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Vali1,2 1 University of Rijeka, School of Medicine, Brae Branchetta 20, Rijeka, 51000, Croatia 2 Rudjer Boakovi Institute, Bijeni ka 54, Zagreb,10000, Croatia<0m<( , , , , , ,   V   >  ; %          D    )  0-  !D<4___PPT9 } spin probe: !   i#Dl  0-3Z?5 D EXPERIMENTAL 2 (ff   0(-$ tu% .4-hydroxy-2,2,6,6-tetramethylpiperidine-1-oxyl/ 2/ B  XB  0D3f) kJ   0P! *M4A GN < 2    Z`C`CA ?"6@ NNN?NQ@ G0   Z {f&" `) Z Objective  (2 6 4  # A( g1  0X) D<4___PPT9 natural rubber (NR) latex  62 wt.% of dry matter (The Rubber Research Institute of India)*2!- _  8 nn  0 65)RD<4___PPT9 g natural rubber latex containing 62 wt.% of dry matter was irradiated with different total irradiation doses of 200 kGy and 300 kGy irradiated NR latex was deluted by ammonia solution (0.6 wt.%) up to 25 wt.% of solid content ~1mm thick NR films were prepared by removing the liquid phase at room temperature spin probe was incorporated in NR samples by swelling the samples in the probe toluene solution at 4 C, 16 C, 24 C and 37 C solvent was slowly removed by evaporation; all samples were then annealed at 60 C for 62 hours ESR spectra were recorded on Varian E-109 ESR spectrometer equipped with Bruker ER 041 XG microwave bridge and Bruker ER 4111 VT variable temperature unit! ^! S! ! `! !            H 3T|  0 FD<4___PPT9 pTo investigate the influence of the temperature of spin probe incorporation process on the shape of ESR spectra.q!q P , *  P>f  p 6 [HdD<4___PPT9 nthe shape of ESR spectra of the spin probe in heterogeneous systems, as shown for NR, depends on the probe incorporation temperature the increase of the probe incorporation temperature results in a higher amount of the broad component higher probe incorporation temperature allows probe molecules to diffuse into the higher density regions of the matrix and consequently leads to the restriction in probe dynamics:!(2 `              o 6H [[ )b !L. J. Berliner, Spin Labeling: Theory and Applications Vol 1. and Vol 2., Academic Press, 1976. Z. Veksli, M Andreis, B. Rakvin, ESR spectroscopy for the study of polymer heterogeneity, Prog Polym. Sci. 25 (2000) 949-986.(2&  !  C*8 E4/I>  c,R2G=   66(5(<[I> qFigure 5. Schematic representation of the spin probe incorporation process at (a) 4 C and (b) 37 C in NR matrix$r 2 i    ffHH'T >3wH$  # E4/I+; &@ 3wxH$ V >3wH$B   3 :>>B   3 BLCz B   3 C#-D~#B   3 UEEB   3 ?M@YB   3 <pE=B   3 R@ @!H   B&CDE|F41Yv*FFHVfXv8VV&*Z(t8@          "`>I`D}0   # B CDEFh1FFT H XhThhD4:X$ ` ` $ Zb<D,$      v  * @ 8 t V$ 8p4ff8(DrhtZhJ814@                       "`=4+G#!   zBCz DEFP144 { ZN <  < x2 ,    @ * N X  z t\ (> T  ^ rP  F` ~ $ v4XDrtTF6DD8b*vV *  h fx%(@                 "`?wF"@   # B C DE$Fl1IIB ` p~  &` $ 6prB TP T    P 4` 4bf V n  & P 4 |    8 * 0     ~ :` B , ` x$ p<h(t:XHvX:8VtJxV<<34@                        "`?xH$\ !  # BC DE0Fp1LLuV( t8 f ,x:<H<xV,VV8  Hh <Ht< (F (HF6Df:D,HB   n  V  P    ` $ U 58@                         3"`[;4@# "  jBCDEFL111;vZX Z  vX::*Xv 8**F TXTTJZ<Tb<xRp:Hp8tTU#$@                "`I<@ $ #  B(CDEXF(1uZf<<8xt, 8H Hth(@       3"`>Bk#\2 $  S "`A A \2 %  S "`D!D!\2 &  S "`zC#C[\2 '  S "`?FwF\2 (  S "`>'>_\2 )  S "`=>\2 *  S "`= = \2 +  S "`A B\2 ,  S "`@q@\2 -  S "`c?0#?h#@ 18" U 3:"( <  B C DE$Fl1IIB ` p~  &` $ 6prB TP T    P 4` 4bf V n  & P 4 |    8 * 0     ~ :` B , ` x$ p<h(t:XHvX:8VtJxV<<34@                        "`48"H 9  B&CDE|F41Yv*FFHVfXv8VV&*Z(t8@          "`s3Q6 :  B CDEFh1FFT H XhThhD4:X$ ` ` $ Zb<D,$      v  * @ 8 t V$ 8p4ff8(DrhtZhJ814@                       "`2Y8  ;  zBCz DEFP144 { ZN <  < x2 ,    @ * N X  z t\ (> T  ^ rP  F` ~ $ v4XDrtTF6DD8b*vV *  h fx%(@                 "`37!D =  BC DE0Fp1LLuV( t8 f ,x:<H<xV,VV8  Hh <Ht< (F (HF6Df:D,HB   n  V  P    ` $ U 58@                         3"`1Y34! >  jBCDEFL111;vZX Z  vX::*Xv 8**F TXTTJZ<Tb<xRp:Hp8tTU#$@                "`&24q $ ?  B(CDEXF(1uZf<<8xt, 8H Hth(@       3"`Y35!N2 @  S  5K E5 N2 A  S 6 6!N2 B  S 5n16N2 C  S {707lN2 D  S S3[3N2 E  S 223N2 F  S 25 &3q N2 G  S 5~U5N2 H  S _44CN2 I  S 3!4!T 2&}8! Q # R2&P8!V 4  C "`U55jP K  3 "`2 2P L  3 "`77-P M  3 "`7s}8P N  3 "`e6Z!6!P O  3 "`n3v 3 P P  3 "`3&#4 S  0P2635 Q(a) 2   T  086:< Q(b) 2  a8 4H6* | b3F*^   S .AFigure34G%   6N64L%H6* EFigure 4. ESR spectra of the spin probe diffusing in NR irradiated with 300 kGy. The probe incorporation temperatures were: (a) 4 C and (b) 24 C. Spectra were measured at 19 C. &(2 (         1Rz V  S .AFigure4=0Py  66Q0 U Figure 3. ESR spectra of the spin probe diffusing in NR irradiated with 200 kGy measured at 0 C. The probe incorporation temperatures were: (a) 16 C and (b) 24 C.&(2         ,lu/P xU  6T68Y0< Figure 2. ESR spectra of the spin probe diffusing in nonirradiated NR measured at -10 C. The probe incorporation temperatures were: (a) 4 C, (b) 24 C and (c) 37 C.&(2      "Ck V  S .A Figure2m'L08I 3@-I[P   #"2&@R2G[P   B6?*FN-I[P 15.1,(bB  @  @@``   Bp,6??N*F[P ~24,(bB  @  @@``   B56?*F7M-IN 20.9,(bB  @  @@``   B?6??7M*FN }4,(bB  @  @@``   BX=6?;97M?[P ~19,(bB  @  @@``   Bd6?37M;9[P  NR 300 kGy, ( bB  @  @@``   B0,Q?*FK-I7M 2.32,(bB  @  @@``   BlQ??K*F7M ~24,(bB  @  @@``   Bx"Q?*FJ-IK 2.47,(bB  @  @@``   B%Q??J*FK ~16,(bB  @  @@``   B?Q?;9J?7M }0,(bB  @  @@``   BP]Q?3J;97M  NR 200 kGy, ( bB  @  @@``   BaQ?*FH-IJ 1.15,(bB  @  @@``   BfQ??H*FJ ~37,(bB  @  @@``   BQ?*FF-IH 1.35,(bB  @  @@``   BLQ??F*FH ~24,(bB  @  @@``   BQ?*F\E-IF 1.61,(bB  @  @@``   B Q??\E*FF }4,(bB  @  @@``   BXQ?;9\E?J -10,(bB  @  @@``   BHQ?3\E;9J NR 0 kGy, (bB  @  @@``e   NQ2?"`*F@-I\E In/Iwb(bjbjB&   @  @@``9   N(Q2?"`?@*F\E 'Temperature of probe incorporation / C.(('bB ( @  @@``m   NQ2?"`;9@?\E Temperature of measurement / CL ( b"bB*   @  @@``   N N2?"`3@;9\E Sample.(bB  @  @@``ZB   s *Ԕ ?3@-I@ZB   s *Ԕ ?3[P-I[PZB   s *Ԕ ?3@3[PZB   s *Ԕ ?-I@-I[PZB   s *Ԕ ?3\E-I\EZB   s *Ԕ ?;9@;9[PZB   s *Ԕ ??@?[PZB   s *Ԕ ?*F@*F[PZB   s *Ԕ ?3J-IJZB   s *1 ??F-IFZB   s *1 ??H-IHZB '  s *Ԕ ?37M-I7MZB 5  s *1 ??K-IKZB T  s *1 ??N-IN q 0PN=Q2FGT 7mTable 1. 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TN gKgKff "`kJ  f^ESR - Spin Probe Method in Studying Crosslinked Elastomers: an Effect of the Probe Incorporation Temperature M. Didovi1, D. Klepac1 and S. Vali1,2 1 University of Rijeka, School of Medicine, Brae Branchetta 20, Rijeka, 51000, Croatia 2 Rudjer Boakovi Institute, Bijeni ka 54, Zagreb,10000, Croatia<0m<( , , , , , ,   V   >  ; %          D    )  08I-  !D<4___PPT9 } spin probe: !   i#Dl  0s-3Z?5 D EXPERIMENTAL 2 (ff   0(-$ tu% .4-hydroxy-2,2,6,6-tetramethylpiperidine-1-oxyl/ 2/ B  XB  0D3f) kJ   0|-*M4A GN < 2    Z`C`CA ?"6@ NNN?NQ@ G0   Z,w-{f&" `) Z Objective  (2 6 4  # A( g1  0| D<4___PPT9 natural rubber (NR) latex  62 wt.% of dry matter (The Rubber Research Institute of India)*2!- _  8 nn[  0-5)SD<4___PPT9 natural rubber latex containing 62 wt.% of dry matter was irradiated with different total irradiation doses of 200 kGy and 300 kGy irradiated NR latex was deluted by ammonia solution (0.6 wt.%) up to 25 wt.