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S  N$H,, PV H n*9 . . . ]]  NXH,, P>~4V  H p*9 . . . ]]  NH,, P%9KV H p*9 . . . ]]H  0 b{% ? 3380___PPT10.gppmh Default Design> 0 @N(    0 P-   `*     0  -  b*   d  c $ ?yg    0 ( 0  RClick to edit Master text styles Second level Third level Fourth level Fifth level!    S   6, NP{   `*     64 N {  b*   H  0޽h@ ? 3380___PPT10.vF}h 0 (     0e P-   R*     0@|  -  T*     6 NP{   R*     6 N {  T*   H  0޽h@ ? 3380___PPT10.vՠ} ]U  (    TH,,DhGd >`THE INFLUENCE OF AMINO ACID SIDE CHAINS ON WATER BINDING TO THE COPPER(II) IN COPPER(II) COMPLEXES: AN EPR AND A MOLECULAR MECHANICS STUDY Krunoslav Mirosavljevi1, Jasmina Sabolovi2, Vesna Nthig-Laslo1 1Ruer Boakovi Institute 2Institute for Medical Research and Occupational Health Zagreb, Croatia1F=0 00 00 0 (( (G( 1 . . . ]]N  C &ARudjer R  C *Aimi_logo >L1  TH-[1 Z)  . . . ]]    TkL# INTRODUCTION Copper(II) complexes with amino acids and peptides are potentially good enzyme mimetics. Interactions of amino acid side chains in those complexes may have important role in their temperature dependent behaviour. The EPR studies of the Brownian motion of bis(N,N-dimethyl-L-a-valinato)copper(II) (Cu(Me2Val)2) and bis(N,N-dimethyl-L-a-leucinato)copper(II) (Cu(Me2Leu)2) dissolved in different solvents (deuterated methanol, ~280-320 K, and deuterated chloroform, ~ 265-305 K) were combined with molecular mechanics calculations. The conformational analysis of these compounds was performed in order to find the most stable conformations. The aim of this work was to find whether different EPR behaviour of these two copper(II) complexes could be connected with the conformational (sterical) reasons. Bis(N,N-dimethyl-L-a-alaninato)copper(II) (Cu(Me2Ala)2) was used as reference complex. There are no interactions of alanine side chains because  CH3 is small group and the apical water molecule must be present for the stability of the complex. The effective volume of the complex is constant in temperature interval examined. f 0(( ($((( (( ( (( ($((( (( (8("({(( ($((( (( (]( ((    F   '  (  ( L   . ;. . ]]^  6'O'z  <"$@*V  JThe EPR spectra of Cu(Me2Leu)2 both in CDCl3 and CD3OD suggest aqua-complex (D2O in coordination sphere of copper) in whole temperature interval examined. In each solvent the spectra were simulated with the same parameters (A0 and g0). The conformational analysis backs EPR results: the energy difference between the most stable conformer and first above it increases for aqua-complex. It means that the presence of the water molecule additionally stabilizes complex. Cu(Me2Val)2 in CD3OD shows more complicated dependence of tQ to h/T. Since it is not linear (i.e. the volume of the complex changes in temperature interval examined), there are some conformational changes. The energy difference between the most stable conformer and first above it is smaller when water molecule is present which allows us to suggest some rearrangements of amino acid side chains and perhaps releasing of apical ligand (water) during the heating.l( (( ( ( (( (( ((( ((( (( (( (( (((((((((((&   .   <dm#N% fTHEORY AND RESULTS0  . ^ 3 6F&OF&p 6 NUUy, )/ 6B(mI) = a + bmI + cmI2 F0#0#0#0#0+0#0#0#0#0#0#0+0+0#0#0#0#0+0+0B4      &&&99LL 8 HUUs&9(, Because of the incomplete averaging of interaction between magnetic moments of an electron and a nuclear spin, line widths in EPR spectra, DB, depend on nuclear magnetic moment, mI . It provides that line widths obtained in EPR spectra can be expressed:0B((B((b(B($B( b ( j ( * ( " (G(&  J &&&99LLx 9 <A "??+8).