns15  #G j   T<9_ж_ж?&sNv)O P0.96#G j   TD9_ж_ж? sN&O TRub.ns10  #G j !  TL9_ж_ж?&Mv)sN P1.75#G j "  TT9_ж_ж? M&sN TRub.ns00  #G j] #   fl9_ж_ж^d?" &Kv)M In/IwN  $#G j $   fh9_ж_ж5d?"  K&M lsample#G jZB %  s *> ? sNv)sNZB &  s *> ? Ov)OZB '  s *> ? 'Qv)'QZB (  s *> ?&K&VZB )  s *> ? Mv)M`B *  0> ? Kv)K`B +  0> ? K V`B ,  0> ?v)Kv)V`B -  0> ? Vv)VZB 5  s *> ? 5Uv)5UZB :  s *> ? Sv)SZB @  s *> ? Rv)R I 09.B9F8E r\Table 3. The intensities ratio of narrow and wide component of ESR spectra measured at 10C.$] 2U      U 0(9B E cThe amount of nanosilica in all samples containing the coupling agent was similar and equal 10 phr.d 2d  , V 09]a{c BESR spectrometar : Varian E-109 Temperature unit Bruker ER 4111 VTCCP   f  <A ??"`- -* x n  <A ??0z/:@  o 0X9Z8JH9a iZ. Veksli, M Andreis, B. Rakvin, Prog Polym. Sci. 25 (2000) 949. G. Jeschke et al., Polymer Engineering and Science 44 (2004) 1112. 2   p 0`9Z<6e ESR spectra show a significant influence of nanosilica on the local chain dynamics. The increase in the nanosilica amount leads to the decrease in segmental motions. The coupling agent makes the role of nanosilica more pronounced. Because of the better contact between the matrix chain segment and nanosilica particles, the restriction in local motions become more and more important as the amount of coupling agent increases.(2             f v 0A?"`]U5}F)<   A "`1E\-8N  09N8O Ia) without coupling agent b) with the coupling agent"J 2I(  M  0 9Q"4T }Figure 5. Schematic presentation of rubber matrices with the same crosslink densities and the same amount of the nanosilica. &~(2 u& g    0D:*MBxHN < 2  f  C >A$logotip%20zaklade Q@F0Z  ) #q   #" 1E ,N n =w  3 #"  ) #qB   B&CDE|F45%Yv*FFHVfXv8VV&*Z(t8@          "`) KO    B CDEFh5%FFT H XhThhD4:X$ ` ` $ Zb<D,$      v  * @ 8 t V$ 8p4ff8(DrhtZhJ814@                       "` _   tBCz DEFP5%44 { ZN <  < x2 ,    @ * N X  z t\ (> T  ^ rP  F` ~ $ v4XDrtTF6DD8b*vV *  h fx%(@                 "`U ="   B C DE$Fl5%IIB ` p~  &` $ 6prB TP T    P 4` 4bf V n  & P 4 |    8 * 0     ~ :` B , ` x$ p<h(t:XHvX:8VtJxV<<34@                        "`s w>   BC DE0Fp5%LLuV( t8 f ,x:<H<xV,VV8  Hh <Ht< (F (HF6Df:D,HB   n  V  P    ` $ U 58@                         3"`    dBCDEFL5%11;vZX Z  vX::*Xv 8**F TXTTJZ<Tb<xRp:Hp8tTU#$@                "`Y #   B(CDEXF(5%uZf<<8xt, 8H Hth(@       3"` aMV2   C "` V2   C "`L?V2   C "`UdHHV2   C "`&rWV2   C "`K0V2   C "`V2   C "`V2   C "`~pV2   C "`>F1(V2   C "`th   c LA (1Small checker board"`lk   c LA (1Small checker board"`ED   c LA (1Small checker board"`]\   c LA (1Small checker board"`   c LA (1Small checker board"`{%z$   c LA (1Small checker board"`ON   c LA (1Small checker board"`UT   c LA (1Small checker board"`!"   