% of solid content ~1mm thick NR films were prepared by removing the liquid phase at room temperature spin probe was incorporated in NR samples by swelling the samples in the probe solution at 4 C, 16 C, 24 C and 37 C. The solvent was toluene. solvent was slowly removed by evaporation; all samples were then annealed at 60 C for 72 hours ESR spectra were recorded on Varian E-109 ESR spectrometer equipped with Bruker ER 041 XG microwave bridge and Bruker ER 4111 VT variable temperature unit! ^! 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TN gKgKff "`kJ  f^ESR - Spin Probe Method in Studying Crosslinked Elastomers: an Effect of the Probe Incorporation Temperature M. Didovi1, D. Klepac1 and S. Vali1,2 1 University of Rijeka, School of Medicine, Brae Branchetta 20, Rijeka, 51000, Croatia 2 Rudjer Boakovi Institute, Bijeni ka 54, Zagreb,10000, Croatia<0m<( , , , , , ,   V   >  ; %          D    )  08I-  !D<4___PPT9 } spin probe: !   i#Dl  0s-3Z?5 D EXPERIMENTAL 2 (ff   0(-$ tu% .4-hydroxy-2,2,6,6-tetramethylpiperidine-1-oxyl/ 2/ B  XB  0D3f) kJ   0|-*M4A GN < 2    Z`C`CA ?"6@ NNN?NQ@ G0   Z,w-{f&" `) Z Objective  (2 6 4  # A( g1  0| D<4___PPT9 natural rubber (NR) latex  62 wt.% of dry matter (The Rubber Research Institute of India)*2!- _  8 nnm  0-5)SD<4___PPT9 natural rubber latex containing 62 wt.% of dry matter was irradiated with different total irradiation doses of 200 kGy and 300 kGy irradiated NR latex was deluted by ammonia solution (0.6 wt.%) up to 25 wt.% of solid content ~1mm thick NR films were prepared by removing the liquid phase at room temperature spin probe was incorporated in NR samples by swelling the samples in the probe solution at 4 C, 16 C, 24 C and 37 C. The solvent was toluene. solvent was slowly removed by evaporation; all samples were then annealed at 60 C for 72 hours ESR spectra were recorded on Varian E-109 ESR spectrometer equipped with Bruker ER 041 XG microwave bridge and Bruker ER 4111 VT variable temperature unit! ^! S! ! `! !            H 3T|  0 FD<4___PPT9 pTo investigate the influence of the temperature of spin probe incorporation process on the shape of ESR spectra.q!q P , *  P>f  p 6t6[HdD<4___PPT9 nthe shape of ESR spectra of the spin probe in heterogeneous systems, as shown for NR, depends on the probe incorporation temperature the increase of the probe incorporation temperature results in a higher amount of the broad component higher probe incorporation temperature allows probe molecules to diffuse into the higher density regions of the matrix and consequently leads to the restriction in probe dynamics:!(2 `              o 6 [[ )b !L. J. Berliner, Spin Labeling: Theory and Applications Vol 1. and Vol 2., Academic Press, 1976. Z. Veksli, M Andreis, B. Rakvin, ESR spectroscopy for the study of polymer heterogeneity, Prog Polym. Sci. 25 (2000) 949-986.(2&  !  C*8 E4/I>  c,R2G=   6D6(5(<[I> qFigure 5. Schematic representation of the spin probe incorporation process at (a) 4 C and (b) 37 C in NR matrix$r 2 i    ffHH'T >3wH$  # E4/I+; &@ 3wxH$ V >3wH$B   3 :>>B   3 BLCz B   3 C#-D~#B   3 UEEB   3 ?M@YB   3 <pE=B   3 R@ @!H   B&CDE|F41Yv*FFHVfXv8VV&*Z(t8@          "`>I`D}0   # B CDEFh1FFT H XhThhD4:X$ ` ` $ Zb<D,$      v  * @ 8 t V$ 8p4ff8(DrhtZhJ814@                       "`=4+G#!   zBCz DEFP144 { ZN <  < x2 ,    @ * N X  z t\ (> T  ^ rP  F` ~ $ v4XDrtTF6DD8b*vV *  h fx%(@                 "`?wF"@   # B C DE$Fl1IIB ` p~  &` $ 6prB TP T    P 4` 4bf V n  & P 4 |    8 * 0     ~ :` B , ` x$ p<h(t:XHvX:8VtJxV<<34@                        "`?xH$\ !  # BC DE0Fp1LLuV( t8 f ,x:<H<xV,VV8  Hh <Ht< (F (HF6Df:D,HB   n  V  P    ` $ U 58@                         3"`[;4@# "  jBCDEFL111;vZX Z  vX::*Xv 8**F TXTTJZ<Tb<xRp:Hp8tTU#$@                "`I<@ $ #  B(CDEXF(1uZf<<8xt, 8H Hth(@       3"`>Bk#\2 $  S "`A A \2 %  S "`D!D!\2 &  S "`zC#C[\2 '  S "`?FwF\2 (  S "`>'>_\2 )  S "`=>\2 *  S "`= = \2 +  S "`A B\2 ,  S "`@q@\2 -  S "`c?0#?h#@ 18" U 3:"( <  B C DE$Fl1IIB ` p~  &` $ 6prB TP T    P 4` 4bf V n  & P 4 |    8 * 0     ~ :` B , ` x$ p<h(t:XHvX:8VtJxV<<34@                        "`48"H 9  B&CDE|F41Yv*FFHVfXv8VV&*Z(t8@          "`s3Q6 :  B CDEFh1FFT H XhThhD4:X$ ` ` $ Zb<D,$      v  * @ 8 t V$ 8p4ff8(DrhtZhJ814@                       "`2Y8  ;  zBCz DEFP144 { ZN <  < x2 ,    @ * N X  z t\ (> T  ^ rP  F` ~ $ v4XDrtTF6DD8b*vV *  h fx%(@                 "`37!D =  BC DE0Fp1LLuV( t8 f ,x:<H<xV,VV8  Hh <Ht< (F (HF6Df:D,HB   n  V  P    ` $ U 58@                         3"`1Y34! >  jBCDEFL111;vZX Z  vX::*Xv 8**F TXTTJZ<Tb<xRp:Hp8tTU#$@                "`&24q $ ?  B(CDEXF(1uZf<<8xt, 8H Hth(@       3"`Y35!N2 @  S  5K E5 N2 A  S 6 6!N2 B  S 5n16N2 C  S {707lN2 D  S S3[3N2 E  S 223N2 F  S 25 &3q N2 G  S 5~U5N2 H  S _44CN2 I  S 3!4!T 2&}8! Q # R2&P8!V 4  C "`U55jP K  3 "`2 2P L  3 "`77-P M  3 "`7s}8P N  3 "`e6Z!6!P O  3 "`n3v 3 P P  3 "`3&#4 S  0635 Q(a) 2   T  0<6:< Q(b) 2  a8 4H6* | b3F*^   S .AFigure34G%   6$64L%H6* EFigure 4. ESR spectra of the spin probe diffusing in NR irradiated with 300 kGy. The probe incorporation temperatures were: (a) 4 C and (b) 24 C. Spectra were measured at 19 C. &(2 (         1Rz V  S .AFigure4=0Py  6̸6Q0 U Figure 3. ESR spectra of the spin probe diffusing in NR irradiated with 200 kGy measured at 0 C. The probe incorporation temperatures were: (a) 16 C and (b) 24 C.&(2         ,lu/P xU  6B68Y0< Figure 2. ESR spectra of the spin probe diffusing in nonirradiated NR measured at -10 C. The probe incorporation temperatures were: (a) 4 C, (b) 24 C and (c) 37 C.&(2      "Ck V  S .A Figure2m'L08I 3@-I[P   #"2&@R2G[P   BM6?*FN-I[P 15.1,(bB  @  @@``   BH6??N*F[P ~24,(bB  @  @@``   B6?*F7M-IN 20.9,(bB  @  @@``   B6??7M*FN }4,(bB  @  @@``   Bx6?;97M?[P ~19,(bB  @  @@``   Bo6?37M;9[P  NR 300 kGy, ( bB  @  @@``   B96?*FK-I7M 2.32,(bB  @  @@``   B6??K*F7M ~24,(bB  @  @@``   B6?*FJ-IK 2.47,(bB  @  @@``   B6??J*FK ~16,(bB  @  @@``   BQ?;9J?7M }0,(bB  @  @@``   B@Q?3J;97M  NR 200 kGy, ( bB  @  @@``   BHQ?*FH-IJ 1.15,(bB  @  @@``   BTQ??H*FJ ~37,(bB  @  @@``   BQ?*FF-IH 1.35,(bB  @  @@``   B\Q??F*FH ~24,(bB  @  @@``   BfQ?*F\E-IF 1.61,(bB  @  @@``   B|"Q??\E*FF }4,(bB  @  @@``   BliQ?;9\E?J -10,(bB  @  @@``   B CQ?3\E;9J NR 0 kGy, (bB  @  @@``e   N4jQ2?"`*F@-I\E In/Iwb(bjbjB&   @  @@``9   NUQ2?"`?@*F\E 'Temperature of probe incorporation / C.(('bB ( @  @@``m   N/Q2?"`;9@?\E Temperature of measurement / CL ( b"bB*   @  @@``   NwQ2?"`3@;9\E Sample.(bB  @  @@``ZB   s *Ԕ ?3@-I@ZB   s *Ԕ ?3[P-I[PZB   s *Ԕ ?3@3[PZB   s *Ԕ ?-I@-I[PZB   s *Ԕ ?3\E-I\EZB   s *Ԕ ?;9@;9[PZB   s *Ԕ ??@?[PZB   s *Ԕ ?*F@*F[PZB   s *Ԕ ?3J-IJZB   s *1 ??F-IFZB   s *1 ??H-IHZB '  s *Ԕ ?37M-I7MZB 5  s *1 ??K-IKZB T  s *1 ??N-IN q 0TQ=Q2FGT 7mTable 1. Intensity ratios of the narrow (In) and broad (Iw) components of ESR spectra shown in Figures 2 - 4.rn(2!   4  Em HL /$R2(  # "<_0&\   0HQ/$R2% 2Figure 1. Typical ESR spectra of spin probe in NR:&3(2 *b 8X   0Q"%+(H@8___PPT9  L^narrow (T > Tg) broad (T < Tg) bimodal (TH"T5mT)l0!    H       8XV  S .AFigure1tLO/"XB r 0De""XB s 0DwZ$Z$#L #& v # Ny"%R t  0Q#6% bIw& 2   u  0ԳQ%& bIn& 2  !  