< " : H!U!U(5J)`8 Reorientation correlation time,tQ, depends on viscosity to temperature ratio,h/T, according to Stokes-Einstein relation:y0(B(((b(B((B(  ( b ( b (' " (B(J( y &&&99LLx ; <A #??%2$4 # < H@&U&U|/)'41 VParameter b is varied by temperature and it is connected with tQ:B0(2 B(B( (B(((B(J( B &&&99LL ? HUU2]/c4 f 0(B(  &&&99LLx C <A ??%;AMN=  D BPO=V? lDISCUSION AND CONCLUSION0  . [  (&;%8   #":. p& (;%8   <( ?"`94;Y6 3.05 0.018 (b"  @  @@``    < ?"`649Y6 18.50 0.018 (b"  @  @@``   <L ?"`9446Y6 8.20 0.018 (b"  @  @@``"   < ?"`1494Y6 2.072 0.0018 (b"  @  @@``"   <d ?"`q/41Y6 2.244 0.0018 (b"  @  @@``"   <( ?"`-4q/Y6 2.129 0.0018 (b"  @  @@``5   <h ?"` (4-Y6 CD3OD 280-295 KT(bjb" "  @  @@``   <?99(;) VB  . ]   <?69(9) VB  . ]   <?949(6) VB  . ]   <)?19(94) VB  . ]   <8?q/9(1) VB  . ]   <??-9(q/) VB  . ]#   <K? (9(-)  Cu(Me2Ala)2T (bjbj  @  @@``   <`D?9);+ ~1.95 0.01$   . ]   <_?6)9+ 18.27 0.01$   . ]   <i?94)6+ ~7.39 0.01$   . ]   <s?1)94+ 2.055 0.001$   . ]   <m?q/)1+ 2.241 0.001.   . ]    <܉?-)q/+ 2.117 0.001:   . ]   <x? ()-+ CD3OD<(BJB  @  @@``  <(?9Y6;%8 3.35 0.01* ("  @  @@``  <ܨ?6Y69%8 18.50 0.018 (b"  @  @@``*  <?94Y66%8 8.40 0.01R (b"b"  @  @@``  <P?1Y694%8 2.067 0.0018 (b"  @  @@``  <$?q/Y61%8 2.244 0.0018 (b"  @  @@``  <?-Y6q/%8 2.126 0.001( (  @  @@``6  <h? (Y6-%8 CD3OD 295 -317 Kb(bjb" "B  @  @@``  <D?92;4 5.23 0.018 (b"  @  @@``  <l?6294 17.90 0.018 (b"  @  @@``  <?94264 9.45 0.018 (b"  @  @@``  <?12944 2.050 0.0018 (b"  @  @@``  <?q/214 2.251 0.0018 (b"  @  @@``  <"?-2q/4 2.117 0.0018 (b"  @  @@``  <,? (2-4 CDCl3<(bjB  @  @@``  <4?91;2 VB  . ]  < >?6192 VB  . ]  <pF?94162 VB  . ]  <O?11942 VB  . ]  <W?q/112 VB  . ]  <`?-1q/2 VB  . ]1  <b? (1-2  Cu(Me2Val)2b (bjbjB  @  @@``  <tw?9O/;1 2.80 0.018 (b"  @  @@``  <?6O/91 17.80 0.018 (b"  @  @@``  <?94O/61 7.80 0.018 (b"  @  @@``  <?1O/941 2.078 0.0018 (b"  @  @@``  <0?q/O/11 2.244 0.0018 (b"  @  @@``  <?-O/q/1 2.133 0.0018 (b"  @  @@``  <X? (O/-1 CD3ODJ(bjbB  @  @@``  <(?9]-;O/ 5.15 0.010 B  . ]  <?6]-9O/ 17.90 0.010 B  . ]  <?94]-6O/ 9.40 0.010 B  . ]  <?1]-94O/ 2.053 0.0010 B  . ]  < ?q/]-1O/ 2.243 0.0010 B  . ]  <?-]-q/O/ 2.116 0.0010 B  . ]  <? (]--O/ CDCl3<(bjB  @  @@``  <?9+;]- VB  . ]  <?6+9]- VB  . ]  <D?94+6]- VB  . ]  <%?1+94]- VB  . ]  <.?q/+1]- VB  . ]  <0?-+q/]- VB  . ]1 ~ <lD? (+-]-  Cu(Me2Leu)2b (bjbjB  @  @@``> } <O?9&;9(  A^/mTV(bb&   @  @@``@ | <h[?6&99(  A||/mTV(bb&   @  @@``> { <Lg?94&69(  A0/mTV(bb&   @  @@`` z <|p?1&949( g^4(b  @  @@`` y <y?q/&19( g||4(b  @  @@`` x <?-&q/9( g04(b  @  @@`` w <$? (&-9( VB  . ]ZB  s *1 ? (&;&ZB  s *1 ? (%8;%8ZB  s *1 ? (& (9(ZB  s *1 ?;&;9(TB  c $1 ? (9(;9(ZB  s *1 ?-&-9(ZB  s *1 ?q/&q/9(ZB  s *1 ?1&19(ZB  s *1 ?94&949(ZB  s *1 ?6&69(ZB  s *1 ?9&99(NB  S  ?;9(;)ZB  s *1 ? (]--]-TB  c $ ?-]-;]-ZB  s *1 ? (O/;O/TB  c $1 ? (1;1NB   S  ? (2;2ZB A  s *1 ? (4-4TB a  c $ ?-4;4TB   c $1 ? (+-+NB   S  ?-+;+TB   c $1 ? ()-)NB   S  ?-);)ZB   s *1 ? (Y6;Y6TB K  c $1 ? (9( ()ZB L  s *1 ? () (+ZB N  s *1 ?-)-+TB Q  c $ ?q/)q/+TB S  c $ ?1)1+TB U  c $ ?94)94+TB W  c $ ?6)6+TB X  c $ ?9)9+TB Y  c $ ?;);+TB l  c $1 ? (+ (]-ZB m  s *1 ? (]- (1ZB n  s *1 ?-]--1TB p  c $ ?q/]-q/1TB r  c $ ?1]-11TB t  c $ ?94]-941TB v  c $ ?6]-61TB x  c $ ?9]-91NB z  S  ?;+;]-TB {  c $ ?;]-;1TB ~  c $1 ? (1 (2ZB   s *1 ? (2 (%8ZB   s *1 ?-2-%8TB   c $ ?q/2q/%8TB   c $ ?121%8TB   c $ ?94294%8TB   c $ ?626%8TB   c $ ?929%8NB   S  ?;1;2TB   c $ ?;2;%8N  < i9(:: hTable 1. EPR parameters used for calculations of tQ.<51 5 . x A  <A ??>,*:W h C @.8AA12w4-3o?%@uJH D <|I_>,MzK (Figure 4. 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