c LA (1Small checker board"`   c LA (1Small checker board"`   c LA (1Small checker board"`  X  0A ?/7D>:H  0U<܍ ? 3380___PPT10.@[roK0 1 (kJmiw   YCorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 GraphicCorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 Graphic SPW 10.0 Graph 0SigmaPlotGraphicObject.90(SigmaPlot 10.0 Graph SPW 10.0 Graph 0SigmaPlotGraphicObject.90(SigmaPlot 10.0 GraphD/ 0|DArialhA RomanTTX5ܖ 0ܖ"DTimes New RomanTTX5ܖ 0ܖ DGaramond RomanTTX5ܖ 0ܖ0DSymbold RomanTTX5ܖ 0ܖ@DWP MathA RomanTTX5ܖ 0ܖ@ . @n?" dd@  @@`` X$ 212$V0,Hw6"$gqN,WGְdEh36"$vHηΈ={>cUH 2$],ֽ4 P R$D<$*q 2$ _s8) \k= $2$C^g¿pSK;&~ r$߀M'$,,Gi 2$fAζg6K/!m*52$s%dgZ1RV f2$ : H=>X񭑹Wa  0AAP3@<ʚ;ʚ;g4dd B 06|p:@p<<4dddd w 0T45 A0___PPT10 pp___PPT9n^,֋S#ޠ"PNG  IHDRF}sRGB PLTE3*ծ cmPPJCmp0712 7tRNS@f8IDATWc``d !$$<[UBS#B(  l J 6Ԕ"`<kJ~U   ``C`CA ?"6@ NNN?N  ~  BA ??TG: ~   BA ??T' h  T8gKgKff "`-G`XP___PPT92* n Natural Rubber Filled by Nanosilica: an ESR  Spin Probe Study Leki1, S. Vali1,2, A.P. Meera3 and S. Thomas3 1 University of Rijeka, School of Medicine, Brae Branchetta 20, Rijeka, 51000, Croatia 2 Rudjer Boakovi Institute, Bijeni ka 54, Zagreb,10000, Croatia 3 Mahatma Gandhi University, School of Chemical Sciences, Kottayam, India - 686 560 Z0?2Y0;*?<, , , , , ,, , V ? R*  !         D  T     Bl*85G^" `-Am Y Objective (2 6   Bp/85G^" `V A" Y Materials (2 6   BX%85G^" `AFAH tSample preparation(26$   B\85G^" `QA3T WMethods(26  BtC85G^" `4C? WResults(26  0_8^D<4___PPT9 'Investigation of the NR samples containg different amounts of the nanosilica particles and their influence on local chain dynamics. Influence of a coupling agent on the changes in matrix structure and chain dynamics.@! U!       8Xv  0 Q8<$ V& JTable 1. Samples of NR with different amounts of nanosilica"KC    t nB*]D3 l  #"&<WVWV'aP0 $ T`8_ж_ж? 1]D3 N20#G j # Tz8_ж_ж?n1 D3 TRub.ns20  #G j " TȂ8_ж_ж? 0]1 N15#G j ! TЋ8_ж_ж?n0 1 TRub.ns15  #G j   Tؔ8_ж_ж? 6/]0 N10#G j  T8_ж_ж?n6/ 0 TRub.ns10  #G j  Tp8_ж_ж? -]6/ M0#G j  T8_ж_ж?n- 6/ TRub.ns00  #G jx   f 8_ж_ж^d?"  B*]- The amount of nanosilica / phrZ #G j!   ft8_ж_ж5d?" nB* - u sample#G jZB ' s *> ?n6/]6/ZB ( s *> ?n0]0ZB ) s *> ?n1]1ZB , s *> ? B* D3ZB & s *> ?n-]-`B % 0> ?nB*]B*`B + 0> ?nB*nD3`B - 0> ?]B*]D3`B * 0> ?nD3]D3~  008i2 4 @The average diametar of the used nanosilica particles was 13 nm.A 2A  l  0|85 A8 RTable 2. NR samples with different amounts of coupling agent (Si 69)"SKt   p ^:@C j  #""a$93zA  Tl8_ж_ж?5 A@C M4#G j  TT8_ж_ж?^A5 @C V Rub.nscp04  #G j  T8_ж_ж?5 @A M2#G j  T8_ж_ж?^@5 A V Rub.nscp02  #G j  T9_ж_ж?5 >@ M1#G j  T9_ж_ж?