ZQ{f&" `) Materials and Methods(266   Z3Q{f&" `4X)tZ Z References (2 6   ZN{f&" `4XHtZ [ Conclusions (2 6   Z.N{f&" `H WResults(26   tAU<܍ ?Pozadina1"@` 3380___PPT10.@[rӼyB 1.(kJmiw   PCorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 Graphic`/ 0՜.+,0    dCustomHG ArialTimes New RomanDefault DesignCorelDRAW 11.0 GraphicSlide 1  Fonts UsedDesign TemplateEmbedded OLE Servers Slide Titles_㜸SigmaSigma  H 3T|  0 FD<4___PPT9 pTo investigate the influence of the temperature of spin probe incorporation process on the shape of ESR spectra.q!q P , *  P>f  p 6t6[HdD<4___PPT9 nthe shape of ESR spectra of the spin probe in heterogeneous systems, as shown for NR, depends on the probe incorporation temperature the increase of the probe incorporation temperature results in a higher amount of the broad component higher probe incorporation temperature allows probe molecules to diffuse into the higher density regions of the matrix and consequently leads to the restriction in probe dynamics:!(2 `              o 6 [[ )b !L. J. Berliner, Spin Labeling: Theory and Applications Vol 1. and Vol 2., Academic Press, 1976. Z. Veksli, M Andreis, B. Rakvin, ESR spectroscopy for the study of polymer heterogeneity, Prog Polym. Sci. 25 (2000) 949-986.(2&  !  C*8 E4/I>  c,R2G=   6D6(5(<[I> qFigure 5. Schematic representation of the spin probe incorporation process at (a) 4 C and (b) 37 C in NR matrix$r 2 i    ffHH'T >3wH$  # E4/I+; &@ 3wxH$ V >3wH$B   3 :>>B   3 BLCz B   3 C#-D~#B   3 UEEB   3 ?M@YB    3 <pE=B   3 R@ @!H   B&CDE|F41Yv*FFHVfXv8VV&*Z(t8@          "`>I`D}0   # B CDEFh1FFT H XhThhD4:X$ ` ` $ Zb<D,$      v  * @ 8 t V$ 8p4ff8(DrhtZhJ814@                       "`=4+G#!   zBCz DEFP144 { ZN <  < x2 ,    @ * N X  z t\ (> T  ^ rP  F` ~ $ v4XDrtTF6DD8b*vV *  h fx%(@                 "`?wF"@   # B C DE$Fl1IIB ` p~  &` $ 6prB TP T    P 4` 4bf V n  & P 4 |    8 * 0     ~ :` B , ` x$ p<h(t:XHvX:8VtJxV<<34@                        "`?xH$\ !  # BC DE0Fp1LLuV( t8 f ,x:<H<xV,VV8  Hh <Ht< (F (HF6Df:D,HB   n  V  P    ` $ U 58@                         3"`[;4@# "  jBCDEFL111;vZX Z  vX::*Xv 8**F TXTTJZ<Tb<xRp:Hp8tTU#$@                "`I<@ $ #  B(CDEXF(1uZf<<8xt, 8H Hth(@       3"`>Bk#\2 $  S "`A A \2 %  S "`D!D!\2 &  S "`zC#C[\2 '  S "`?FwF\2 (  S "`>'>_\2 )  S "`=>\2 *  S "`= = \2 +  S "`A B\2 ,  S "`@q@\2 -  S "`c?0#?h#@ 18" U 3:"( <  B C DE$Fl1IIB ` p~  &` $ 6prB TP T    P 4` 4bf V n  & P 4 |    8 * 0     ~ :` B , ` x$ p<h(t:XHvX:8VtJxV<<34@                        "`48"H 9  B&CDE|F41Yv*FFHVfXv8VV&*Z(t8@          "`s3Q6 :  B CDEFh1FFT H XhThhD4:X$ ` ` $ Zb<D,$      v  * @ 8 t V$ 8p4ff8(DrhtZhJ814@                       "`2Y8  ;  zBCz DEFP144 { ZN <  < x2 ,    @ * N X  z t\ (> T  ^ rP  F` ~ $ v4XDrtTF6DD8b*vV *  h fx%(@                 "`37!D =  BC DE0Fp1LLuV( t8 f ,x:<H<xV,VV8  Hh <Ht< (F (HF6Df:D,HB   n  V  P    ` $ U 58@                         3"`1Y34! >  jBCDEFL111;vZX Z  vX::*Xv 8**F TXTTJZ<Tb<xRp:Hp8tTU#$@                "`&24q $ ?  B(CDEXF(1uZf<<8xt, 8H Hth(@       3"`Y35!N2 @  S  5K E5 N2 A  S 6 6!N2 B  S 5n16N2 C  S {707lN2 D  S S3[3N2 E  S 223N2 F  S 25 &3q N2 G  S 5~U5N2 H  S _44CN2 I  S 3!4!T 2&}8! Q # R2&P8!V 4  C "`U55jP K  3 "`2 2P L  3 "`77-P M  3 "`7s}8P N  3 "`e6Z!6!P O  3 "`n3v 3 P P  3 "`3&#4 S  0635 Q(a) 2   T  0<6:< Q(b) 2  K8 4H6* | b3F*^   S .AFigure34G%   6$64L%H6* /Figure 4. ESR spectra of spin probe diffusing in NR irradiated with 300 kGy. The probe incorporation temperatures were: (a) 4 C and (b) 24 C. Spectra were measured at 19 C. &(2          1Rz V  S .AFigure4=0Pc  6̸6Q0 U Figure 3. ESR spectra of spin probe diffusing in NR irradiated with 200 kGy measured at 0 C. The probe incorporation temperatures were: (a) 16 C and (b) 24 C.&(2         ,lu/P x?  6B68Y0< Figure 2. ESR spectra of spin probe diffusing in nonirradiated NR measured at -10 C. The probe incorporation temperatures were: (a) 4 C, (b) 24 C and (c) 37 C.&(2      "Ck V  S .A Figure2m'L08I 3@-I[P   #"2&@R2G[P   BM6?*FN-I[P 15.1,(bB  @  @@``   BH6??N*F[P ~24,(bB  @  @@``   B6?*F7M-IN 20.9,(bB  @  @@``   B6??7M*FN }4,(bB  @  @@``   Bx6?;97M?[P ~19,(bB  @  @@``   Bo6?37M;9[P  NR 300 kGy, ( bB  @  @@``   B96?*FK-I7M 2.32,(bB  @  @@``   B6??K*F7M ~24,(bB  @  @@``   B6?*FJ-IK 2.47,(bB  @  @@``   B6??J*FK ~16,(bB  @  @@``   BQ?;9J?7M }0,(bB  @  @@``   B@Q?3J;97M  NR 200 kGy, ( bB  @  @@``   BHQ?*FH-IJ 1.15,(bB  @  @@``   BTQ??H*FJ ~37,(bB  @  @@``   BQ?*FF-IH 1.35,(bB  @  @@``   B\Q??F*FH ~24,(bB  @  @@``   BfQ?*F\E-IF 1.61,(bB  @  @@``   B|"Q??\E*FF }4,(bB  @  @@``   BliQ?;9\E?J -10,(bB  @  @@``   B CQ?3\E;9J NR 0 kGy, (bB  @  @@``e   N4jQ2?"`*F@-I\E In/Iwb(bjbjB&   @  @@``9   NUQ2?"`?@*F\E 'Temperature of probe incorporation / C.(('bB ( @  @@``m   N/Q2?"`;9@?\E Temperature of measurement / CL ( b"bB*   @  @@``   NwQ2?"`3@;9\E Sample.(bB  @  @@``ZB   s *Ԕ ?3@-I@ZB   s *Ԕ ?3[P-I[PZB   s *Ԕ ?3@3[PZB   s *Ԕ ?-I@-I[PZB   s *Ԕ ?3\E-I\EZB   s *Ԕ ?;9@;9[PZB   s *Ԕ ??@?[PZB   s *Ԕ ?*F@*F[PZB   s *Ԕ ?3J-IJZB   s *1 ??F-IFZB   s *1 ??H-IHZB '  s *Ԕ ?37M-I7MZB 5  s *1 ??K-IKZB T  s *1 ??N-IN q 0TQ=Q2FGT 7mTable 1. Intensity ratios of the narrow (In) and broad (Iw) components of ESR spectra shown in Figures 2 - 4.rn(2!   4  Em HL /$R2(  # "<_0&\   0HQ/$R2% 2Figure 1. Typical ESR spectra of spin probe in NR:&3(2 *b 8X   0Q"%+(H@8___PPT9  L^narrow (T > Tg) broad (T < Tg) bimodal (TH"T5mT)l0!    H       8XV  S .AFigure1tLO/"XB r 0De""XB s 0DwZ$Z$#L #& v # Ny"%R t  0Q#6% bIw& 2   u  0ԳQ%& bIn& 2  !  ZQ{f&" `) Materials and Methods(266   Z3Q{f&" `4X)tZ Z References (2 6   ZN{f&" `4XHtZ [ Conclusions (2 6   Z.N{f&" `H WResults(26   tAU<܍ ?Pozadina1"@` 3380___PPT10.@[rBKB 1.(kJmiw   PCorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 Graphic`/ 0DArialNew RomanTT-ܖ 0ܖ"DTimes New RomanTT-ܖ 0ܖ@ . @n?" dd@  @@`` x421  2$V0,Hw6b$HIG'"@"$vHηΈ={>cپb$ `يB-/*b$9,@?_"ml\ $b$7&(1pwz2$C^g¿pSK;&s b$Oh,m1[+ 0AA 3ff3ff@ʚ;:ʚ;g4!d!d- 0p:@p<<4dddd w 0T- 0___PPT10 pp___PPT9kc[nQy  a*lD!@PNG  IHDR exsRGBNPLTEkc{絔έֽεƭƥƽ{s cmPPJCmp0712x~tRNS AyIDATMI0{d{1@Gs @c3|bXֻ$镰3дY ;6TJ~UCo@{} P{4$]$gc>/13"+^ZCLKs}XmIENDB`O  = 0   d    ƒ(  l J 61"`HU~   BA ??    TN gKgKff "`kJ  f^ESR - Spin Probe Method in Studying Crosslinked Elastomers: an Effect of the Probe Incorporation Temperature M. Didovi1, D. Klepac1 and S. Vali1,2 1 University of Rijeka, School of Medicine, Brae Branchetta 20, Rijeka, 51000, Croatia 2 Rudjer Boakovi Institute, Bijeni ka 54, Zagreb,10000, Croatia<0m<( , , , , , ,   V   >  ; %          D    )  08I-  !D<4___PPT9 } spin probe: !   i#Dl  0s-3Z?5 D EXPERIMENTAL 2 (ff   0(-$ tu% .4-hydroxy-2,2,6,6-tetramethylpiperidine-1-oxyl/ 2/ B  XB  0D3f) kJ   0|-*M4A GN < 2    Z`C`CA ?"6@ NNN?NQ@ G0   Z,w-{f&" `) Z Objective  (2 6 4  # A( g1  0| D<4___PPT9 natural rubber (NR) latex  62 wt.% of dry matter (The Rubber Research Institute of India)*2!- _  8 nn[  0-5)SD<4___PPT9 natural rubber latex containing 62 wt.% of dry matter was irradiated with different total irradiation doses of 200 kGy and 300 kGy irradiated NR latex was deluted by ammonia solution (0.6 wt.%) up to 25 wt.% of solid content ~1mm thick NR films were prepared by removing the liquid phase at room temperature spin probe was incorporated in NR samples by swelling the samples in the probe solution at 4 C, 16 C, 24 C and 37 C. The solvent was toluene. solvent was slowly removed by evaporation; all samples were then annealed at 60 C for 72 hours ESR spectra were recorded on Varian E-109 ESR spectrometer equipped with Bruker ER 041 XG microwave bridge and Bruker ER 4111 VT variable temperature unit! ^! S! ! `! !            H 3T|  0 FD<4___PPT9 pTo investigate the influence of the temperature of spin probe incorporation process on the shape of ESR spectra.q!q P , *  P>f  p 6t6[HdD<4___PPT9 nthe shape of ESR spectra of the spin probe in heterogeneous systems, as shown for NR, depends on the probe incorporation temperature the increase of the probe incorporation temperature results in a higher amount of the broad component higher probe incorporation temperature allows probe molecules to diffuse into the higher density regions of the matrix and consequently leads to the restriction in probe dynamics:!(2 `              o 6 [[ )b !L. J. Berliner, Spin Labeling: Theory and Applications Vol 1. and Vol 2., Academic Press, 1976. Z. Veksli, M Andreis, B. Rakvin, ESR spectroscopy for the study of polymer heterogeneity, Prog Polym. Sci. 25 (2000) 949-986.(2&  !  C*8 E4/I>  c,R2G=   6D6(5(<[I> qFigure 5. Schematic representation of the spin probe incorporation process at (a) 4 C and (b) 37 C in NR matrix$r 2 i    ffHH'T >3wH$  # E4/I+; &@ 3wxH$ V >3wH$B   3 :>>B   3 BLCz B   3 C#-D~#B   3 UEEB   3 ?M@YB   3 <pE=B   3 R@ @!H   B&CDE|F41Yv*FFHVfXv8VV&*Z(t8@          "`>I`D}0   # B CDEFh1FFT H XhThhD4:X$ ` ` $ Zb<D,$      v  * @ 8 t V$ 8p4ff8(DrhtZhJ814@                       "`=4+G#!   zBCz DEFP144 { ZN <  < x2 ,    @ * N X  z t\ (> T  ^ rP  F` ~ $ v4XDrtTF6DD8b*vV *  h fx%(@                 "`?wF"@   # B C DE$Fl1IIB ` p~  &` $ 6prB TP T    P 4` 4bf V n  & P 4 |    8 * 0     ~ :` B , ` x$ p<h(t:XHvX:8VtJxV<<34@                        "`?xH$\ !  # BC DE0Fp1LLuV( t8 f ,x:<H<xV,VV8  Hh <Ht< (F (HF6Df:D,HB   n  V  P    ` $ U 58@                         3"`[;4@# "  jBCDEFL111;vZX Z  vX::*Xv 8**F TXTTJZ<Tb<xRp:Hp8tTU#$@                "`I<@ $ #  B(CDEXF(1uZf<<8xt, 8H Hth(@       3"`>Bk#\2 $  S "`A A \2 %  S "`D!D!\2 &  S "`zC#C[\2 '  S "`?FwF\2 (  S "`>'>_\2 )  S "`=>\2 *  S "`= = \2 +  S "`A B\2 ,  S "`@q@\2 -  S "`c?0#?h#@ 18" U 3:"( <  B C DE$Fl1IIB ` p~  &` $ 6prB TP T    P 4` 4bf V n  & P 4 |    8 * 0     ~ :` B , ` x$ p<h(t:XHvX:8VtJxV<<34@                        "`48"H 9  B&CDE|F41Yv*FFHVfXv8VV&*Z(t8@          "`s3Q6 :  B CDEFh1FFT H XhThhD4:X$ ` ` $ Zb<D,$      v  * @ 8 t V$ 8p4ff8(DrhtZhJ814@                       "`2Y8  ;  zBCz DEFP144 { ZN <  < x2 ,    @ * N X  z t\ (> T  ^ rP  F` ~ $ v4XDrtTF6DD8b*vV *  h fx%(@                 "`37!D =  BC DE0Fp1LLuV( t8 f ,x:<H<xV,VV8  Hh <Ht< (F (HF6Df:D,HB   n  V  P    ` $ U 58@                         3"`1Y34! >  jBCDEFL111;vZX Z  vX::*Xv 8**F TXTTJZ<Tb<xRp:Hp8tTU#$@                "`&24q $ ?  B(CDEXF(1uZf<<8xt, 8H Hth(@       3"`Y35!N2 @  S  5K E5 N2 A  S 6 6!N2 B  S 5n16N2 C  S {707lN2 D  S S3[3N2 E  S 223N2 F  S 25 &3q N2 G  S 5~U5N2 H  S _44CN2 I  S 3!4!T 2&}8! Q # R2&P8!V 4  C "`U55jP K  3 "`2 2P L  3 "`77-P M  3 "`7s}8P N  3 "`e6Z!6!P O  3 "`n3v 3 P P  3 "`3&#4 S  0635 Q(a) 2   T  0<6:< Q(b) 2  K8 4H6* | b3F*^   S .AFigure34G%   6$64L%H6* /Figure 4. ESR spectra of spin probe diffusing in NR irradiated with 300 kGy. The probe incorporation temperatures were: (a) 4 C and (b) 24 C. Spectra were measured at 19 C. &(2          1Rz V  S .AFigure4=0Pc  6̸6Q0 U Figure 3. ESR spectra of spin probe diffusing in NR irradiated with 200 kGy measured at 0 C. The probe incorporation temperatures were: (a) 16 C and (b) 24 C.&(2         ,lu/P x?  6B68Y0< Figure 2. ESR spectra of spin probe diffusing in nonirradiated NR measured at -10 C. The probe incorporation temperatures were: (a) 4 C, (b) 24 C and (c) 37 C.&(2      "Ck V  S .A Figure2m'L08I 3@-I[P   #"2&@R2G[P   BM6?*FN-I[P 15.1,(bB  @  @@``   BH6??N*F[P ~24,(bB  @  @@``   B6?*F7M-IN 20.9,(bB  @  @@``   B6??7M*FN }4,(bB  @  @@``   Bx6?;97M?[P ~19,(bB  @  @@``   Bo6?37M;9[P  NR 300 kGy, ( bB  @  @@``   B96?*FK-I7M 2.32,(bB  @  @@``   B6??K*F7M ~24,(bB  @  @@``   B6?*FJ-IK 2.47,(bB  @  @@``   B6??J*FK ~16,(bB  @  @@``   BQ?;9J?7M }0,(bB  @  @@``   B@Q?3J;97M  NR 200 kGy, ( bB  @  @@``   BHQ?*FH-IJ 1.15,(bB  @  @@``   BTQ??H*FJ ~37,(bB  @  @@``   BQ?*FF-IH 1.35,(bB  @  @@``   B\Q??F*FH ~24,(bB  @  @@``   BfQ?*F\E-IF 1.61,(bB  @  @@``   B|"Q??\E*FF }4,(bB  @  @@``   BliQ?;9\E?J -10,(bB  @  @@``   B CQ?3\E;9J NR 0 kGy, (bB  @  @@``e   N4jQ2?"`*F@-I\E In/Iwb(bjbjB&   @  @@``9   NUQ2?"`?@*F\E 'Temperature of probe incorporation / C.(('bB ( @  @@``m   N/Q2?"`;9@?\E Temperature of measurement / CL ( b"bB*   @  @@``   NwQ2?"`3@;9\E Sample.(bB  @  @@``ZB   s *Ԕ ?3@-I@ZB   s *Ԕ ?3[P-I[PZB   s *Ԕ ?3@3[PZB   s *Ԕ ?-I@-I[PZB   s *Ԕ ?3\E-I\EZB   s *Ԕ ?;9@;9[PZB   s *Ԕ ??@?[PZB   s *Ԕ ?*F@*F[PZB   s *Ԕ ?3J-IJZB   s *1 ??F-IFZB   s *1 ??H-IHZB '  s *Ԕ ?37M-I7MZB 5  s *1 ??K-IKZB T  s *1 ??N-IN q 0TQ=Q2FGT GkTable 1. Intensity ratios of the narrow (In) and broad (Iw) components of ESR spectra shown in Figures 2-4.rl(2!   2(  Em HL /$R2(  # "<_0&\   0HQ/$R2% 2Figure 1. Typical ESR spectra of spin probe in NR:&3(2 *b 8X   0Q"%+(H@8___PPT9  L^narrow (T > Tg) broad (T < Tg) bimodal (TH"T5mT)l0!    H       8XV  S .AFigure1tLO/"XB r 0De""XB s 0DwZ$Z$#L #& v # Ny"%R t  0Q#6% bIw& 2   u  0ԳQ%& bIn& 2  !  ZQ{f&" `) Materials and Methods(266   Z3Q{f&" `4X)tZ Z References (2 6   ZN{f&" `4XHtZ [ Conclusions (2 6   Z.N{f&" `H WResults(26   tAU<܍ ?Pozadina1"@` 3380___PPT10.@[r^ 1.(kJmiw   PCorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 Graphic`/ 0DArialNew RomanTT-ܖ 0ܖ"DTimes New RomanTT-ܖ 0ܖ@ . @n?" dd@  @@`` x421  2$V0,Hw6b$HIG'"@"$vHηΈ={>cپb$ `يB-/*b$9,@?_"ml\ $b$7&(1pwz2$C^g¿pSK;&s b$Oh,m1[+ 0AA 3ff3ff@ʚ;:ʚ;g4!d!d- 0p:@p<<4dddd w 0T- 0___PPT10 pp___PPT9kc[nQy  a*lD!@PNG  IHDR exsRGBNPLTEkc{絔έֽεƭƥƽ{s cmPPJCmp0712x~tRNS AyIDATMI0{d{1@Gs @c3|bXֻ$镰3дY ;6TJ~UCo@{} P{4$]$gc>/13"+^ZCLKs}XmIENDB`O  =f 0 ք΄  d    (  l J 61"`HU~   BA ??    TN gKgKff "`kJ  f^ESR - Spin Probe Method in Studying Crosslinked Elastomers: an Effect of the Probe Incorporation Temperature M. Didovi1, D. Klepac1 and S. Vali1,2 1 University of Rijeka, School of Medicine, Brae Branchetta 20, Rijeka, 51000, Croatia 2 Rudjer Boakovi Institute, Bijeni ka 54, Zagreb,10000, Croatia<0m<( , , , , , ,   V   >  ; %          D    )  08I-  !D<4___PPT9 } spin probe: !   i#Dl  0s-3Z?5 D EXPERIMENTAL 2 (ff   0(-      !"#$%&'()*+,-./0123456789:;<=>?@ABCDEFGHIJKLMNOPQRSTUVWXYZ[\]^_`abcdefghijklmnopqrstuvwxz{|}~$ tu% .4-hydroxy-2,2,6,6-tetramethylpiperidine-1-oxyl/ 2/ B  XB  0D3f) kJ   0|-*M4A GN < 2    Z`C`CA ?"6@ NNN?NQ@ G0   Z,w-{f&" `) Z Objective  (2 6 4  # A( g1  0| D<4___PPT9 natural rubber (NR) latex  62 wt.% of dry matter (The Rubber Research Institute of India)*2!