^>5 @ V Rub.nscp01  #G j|   f9_ж_ж^d?" 5 :> "The amount of coupling agent / phr##Z #G j-   f(&9_ж_ж5d?" ^:5 >  sample&#G jZB   s *> ?^@@ZB   s *> ?^AAZB   s *> ?5 :5 @CZB   s *> ?^>>`B   0> ?^::`B   0> ?^:^@C`B   0> ?:@C`B   0> ?^@C@C\  0)9'J{c!QD<4___PPT9 Two-roll mixing folowed by compression moulding. Swelling in the toluene probe solution at the constant temperature (35C). Removing the solvent by evaporationand annealing at 60 C during tree days.6!   8X  079WZ] XESR  spin probe method probe amount in the samples was 0.15 wt% DD 4  # A#U~ ^   0Q9Z^{F_ .4-hydroxy-2,2,6,6-tetramethylpiperidine-1-oxyl/ 2/B  XB  0D)wkJw  BTU95G^" `W|/Y Z Conclusion (2 6   BlY95G^" `W7hGY [ References  (2 6   0]9%+3KH?- N\Figure 2. ESR spectra of samples containing different amount of nanosilica measured at 10C.$] 2 T    j  0g9;5F> Figure 4. Temperature dependence of the outer extrema (2Azz) of ESR spectra for Rub.ns10 (L) and Rub.nscp04 (%).Zr(2 0   -  0h{9A_0(D Figure 3. ESR spectra of samples containing the same amount of nanosilica and various amounts of coupling agent measured at 10C.$ 2 y     0,9+L1. mFigure 1. ESR spectra of the spin probe diffusing in the matrix of Rub.ns00 sample at different temperatures.&n(2 e      Kv)V   #"2&F;eDS A  T9_ж_ж ?"`&'Qv)R P0.92#G j ?  Th9_ж_ж ?"` 'Q&R TRub.ns20  #G j ;  T9_ж_ж?&Rv)S P0.29#G j 9  T9_ж_ж ?"` R&S V Rub.nscp01  #G j 6  T9_ж_ж?&Sv)5U P0.40#G j 4  T9_ж_ж ?"` S&5U V Rub.nscp02  #G j 1  T9_ж_ж?&5Uv)V P0.31#G j /  TT9_ж_ж ?"` 5U&V V Rub.nscp04  #G j   T9_ж_ж?&Ov)'Q P0.94#G j   T9_ж_ж? O&'Q TRub.ns15  #G j   T9_ж_ж?&sNv)O P0.96#G j   T9_ж_ж? sN&O TRub.ns10  #G j !  T:_ж_ж?&Mv)sN P1.75#G j "  T :_ж_ж? M&sN TRub.ns00  #G j] #   fx:_ж_ж^d?" &Kv)M In/IwN  $#G j $   f%:_ж_ж5d?"  K&M lsample#G jZB %  s *> ? sNv)sNZB &  s *> ? Ov)OZB '  s *> ? 'Qv)'QZB (  s *> ?&K&VZB )  s *> ? Mv)M`B *  0> ? Kv)K`B +  0> ? K V`B ,  0> ?v)Kv)V`B -  0> ? Vv)VZB 5  s *> ? 5Uv)5UZB :  s *> ? Sv)SZB @  s *> ? Rv)R I 0*:.B9F8E r\Table 3. The intensities ratio of narrow and wide component of ESR spectra measured at 10C.$] 2U      U 0;:B E cThe amount of nanosilica in all samples containing the coupling agent was similar and equal 10 phr.d 2d  , V 0D:]a{c BESR spectrometar : Varian E-109 Temperature unit Bruker ER 4111 VTCCP   f  <A ??"`- -* x n  <A ??0z/:@  o 0XL:Z8JH9a iZ. Veksli, M Andreis, B. Rakvin, Prog Polym. Sci. 25 (2000) 949. G. Jeschke et al., Polymer Engineering and Science 44 (2004) 1112. 2   p 0 b:Z<6e ESR spectra show a significant influence of nanosilica on the local chain dynamics. The increase in the nanosilica amount leads to the decrease in segmental motions. The coupling agent makes the role of nanosilica more pronounced. 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