- _  8 nn[  0-5)SD<4___PPT9 natural rubber latex containing 62 wt.% of dry matter was irradiated with different total irradiation doses of 200 kGy and 300 kGy irradiated NR latex was deluted by ammonia solution (0.6 wt.%) up to 25 wt.% of solid content ~1mm thick NR films were prepared by removing the liquid phase at room temperature spin probe was incorporated in NR samples by swelling the samples in the probe solution at 4 C, 16 C, 24 C and 37 C. The solvent was toluene. solvent was slowly removed by evaporation; all samples were then annealed at 60 C for 72 hours ESR spectra were recorded on Varian E-109 ESR spectrometer equipped with Bruker ER 041 XG microwave bridge and Bruker ER 4111 VT variable temperature unit! ^! S! ! `! !            H 3T|  0 FD<4___PPT9 pTo investigate the influence of the temperature of spin probe incorporation process on the shape of ESR spectra.q!q P , *  P>f p 6t6[HdD<4___PPT9 fthe shape of ESR spectra of the spin probe in heterogeneous systems, as shown for NR, depends on the probe incorporation temperature the increase of the probe incorporation temperature results in a higher amount of the broad component higher probe incorporation temperature allows probe molecules to diffuse into the higher density regions of the matrix and consequently leads to the restriction in probe dynamics:!(2 X              o 6 [[ )b !L. J. Berliner, Spin Labeling: Theory and Applications Vol 1. and Vol 2., Academic Press, 1976. Z. Veksli, M Andreis, B. Rakvin, ESR spectroscopy for the study of polymer heterogeneity, Prog Polym. Sci. 25 (2000) 949-986.(2&  !  C*8 E4/I>  c,R2G=   6D6(5(<[I> qFigure 5. Schematic representation of the spin probe incorporation process at (a) 4 C and (b) 37 C in NR matrix$r 2 i    ffHH'T >3wH$  # E4/I+; &@ 3wxH$ V >3wH$B   3 :>>B   3 BLCz B   3 C#-D~#B   3 UEEB   3 ?M@YB   3 <pE=B   3 R@ @!H   B&CDE|F41Yv*FFHVfXv8VV&*Z(t8@          "`>I`D}0   # B CDEFh1FFT H XhThhD4:X$ ` ` $ Zb<D,$      v  * @ 8 t V$ 8p4ff8(DrhtZhJ814@                       "`=4+G#!   zBCz DEFP144 { ZN <  < x2 ,    @ * N X  z t\ (> T  ^ rP  F` ~ $ v4XDrtTF6DD8b*vV *  h fx%(@                 "`?wF"@   # B C DE$Fl1IIB ` p~  &` $ 6prB TP T    P 4` 4bf V n  & P 4 |    8 * 0     ~ :` B , ` x$ p<h(t:XHvX:8VtJxV<<34@                        "`?xH$\ !  # BC DE0Fp1LLuV( t8 f ,x:<H<xV,VV8  Hh <Ht< (F (HF6Df:D,HB   n  V  P    ` $ U 58@                         3"`[;4@# "  jBCDEFL111;vZX Z  vX::*Xv 8**F TXTTJZ<Tb<xRp:Hp8tTU#$@                "`I<@ $ #  B(CDEXF(1uZf<<8xt, 8H Hth(@       3"`>Bk#\2 $  S "`A A \2 %  S "`D!D!\2 &  S "`zC#C[\2 '  S "`?FwF\2 (  S "`>'>_\2 )  S "`=>\2 *  S "`= = \2 +  S "`A B\2 ,  S "`@q@\2 -  S "`c?0#?h#@ 18" U 3:"( <  B C DE$Fl1IIB ` p~  &` $ 6prB TP T    P 4` 4bf V n  & P 4 |    8 * 0     ~ :` B , ` x$ p<h(t:XHvX:8VtJxV<<34@                        "`48"H 9  B&CDE|F41Yv*FFHVfXv8VV&*Z(t8@          "`s3Q6 :  B CDEFh1FFT H XhThhD4:X$ ` ` $ Zb<D,$      v  * @ 8 t V$ 8p4ff8(DrhtZhJ814@                       "`2Y8  ;  zBCz DEFP144 { ZN <  < x2 ,    @ * N X  z t\ (> T  ^ rP  F` ~ $ v4XDrtTF6DD8b*vV *  h fx%(@                 "`37!D =  BC DE0Fp1LLuV( t8 f ,x:<H<xV,VV8  Hh <Ht< (F (HF6Df:D,HB   n  V  P    ` $ U 58@                         3"`1Y34! >  jBCDEFL111;vZX Z  vX::*Xv 8**F TXTTJZ<Tb<xRp:Hp8tTU#$@                "`&24q $ ?  B(CDEXF(1uZf<<8xt, 8H Hth(@       3"`Y35!N2 @  S  5K E5 N2 A  S 6 6!N2 B  S 5n16N2 C  S {707lN2 D  S S3[3N2 E  S 223N2 F  S 25 &3q N2 G  S 5~U5N2 H  S _44CN2 I  S 3!4!T 2&}8! Q # R2&P8!V 4  C "`U55jP K  3 "`2 2P L  3 "`77-P M  3 "`7s}8P N  3 "`e6Z!6!P O  3 "`n3v 3 P P  3 "`3&#4 S  0635 Q(a) 2   T  0<6:< Q(b) 2  K8 4H6* | b3F*^   S .AFigure34G%   6$64L%H6* /Figure 4. ESR spectra of spin probe diffusing in NR irradiated with 300 kGy. The probe incorporation temperatures were: (a) 4 C and (b) 24 C. Spectra were measured at 19 C. &(2          1Rz V  S .AFigure4=0Pc  6̸6Q0 U Figure 3. ESR spectra of spin probe diffusing in NR irradiated with 200 kGy measured at 0 C. The probe incorporation temperatures were: (a) 16 C and (b) 24 C.&(2         ,lu/P x?  6B68Y0< Figure 2. ESR spectra of spin probe diffusing in nonirradiated NR measured at -10 C. The probe incorporation temperatures were: (a) 4 C, (b) 24 C and (c) 37 C.&(2      "Ck V  S .A Figure2m'L08I 3@-I[P   #"2&@R2G[P   BM6?*FN-I[P 15.1,(bB  @  @@``   BH6??N*F[P ~24,(bB  @  @@``   B6?*F7M-IN 20.9,(bB  @  @@``   B6??7M*FN }4,(bB  @  @@``   Bx6?;97M?[P ~19,(bB  @  @@``   Bo6?37M;9[P  NR 300 kGy, ( bB  @  @@``   B96?*FK-I7M 2.32,(bB  @  @@``   B6??K*F7M ~24,(bB  @  @@``   B6?*FJ-IK 2.47,(bB  @  @@``   B6??J*FK ~16,(bB  @  @@``   BQ?;9J?7M }0,(bB  @  @@``   B@Q?3J;97M  NR 200 kGy, ( bB  @  @@``   BHQ?*FH-IJ 1.15,(bB  @  @@``   BTQ??H*FJ ~37,(bB  @  @@``   BQ?*FF-IH 1.35,(bB  @  @@``   B\Q??F*FH ~24,(bB  @  @@``   BfQ?*F\E-IF 1.61,(bB  @  @@``   B|"Q??\E*FF }4,(bB  @  @@``   BliQ?;9\E?J -10,(bB  @  @@``   B CQ?3\E;9J NR 0 kGy, (bB  @  @@``e   N4jQ2?"`*F@-I\E In/Iwb(bjbjB&   @  @@``9   NUQ2?"`?@*F\E 'Temperature of probe incorporation / C.(('bB ( @  @@``m   N/Q2?"`;9@?\E Temperature of measurement / CL ( b"bB*   @  @@``   NwQ2?"`3@;9\E Sample.(bB  @  @@``ZB   s *Ԕ ?3@-I@ZB   s *Ԕ ?3[P-I[PZB   s *Ԕ ?3@3[PZB   s *Ԕ ?-I@-I[PZB   s *Ԕ ?3\E-I\EZB   s *Ԕ ?;9@;9[PZB   s *Ԕ ??@?[PZB   s *Ԕ ?*F@*F[PZB   s *Ԕ ?3J-IJZB   s *1 ??F-IFZB   s *1 ??H-IHZB '  s *Ԕ ?37M-I7MZB 5  s *1 ??K-IKZB T  s *1 ??N-IN q 0TQ=Q2FGT 5kTable 1. Intensity ratios of the narrow (In) and broad (Iw) components of ESR spectra shown in Figures 2-4.rl(2!   2  Em HL /$R2(  # "<_0&\   0HQ/$R2% 2Figure 1. Typical ESR spectra of spin probe in NR:&3(2 *b 8X   0Q"%+(H@8___PPT9  L^narrow (T > Tg) broad (T < Tg) bimodal (TH"T5mT)l0!    H       8XV  S .AFigure1tLO/"XB r 0De""XB s 0DwZ$Z$#L #& v # Ny"%R t  0Q#6% bIw& 2   u  0ԳQ%& bIn& 2  !  ZQ{f&" `) Materials and Methods(266   Z3Q{f&" `4X)tZ Z References (2 6   ZN{f&" `4XHtZ [ Conclusions (2 6   Z.N{f&" `H WResults(26   tAU<܍ ?Pozadina1"@` 3380___PPT10.@[r^f^c 1.(kJmiw   PCorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 Graphic`/ 0DArialNew RomanTT-ܖ 0ܖ"DTimes New RomanTT-ܖ 0ܖ@ . @n?" dd@  @@`` x421  2$V0,Hw6b$HIG'"@"$vHηΈ={>cپb$ `يB-/*b$9,@?_"ml\ $b$7&(1pwz2$C^g¿pSK;&s b$Oh,m1[+ 0AA 3ff3ff@ʚ;:ʚ;g4!d!d- 0p:@p<<4dddd w 0T- 0___PPT10 pp___PPT9kc[nQy  a*lD!@PNG  IHDR exsRGBNPLTEkc{絔έֽεƭƥƽ{s cmPPJCmp0712x~tRNS AyIDATMI0{d{1@Gs @c3|bXֻ$镰3дY ;6TJ~UCo@{} P{4$]$gc>/13"+^ZCLKs}XmIENDB`O  =r{ 1.(kJmiw   PCorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 Graphic`/ 0DArialNew RomanTT-ܖ 0ܖ"DTimes New RomanTT-ܖ 0ܖ@ . @n?" dd@  @@`` x421  2$V0,Hw6b$HIG'"@"$vHηΈ={>cپb$ `يB-/*b$9,@?_"ml\ $b$7&(1pwz2$C^g¿pSK;&s b$Oh,m1[+ 0AA 3ff3ff@ʚ;:ʚ;g4dd- 0^p:@p<<4dddd w 0T- 0___PPT10 pp___PPT9kc[nQy  a*lD!@PNG  IHDR exsRGBNPLTEkc{絔έֽεƭƥƽ{s cmPPJCmp0712x~tRNS AyIDATMI0{d{1@Gs @c3|bXֻ$镰3дY ;6TJ~UCo@{} P{4$]$gc>/13"+^ZCLKs}XmIENDB`O  =n 0 ބք  d    (  l J 61"`HU~   BA ??    TN gKgKff "`kJ  f^ESR - Spin Probe Method in Studying Crosslinked Elastomers: an Effect of the Probe Incorporation Temperature M. Didovi1, D. Klepac1 and S. Vali1,2 1 University of Rijeka, School of Medicine, Brae Branchetta 20, Rijeka, 51000, Croatia 2 Rudjer Boakovi Institute, Bijeni ka 54, Zagreb,10000, Croatia<0m<( , , , , , ,   V   >  ; %          D    )  08I-  !D<4___PPT9 } spin probe: !   i#Dl  0s-3Z?5 D EXPERIMENTAL 2 (ff   0(-$ tu% .4-hydroxy-2,2,6,6-tetramethylpiperidine-1-oxyl/ 2/ B  XB  0D3f) kJ   0|-*M4A GN < 2    Z`C`CA ?"6@ NNN?NQ@ G0   Z,w-{f&" `) Z Objective  (2 6 4  # A( g1  0| D<4___PPT9 natural rubber (NR) latex  62 wt.% of dry matter (The Rubber Research Institute of India)*2!- _  8 nn[  0-5)SD<4___PPT9 natural rubber latex containing 62 wt.% of dry matter was irradiated with different total irradiation doses of 200 kGy and 300 kGy irradiated NR latex was deluted by ammonia solution (0.6 wt.%) up to 25 wt.% of solid content ~1mm thick NR films were prepared by removing the liquid phase at room temperature spin probe was incorporated in NR samples by swelling the samples in the probe solution at 4 C, 16 C, 24 C and 37 C. The solvent was toluene. solvent was slowly removed by evaporation; all samples were then annealed at 60 C for 72 hours ESR spectra were recorded on Varian E-109 ESR spectrometer equipped with Bruker ER 041 XG microwave bridge and Bruker ER 4111 VT variable temperature unit! ^! S! ! `! !            H 3T|  0 FD<4___PPT9 pTo investigate the influence of the temperature of spin probe incorporation process on the shape of ESR spectra.q!q P , *  P>f  p 6t6[HdD<4___PPT9 nthe shape of ESR spectra of the spin probe in heterogeneous systems, as shown for NR, depends on the probe incorporation temperature the increase of the probe incorporation temperature results in a higher amount of the broad component higher probe incorporation temperature allows probe molecules to diffuse into the higher density regions of the matrix and consequently leads to the restriction in probe dynamics:!(2 `              o 6 [[ )b !L. J. Berliner, Spin Labeling: Theory and Applications Vol 1. and Vol 2., Academic Press, 1976. Z. Veksli, M Andreis, B. Rakvin, ESR spectroscopy for the study of polymer heterogeneity, Prog Polym. Sci. 25 (2000) 949-986.(2&  !  C*8 E4/I>  c,R2G=   6D6(5(<[I> qFigure 5. Schematic representation of the spin probe incorporation process at (a) 4 C and (b) 37 C in NR matrix$r 2 i    ffHH'T >3wH$  # E4/I+; &@ 3wxH$ V >3wH$B   3 :>>B   3 BLCz B   3 C#-D~#B   3 UEEB   3 ?M@YB   3 <pE=B   3 R@ @!H   B&CDE|F41Yv*FFHVfXv8VV&*Z(t8@          "`>I`D}0   # B CDEFh1FFT H XhThhD4:X$ ` ` $ Zb<D,$      v  * @ 8 t V$ 8p4ff8(DrhtZhJ814@                       "`=4+G#!   zBCz DEFP144 { ZN <  < x2 ,    @ * N X  z t\ (> T  ^ rP  F` ~ $ v4XDrtTF6DD8b*vV *  h fx%(@                 "`?wF"@   # B C DE$Fl1IIB ` p~  &` $ 6prB TP T    P 4` 4bf V n  & P 4 |    8 * 0     ~ :` B , ` x$ p<h(t:XHvX:8VtJxV<<34@                        "`?xH$\ !  # BC DE0Fp1LLuV( t8 f ,x:<H<xV,VV8  Hh <Ht< (F (HF6Df:D,HB   n  V  P    ` $ U 58@                         3"`[;4@# "  jBCDEFL111;vZX Z  vX::*Xv 8**F TXTTJZ<Tb<xRp:Hp8tTU#$@                "`I<@ $ #  B(CDEXF(1uZf<<8xt, 8H Hth(@       3"`>Bk#\2 $  S "`A A \2 %  S "`D!D!\2 &  S "`zC#C[\2 '  S "`?FwF\2 (  S "`>'>_\2 )  S "`=>\2 *  S "`= = \2 +  S "`A B\2 ,  S "`@q@\2 -  S "`c?0#?h#@ 18" U 3:"( <  B C DE$Fl1IIB ` p~  &` $ 6prB TP T    P 4` 4bf V n  & P 4 |    8 * 0     ~ :` B , ` x$ p<h(t:XHvX:8VtJxV<<34@                        "`48"H 9  B&CDE|F41Yv*FFHVfXv8VV&*Z(t8@          "`s3Q6 :  B CDEFh1FFT H XhThhD4:X$ ` ` $ Zb<D,$      v  * @ 8 t V$ 8p4ff8(DrhtZhJ814@                       "`2Y8  ;  zBCz DEFP144 { ZN <  < x2 ,    @ * N X  z t\ (> T  ^ rP  F` ~ $ v4XDrtTF6DD8b*vV *  h fx%(@                 "`37!D =  BC DE0Fp1LLuV( t8 f ,x:<H<xV,VV8  Hh <Ht< (F (HF6Df:D,HB   n  V  P    ` $ U 58@                         3"`1Y34! >  jBCDEFL111;vZX Z  vX::*Xv 8**F TXTTJZ<Tb<xRp:Hp8tTU#$@                "`&24q $ ?  B(CDEXF(1uZf<<8xt, 8H Hth(@       3"`Y35!N2 @  S  5K E5 N2 A  S 6 6!N2 B  S 5n16N2 C  S {707lN2 D  S S3[3N2 E  S 223N2 F  S 25 &3q N2 G  S 5~U5N2 H  S _44CN2 I  S 3!4!T 2&}8! Q # R2&P8!V 4  C "`U55jP K  3 "`2 2P L  3 "`77-P M  3 "`7s}8P N  3 "`e6Z!6!P O  3 "`n3v 3 P P  3 "`3&#4 S  0635 Q(a) 2   T  0<6:< Q(b) 2  K8 4H6* | b3F*^   S .AFigure34G%   6$64L%H6* /Figure 4. ESR spectra of spin probe diffusing in NR irradiated with 300 kGy. The probe incorporation temperatures were: (a) 4 C and (b) 24 C. Spectra were measured at 19 C. &(2          1Rz V  S .AFigure4=0Pc  6̸6Q0 U Figure 3. ESR spectra of spin probe diffusing in NR irradiated with 200 kGy measured at 0 C. The probe incorporation temperatures were: (a) 16 C and (b) 24 C.&(2         ,lu/P x?  6B68Y0< Figure 2. ESR spectra of spin probe diffusing in nonirradiated NR measured at -10 C. The probe incorporation temperatures were: (a) 4 C, (b) 24 C and (c) 37 C.&(2      "Ck V  S .A Figure2m'L08I 3@-I[P   #"2&@R2G[P   BM6?*FN-I[P 15.1,(bB  @  @@``   BH6??N*F[P ~24,(bB  @  @@``   B6?*F7M-IN 20.9,(bB  @  @@``   B6??7M*FN }4,(bB  @  @@``   Bx6?;97M?[P ~19,(bB  @  @@``   Bo6?37M;9[P  NR 300 kGy, ( bB  @  @@``   B96?*FK-I7M 2.32,(bB  @  @@``   B6??K*F7M ~24,(bB  @  @@``   B6?*FJ-IK 2.47,(bB  @  @@``   B6??J*FK ~16,(bB  @  @@``   BQ?;9J?7M }0,(bB  @  @@``   B@Q?3J;97M  NR 200 kGy, ( bB  @  @@``   BHQ?*FH-IJ 1.15,(bB  @  @@``   BTQ??H*FJ ~37,(bB  @  @@``   BQ?*FF-IH 1.35,(bB  @  @@``   B\Q??F*FH ~24,(bB  @  @@``   BfQ?*F\E-IF 1.61,(bB  @  @@``   B|"Q??\E*FF }4,(bB  @  @@``   BliQ?;9\E?J -10,(bB  @  @@``   B CQ?3\E;9J NR 0 kGy, (bB  @  @@``e   N4jQ2?"`*F@-I\E In/Iwb(bjbjB&   @  @@``9   NUQ2?"`?@*F\E 'Temperature of probe incorporation / C.(('bB ( @  @@``m   N/Q2?"`;9@?\E Temperature of measurement / CL ( b"bB*   @  @@``   NwQ2?"`3@;9\E Sample.(bB  @  @@``ZB   s *Ԕ ?3@-I@ZB   s *Ԕ ?3[P-I[PZB   s *Ԕ ?3@3[PZB   s *Ԕ ?-I@-I[PZB   s *Ԕ ?3\E-I\EZB   s *Ԕ ?;9@;9[PZB   s *Ԕ ??@?[PZB   s *Ԕ ?*F@*F[PZB   s *Ԕ ?3J-IJZB   s *1 ??F-IFZB   s *1 ??H-IHZB '  s *Ԕ ?37M-I7MZB 5  s *1 ??K-IKZB T  s *1 ??N-IN q 0TQ=Q2FGT 5kTable 1. Intensity ratios of the narrow (In) and broad (Iw) components of ESR spectra shown in Figures 2-4.rl(2!   2  Em HL /$R2(  # "<_0&\   0HQ/$R2% 2Figure 1. Typical ESR spectra of spin probe in NR:&3(2 *b 8X   0Q"%+(H@8___PPT9  L^narrow (T > Tg) broad (T < Tg) bimodal (TH"T5mT)l0!    H       8XV  S .AFigure1tLO/"XB r 0De""XB s 0DwZ$Z$#L #& v # Ny"%R t  0Q#6% bIw& 2   u  0ԳQ%& bIn& 2  !  ZQ{f&" ` V Materials and Methods(266   Z3Q{f&" `4X)tZ Z References (2 6   ZN{f&" `4XHtZ [ Conclusions (2 6   Z.N{f&" `H WResults(26   tAU<܍ ?Pozadina1"@` 3380___PPT10.@[r ? 1.(kJmiw   PCorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 Graphic`/ 0DArialNew RomanTT-ܖ 0ܖ"DTimes New RomanTT-ܖ 0ܖ@ . @n?" dd@  @@`` x421  2$V0,Hw6b$HIG'"@"$vHηΈ={>cپb$ `يB-/*b$9,@?_"ml\ $b$7&(1pwz2$C^g¿pSK;&s b$Oh,m1[+ 0AA 3ff3ff@ʚ;:ʚ;g4dd- 0^p:@p<<4dddd w 0T- 0___PPT10 pp___PPT9kc[nQy  a*lD!@PNG  IHDR exsRGBNPLTEkc{絔έֽεƭƥƽ{s cmPPJCmp0712x~tRNS AyIDATMI0{d{1@Gs @c3|bXֻ$镰3дY ;6TJ~UCo@{} P{4$]$gc>/13"+^ZCLKs}XmIENDB`O  =r͂' 1.(kJmiw   QCorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 Graphic`/ 0DArialNew RomanTT,4ܖ 0ܖDTimes New RomanTT,4ܖ 0ܖ@ . @n?" dd@  @@`` x421  2$V0,Hw6b$HIG'"@"$vHηΈ={>cپb$ `يB-/*b$9,@?_"ml\ $b$7&(1pwz2$C^g¿pSK;&s b$Oh,m1[+ 0AA 3ff3ff@ʚ;:ʚ;g4dd@ 0^p:@p<<4dddd w 0T4 0___PPT10 pp___PPT9kc[nQy  a*lD!@PNG  IHDR exsRGBNPLTEkc{絔έֽεƭƥƽ{s cmPPJCmp0712x~tRNS AyIDATMI0{d{1@Gs @c3|bXֻ$镰3дY ;6TJ~UCo@{} P{4$]$gc>/13"+^ZCLKs}XmIENDB`O  = 0   d    (  l J 61"`HU~   BA ??    T@7gKgKff "`kJ  f^ESR - Spin Probe Method in Studying Crosslinked Elastomers: an Effect of the Probe Incorporation Temperature M. Didovi1, D. Klepac1 and S. Vali1,2 1 University of Rijeka, School of Medicine, Brae Branchetta 20, Rijeka, 51000, Croatia 2 Rudjer Boakovi Institute, Bijeni ka 54, Zagreb,10000, Croatia<0m<( , , , , , ,   V   >  ; %          D    )  0ۖ  !D<4___PPT9 } spin probe: !   i#Dl  03Z?5 D EXPERIMENTAL 2 (ff   0$ tu% .4-hydroxy-2,2,6,6-tetramethylpiperidine-1-oxyl/ 2/ B  XB  0D3f) kJ   07*M4A GN < 2    Z`C`CA ?"6@ NNN?NQ@ G0   Z47{f&" `) Z Objective  (2 6 4  # A( g1  0D<4___PPT9 natural rubber (NR) latex  62 wt.% of dry matter (The Rubber Research Institute of India)*2!- _  8 nn[  0/75)SD<4___PPT9 natural rubber latex containing 62 wt.% of dry matter was irradiated with different total irradiation doses of 200 kGy and 300 kGy irradiated NR latex was deluted by ammonia solution (0.6 wt.%) up to 25 wt.% of solid content ~1mm thick NR films were prepared by removing the liquid phase at room temperature spin probe was incorporated in NR samples by swelling the samples in the probe solution at 4 C, 16 C, 24 C and 37 C. The solvent was toluene. solvent was slowly removed by evaporation; all samples were then annealed at 60 C for 72 hours ESR spectra were recorded on Varian E-109 ESR spectrometer equipped with Bruker ER 041 XG microwave bridge and Bruker ER 4111 VT variable temperature unit! ^! S! ! `! !            H 3T|  0lR7FD<4___PPT9 pTo investigate the influence of the temperature of spin probe incorporation process on the shape of ESR spectra.q!q P , *  P>f  p 67[HdD<4___PPT9 nthe shape of ESR spectra of the spin probe in heterogeneous systems, as shown for NR, depends on the probe incorporation temperature the increase of the probe incorporation temperature results in a higher amount of the broad component higher probe incorporation temperature allows probe molecules to diffuse into the higher density regions of the matrix and consequently leads to the restriction in probe dynamics:!(2 `              o 6\q7[[ )b !L. J. Berliner, Spin Labeling: Theory and Applications Vol 1. and Vol 2., Academic Press, 1976. Z. Veksli, M Andreis, B. Rakvin, ESR spectroscopy for the study of polymer heterogeneity, Prog Polym. Sci. 25 (2000) 949-986.(2&  !  C*8 E4/I>  c,R2G=   6h7(5(<[I> qFigure 5. Schematic representation of the spin probe incorporation process at (a) 4 C and (b) 37 C in NR matrix$r 2 i    ffHH'T >3wH$  # E4/I+; &@ 3wxH$ V >3wH$B   3 :>>B   3 BLCz B   3 C#-D~#B   3 UEEB   3 ?M@YB   3 <pE=B   3 R@ @!H   B&CDE|F41Yv*FFHVfXv8VV&*Z(t8@          "`>I`D}0   # B CDEFh1FFT H XhThhD4:X$ ` ` $ Zb<D,$      v  * @ 8 t V$ 8p4ff8(DrhtZhJ814@                       "`=4+G#!   zBCz DEFP144 { ZN <  < x2 ,    @ * N X  z t\ (> T  ^ rP  F` ~ $ v4XDrtTF6DD8b*vV *  h fx%(@                 "`?wF"@   # B C DE$Fl1IIB ` p~  &` $ 6prB TP T    P 4` 4bf V n  & P 4 |    8 * 0     ~ :` B , ` x$ p<h(t:XHvX:8VtJxV<<34@                        "`?xH$\ !  # BC DE0Fp1LLuV( t8 f ,x:<H<xV,VV8  Hh <Ht< (F (HF6Df:D,HB   n  V  P    ` $ U 58@                         3"`[;4@# "  jBCDEFL111;vZX Z  vX::*Xv 8**F TXTTJZ<Tb<xRp:Hp8tTU#$@                "`I<@ $ #  B(CDEXF(1uZf<<8xt, 8H Hth(@       3"`>Bk#\2 $  S "`A A \2 %  S "`D!D!\2 &  S "`zC#C[\2 '  S "`?FwF\2 (  S "`>'>_\2 )  S "`=>\2 *  S "`= = \2 +  S "`A B\2 ,  S "`@q@\2 -  S "`c?0#?h#@ 18" U 3:"( <  B C DE$Fl1IIB ` p~  &` $ 6prB TP T    P 4` 4bf V n  & P 4 |    8 * 0     ~ :` B , ` x$ p<h(t:XHvX:8VtJxV<<34@                        "`48"H 9  B&CDE|F41Yv*FFHVfXv8VV&*Z(t8@          "`s3Q6 :  B CDEFh1FFT H XhThhD4:X$ ` ` $ Zb<D,$      v  * @ 8 t V$ 8p4ff8(DrhtZhJ814@                       "`2Y8  ;  zBCz DEFP144 { ZN <  < x2 ,    @ * N X  z t\ (> T  ^ rP  F` ~ $ v4XDrtTF6DD8b*vV *  h fx%(@                 "`37!D =  BC DE0Fp1LLuV( t8 f ,x:<H<xV,VV8  Hh <Ht< (F (HF6Df:D,HB   n  V  P    ` $ U 58@                         3"`1Y34! >  jBCDEFL111;vZX Z  vX::*Xv 8**F TXTTJZ<Tb<xRp:Hp8tTU#$@                "`&24q $ ?  B(CDEXF(1uZf<<8xt, 8H Hth(@       3"`Y35!N2 @  S  5K E5 N2 A  S 6 6!N2 B  S 5n16N2 C  S {707lN2 D  S S3[3N2 E  S 223N2 F  S 25 &3q N2 G  S 5~U5N2 H  S _44CN2 I  S 3!4!T 2&}8! Q # R2&P8!V 4  C "`U55jP K  3 "`2 2P L  3 "`77-P M  3 "`7s}8P N  3 "`e6Z!6!P O  3 "`n3v 3 P P  3 "`3&#4 S  0735 Q(a) 2   T  07:< Q(b) 2  K8 4H6* | b3F*^   S .AFigure34G%   674L%H6* /Figure 4. ESR spectra of spin probe diffusing in NR irradiated with 300 kGy. The probe incorporation temperatures were: (a) 4 C and (b) 24 C. Spectra were measured at 19 C. &(2          1Rz V  S .AFigure4=0Pc  6, 8Q0 U Figure 3. ESR spectra of spin probe diffusing in NR irradiated with 200 kGy measured at 0 C. The probe incorporation temperatures were: (a) 16 C and (b) 24 C.&(2         ,lu/P x?  6078Y0< Figure 2. ESR spectra of spin probe diffusing in nonirradiated NR measured at -10 C. The probe incorporation temperatures were: (a) 4 C, (b) 24 C and (c) 37 C.&(2      "Ck V  S .A Figure2m'L08I 3@-I[P   #"2&@R2G[P   B'8?*FN-I[P 15.1,(bB  @  @@``   B18??N*F[P ~24,(bB  @  @@``   B ;8?*F7M-IN 20.9,(bB  @  @@``   BD8??7M*FN }4,(bB  @  @@``   BX58?;97M?[P ~19,(bB  @  @@``   B$I8?37M;9[P  NR 300 kGy, ( bB  @  @@``   BR8?*FK-I7M 2.32,(bB  @  @@``   Bx\8??K*F7M ~24,(bB  @  @@``   B8]8?*FJ-IK 2.47,(bB  @  @@``   BS8??J*FK ~16,(bB  @  @@``   B@8?;9J?7M }0,(bB  @  @@``   B8?3J;97M  NR 200 kGy, ( bB  @  @@``   Bz8?*FH-IJ 1.15,(bB  @  @@``   Bx8??H*FJ ~37,(bB  @  @@``   B`8?*FF-IH 1.35,(bB  @  @@``   B\8??F*FH ~24,(bB  @  @@``   B8?*F\E-IF 1.61,(bB  @  @@``   B8??\E*FF }4,(bB  @  @@``   Bx8?;9\E?J -10,(bB  @  @@``   B 8?3\E;9J NR 0 kGy, (bB  @  @@``e   N82?"`*F@-I\E In/Iwb(bjbjB&   @  @@``9   N82?"`?@*F\E 'Temperature of probe incorporation / C.(('bB ( @  @@``m   N92?"`;9@?\E Temperature of measurement / CL ( b"bB*   @  @@``   N92?"`3@;9\E Sample.(bB  @  @@``ZB   s *Ԕ ?3@-I@ZB   s *Ԕ ?3[P-I[PZB   s *Ԕ ?3@3[PZB   s *Ԕ ?-I@-I[PZB   s *Ԕ ?3\E-I\EZB   s *Ԕ ?;9@;9[PZB   s *Ԕ ??@?[PZB   s *Ԕ ?*F@*F[PZB   s *Ԕ ?3J-IJZB   s *1 ??F-IFZB   s *1 ??H-IHZB '  s *Ԕ ?37M-I7MZB 5  s *1 ??K-IKZB T  s *1 ??N-IN q 0.9=Q2FGT 5kTable 1. Intensity ratios of the narrow (In) and broad (Iw) components of ESR spectra shown in Figures 2-4.rl(2!   2  Em HL /$R2(  # "<_0&\   0=9/$R2% 2Figure 1. Typical ESR spectra of spin probe in NR:&3(2 *b 8X   09"%+(H@8___PPT9  L^narrow (T > Tg) broad (T < Tg) bimodal (TH"T5mT)l0!    H       8XV  S .AFigure1tLO/"XB r 0De""XB s 0DwZ$Z$#L #& v # Ny"%R t  0S9#6% bIw& 2   u  0W9%& bIn& 2  !  Z[9{f&" ` V Materials and Methods(266   Z@`9{f&" `4X)tZ Z References (2 6   Zd9{f&" `4XHtZ [ Conclusions (2 6   Zh9{f&" `H WResults(26J  c $ ?"@` 3380___PPT10.@[r[7 1.(kJmiw   RCorelDRAW (CorelDRAW.Graphic.110,CorelDRAW 11.0 Graphic`/ 0DArialNew RomanTTH6ܖ 0ܖDTimes New RomanTTH6ܖ 0ܖ@ . @n?" dd@  @@`` x421  2$V0,Hw6b$HIG'"@"$vHηΈ={>cپb$ `يB-/*b$9,@?_"ml\ $b$7&(1pwz2$C^g¿pSK;&s b$Oh,m1[+ 0AA 3ff3ff@ʚ;:ʚ;g4ddB 0^p:@p<<4dddd w 0T$6 0___PPT10 pp___PPT9kc[nQy  a*lD!@PNG  IHDR exsRGBNPLTEkc{絔έֽεƭƥƽ{s cmPPJCmp0712x~tRNS AyIDATMI0{d{1@Gs @c3|bXֻ$镰3дY ;6TJ~UCo@{} P{4$]$gc>/13"+^ZCLKs}XmIENDB`O  = 0   d    (  l J 61"`HU~   BA ??    T6gKgKff "`kJ  f^ESR - Spin Probe Method in Studying Crosslinked Elastomers: an Effect of the Probe Incorporation Temperature M. Didovi1, D. Klepac1 and S. Vali1,2 1 University of Rijeka, School of Medicine, Brae Branchetta 20, Rijeka, 51000, Croatia 2 Rudjer Boakovi Institute, Bijeni ka 54, Zagreb,10000, Croatia<0m<( , , , , , ,   V   >  ; %          D    )  0  !D<4___PPT9 } spin probe: !   i#Dl  03Z?5 D EXPERIMENTAL 2 (ff   0 6$ tu% .4-hydroxy-2,2,6,6-tetramethylpiperidine-1-oxyl/ 2/ B  XB  0D3f) kJ   06*M4A GN < 2    Z`C`CA ?"6@ NNN?NQ@ G0   Z6{f&" `) Z Objective  (2 6 4  # A( g1  0)6D<4___PPT9 natural rubber (NR) latex  62 wt.% of dry matter (The Rubber Research Institute of India)*2!- _  8 nn[  065)SD<4___PPT9 natural rubber latex containing 62 wt.% of dry matter was irradiated with different total irradiation doses of 200 kGy and 300 kGy irradiated NR latex was deluted by ammonia solution (0.6 wt.%) up to 25 wt.% of solid content ~1mm thick NR films were prepared by removing the liquid phase at room temperature spin probe was incorporated in NR samples by swelling the samples in the probe solution at 4 C, 16 C, 24 C and 37 C. The solvent was toluene. solvent was slowly removed by evaporation; all samples were then annealed at 60 C for 72 hours ESR spectra were recorded on Varian E-109 ESR spectrometer equipped with Bruker ER 041 XG microwave bridge and Bruker ER 4111 VT variable temperature unit! ^! S! ! `! !            H 3T|  0LT6FD<4___PPT9 pTo investigate the influence of the temperature of spin probe incorporation process on the shape of ESR spectra.q!q P , *  P>f  p 6X6[HdD<4___PPT9 nthe shape of ESR spectra of the spin probe in heterogeneous systems, as shown for NR, depends on the probe incorporation temperature the increase of the probe incorporation temperature results in a higher amount of the broad component higher probe incorporation temperature allows probe molecules to diffuse into the higher density regions of the matrix and consequently leads to the restriction in probe dynamics:!(2 `              o 6u6[[ )b !L. J. Berliner, Spin Labeling: Theory and Applications Vol 1. and Vol 2., Academic Press, 1976. Z. Veksli, M Andreis, B. Rakvin, ESR spectroscopy for the study of polymer heterogeneity, Prog Polym. Sci. 25 (2000) 949-986.(2&  !  C*8 E4/I>  c,R2G=   66(5(<[I> qFigure 5. Schematic representation of the spin probe incorporation process at (a) 4 C and (b) 37 C in NR matrix$r 2 i    ffHH'T >3wH$  # E4/I+; &@ 3wxH$ V >3wH$B   3 :>>B   3 BLCz B   3 C#-D~#B   3 UEEB   3 ?M@YB   3 <pE=B   3 R@ @!H   B&CDE|F41Yv*FFHVfXv8VV&*Z(t8@          "`>I`D}0   # B CDEFh1FFT H XhThhD4:X$ ` ` $ Zb<D,$      v  * @ 8 t V$ 8p4ff8(DrhtZhJ814@                       "`=4+G#!   zBCz DEFP144 { ZN <  < x2 ,    @ * N X  z t\ (> T  ^ rP  F` ~ $ v4XDrtTF6DD8b*vV *  h fx%(@                 "`?wF"@   # B C DE$Fl1IIB ` p~  &` $ 6prB TP T    P 4` 4bf V n  & P 4 |    8 * 0     ~ :` B , ` x$ p<h(t:XHvX:8VtJxV<<34@                        "`?xH$\ !  # BC DE0Fp1LLuV( t8 f ,x:<H<xV,VV8  Hh <Ht< (F (HF6Df:D,HB   n  V  P    ` $ U 58@                         3"`[;4@# "  jBCDEFL111;vZX Z  vX::*Xv 8**F TXTTJZ<Tb<xRp:Hp8tTU#$@                "`I<@ $ #  B(CDEXF(1uZf<<8xt, 8H Hth(@       3"`>Bk#\2 $  S "`A A \2 %  S "`D!D!\2 &  S "`zC#C[\2 '  S "`?FwF\2 (  S "`>'>_\2 )  S "`=>\2 *  S "`= = \2 +  S "`A B\2 ,  S "`@q@\2 -  S "`c?0#?h#@ 18" U 3:"( <  B C DE$Fl1IIB ` p~  &` $ 6prB TP T    P 4` 4bf V n  & P 4 |    8 * 0     ~ :` B , ` x$ p<h(t:XHvX:8VtJxV<<34@                        "`48"H 9  B&CDE|F41Yv*FFHVfXv8VV&*Z(t8@          "`s3Q6 :  B CDEFh1FFT H XhThhD4:X$ ` ` $ Zb<D,$      v  * @ 8 t V$ 8p4ff8(DrhtZhJ814@                       "`2Y8  ;  zBCz DEFP144 { ZN <  < x2 ,    @ * N X  z t\ (> T  ^ rP  F` ~ $ v4XDrtTF6DD8b*vV *  h fx%(@                 "`37!D =  BC DE0Fp1LLuV( t8 f ,x:<H<xV,VV8  Hh <Ht< (F (HF6Df:D,HB   n  V  P    ` $ U 58@                         3"`1Y34! >  jBCDEFL111;vZX Z  vX::*Xv 8**F TXTTJZ<Tb<xRp:Hp8tTU#$@                "`&24q $ ?  B(CDEXF(1uZf<<8xt, 8H Hth(@       3"`Y35!N2 @  S  5K E5 N2 A  S 6 6!N2 B  S 5n16N2 C  S {707lN2 D  S S3[3N2 E  S       !"#$223N2 F  S 25 &3q N2 G  S 5~U5N2 H  S _44CN2 I  S 3!4!T 2&}8! Q # R2&P8!V 4  C "`U55jP K  3 "`2 2P L  3 "`77-P M  3 "`7s}8P N  3 "`e6Z!6!P O  3 "`n3v 3 P P  3 "`3&#4 S  0@635 Q(a) 2   T  06:< Q(b) 2  K8 4H6* | b3F*^   S .AFigure34G%   6X64L%H6* /Figure 4. ESR spectra of spin probe diffusing in NR irradiated with 300 kGy. The probe incorporation temperatures were: (a) 4 C and (b) 24 C. Spectra were measured at 19 C. &(2          1Rz V  S .AFigure4=0Pc  67Q0 U Figure 3. ESR spectra of spin probe diffusing in NR irradiated with 200 kGy measured at 0 C. The probe incorporation temperatures were: (a) 16 C and (b) 24 C.&(2         ,lu/P x?  6\78Y0< Figure 2. ESR spectra of spin probe diffusing in nonirradiated NR measured at -10 C. The probe incorporation temperatures were: (a) 4 C, (b) 24 C and (c) 37 C.&(2      "Ck V  S .A Figure2m'L08I 3@-I[P   #"2&@R2G[P   Bx*7?*FN-I[P 15.1,(bB  @  @@``   B#7??N*F[P ~24,(bB  @  @@``   Bd$7?*F7M-IN 20.9,(bB  @  @@``   BH7??7M*FN }4,(bB  @  @@``   BdB7?;97M?[P ~19,(bB  @  @@``   B\7?37M;9[P  NR 300 kGy, ( bB  @  @@``   Bf7?*FK-I7M 2.32,(bB  @  @@``   BV7??K*F7M ~24,(bB  @  @@``   By7?*FJ-IK 2.47,(bB  @  @@``   B t7??J*FK ~16,(bB  @  @@``   Bx}7?;9J?7M }0,(bB  @  @@``   B7?3J;97M  NR 200 kGy, ( bB  @  @@``   Bx7?*FH-IJ 1.15,(bB  @  @@``   B7??H*FJ ~37,(bB  @  @@``   BX7?*FF-IH 1.35,(bB  @  @@``   B@7??F*FH ~24,(bB  @  @@``   B<7?*F\E-IF 1.61,(bB  @  @@``   B7??\E*FF }4,(bB  @  @@``   B7?;9\E?J -10,(bB  @  @@``   BX7?3\E;9J NR 0 kGy, (bB  @  @@``e   N72?"`*F@-I\E In/Iwb(bjbjB&   @  @@``9   ND82?"`?@*F\E 'Temperature of probe incorporation / C.(('bB ( @  @@``m   N 82?"`;9@?\E Temperature of measurement / CL ( b"bB*   @  @@``   N482?"`3@;9\E Sample.(bB  @  @@``ZB   s *Ԕ ?3@-I@ZB   s *Ԕ ?3[P-I[PZB   s *Ԕ ?3@3[PZB   s *Ԕ ?-I@-I[PZB   s *Ԕ ?3\E-I\EZB   s *Ԕ ?;9@;9[PZB   s *Ԕ ??@?[PZB   s *Ԕ ?*F@*F[PZB   s *Ԕ ?3J-IJZB   s *1 ??F-IFZB   s *1 ??H-IHZB '  s *Ԕ ?37M-I7MZB 5  s *1 ??K-IKZB T  s *1 ??N-IN q 08=Q2FGT 5kTable 1. Intensity ratios of the narrow (In) and broad (Iw) components of ESR spectra shown in Figures 2-4.rl(2!   2  Em HL /$R2(  # "<_0&\   0@8/$R2% 2Figure 1. Typical ESR spectra of spin probe in NR:&3(2 *b 8X   0|!8"%+(H@8___PPT9  L^narrow (T > Tg) broad (T < Tg) bimodal (TH"T5mT)l0!    H       8XV  S .AFigure1tLO/"XB r 0De""XB s 0DwZ$Z$#L #& v # Ny"%R t  0Q8#6% bIw& 2   u  0X8%& bIn& 2  !  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