若干典型高分子体系的离子特异性效应
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摘要
在本论文中,我们研究不同高分子体系中的离子特异性效应,包括中性高分子聚(N-异丙基丙烯酰胺)(PNIPAM)、阴离子聚电解质聚苯乙烯磺酸钠(PSSNa)以及两性聚电解质(PSBMA)体系,主要研究内容如下：
(1)我们通过浊度法与差示扫描量热法系统研究了PNIPAM在水-甲醇混合溶剂中reentrant行为的离子特异性效应。研究结果表明SCN-与ClO4-离子能够抑制reentrant行为,而其它离子则能突显这一行为。当离子逐步从chaotrope过渡到kosmotrope, PNIPAM的最低相转变温度逐渐降低,并且其所对应的甲醇体积分数逐渐增加。阴离子特异性效应是由于阴离子影响水-甲醇络合物结构造成的。阳离子特异性效应则是其与PNIPAM链的相互作用强弱不同导致的。随着甲醇含量增加,离子特异性效应被逐渐放大。DSC结果表明不同盐溶液中PNIPAM发生相转变时的焓变基本相同,说明离子特异性效应可能为熵效应所主导。
(2)我们利用耗散测量型石英晶体微天平(QCM-D)研究了PSSNa刷在水-甲醇混合溶剂中构象行为的离子特异性效应。随着甲醇体积分数从0%增加到100%, PSSNa刷逐步塌缩,表明溶剂质量随着甲醇的加入逐渐变差。在不同的甲醇含量下,随着NaCl浓度的增加,PSSNa刷在塌缩过程中形成松散结构,并随着塌缩的继续,松散结构最终又变得较为致密均一。当加入CsCl时,除去上述的构象变化过程,PSSNa刷在高盐浓度时会呈现再溶胀的过程,且这一转变随甲醇含量增加而不断改变。当加入MgCl2时,这一塌缩再溶胀的过程随甲醇含量的增加变得更加明显。
(3)我们利用QCM-D与表面等离子体共振仪(SPR)研究了PSBMA刷构象行为的离子特异性效应。研究结果表明阴离子能够减弱链内／间吸引相互作用,使接枝链水化程度随离子强度的增加而增加。在低离子强度区,从kosmotrope到chaotrope,阴离子减弱链内／间偶极-偶极相互作用能力逐渐增强,然而在高离子强度区,阴离子序列发生反转。同时,PSBMA刷在chaotrope型阴离子存在下,在水化过程呈现不均匀的结构。SPR结果中没有观察到明显的离子特异性效应,这是因为SPR信号变化对链的水化不敏感导致的。此外,chaotrope型阴离子能促使PSBMA刷更有效地阻抗蛋白质吸附。同样,chaotrope型阴离子能够更加有效地使蛋白质分子从PSBMA刷表面解吸附。
In this thesis, we will present the investigations on the specific ion effect in different polymer systems including netural PNIPAM system, negtively charged PSSNa system, and ziwtterionic PSBMA system. The main results are as follows:
(1) We have systematically investigated the ion specific reentrant behavior of PNIPAM in water-methanol mixtures. Turbidity measurements demonstrate that SCN-and ClO4-depress the reentrant transition, whereas other anions enhance the transition. As the anion changes from chaotropic to kosmotropic, the minimum critical phase transition temperature (Tmin) decreases and the corresponding volume fraction of methanol (XM) shifts to a larger value. Our results demonstrate that anion specificity is due to the anionic structure making/breaking effect on water/methanol complexes. Cations are found to have a lesser but still significant effect on the reentrant transition and as Tmin decreases the corresponding XM also shifts to larger values as with the anions. Our studies show that cation specificity is induced by specific interactions between cations and PNIPAM chains. Furthermore, both anion and cation specificities are amplified as XM is increased due to the formation of additional water/methanol complexes. Calorimetry measurements demonstrate that the ion specificity is dominated by changes in entropy.
(2) We have studied the salt effects on the conformational behavior of PSSNa brushes in the water-methanol mixtures using a quartz crystal microbalance with dissipation (QCM-D). As the methanol fraction increases, PSSNa brushes become more collapsed, indicating that the addition of methanol leads to a poorer solvent for PSSNa chains. When NaCl is introduced, as the salt concentration increases, the extended PSSNa brushes first shrink into an inhomogeneous structure, followed by the formation of a denser and homogeneous polymer layer with the further increase of salt concentration. When CsCl is introduced, besides abovermentioned conformational change, the PSSNa chains will be recharged again at high salt concentrations accompanied by the stretching of grafted chians. PSSNa brushes in the presence of MgCl2exhibit a similar conformational change to that in the presence of CsCl, but the reentrant behavior of conformational change becomes more obvious with the methanol fraction.
(3) By use of QCM-D and surface plasmon resonance (SPR), we have systematically investigated the conformational behavior of poly(sulfobetaine methacrylate)(PSBMA) brushes as a function of ionic strength in the presence of different ions. The frequency change demonstrates that the effectiveness of anions to weaken the inter-/intrachain association and to enhance the hydration of the grafted chains increases from kosmotrope to chaotrope in the low ionic strength regime, but the ordering of anions is almost reversed at the high ionic strengths. The dissipation change indicates that some heterogeneous structures are formed inside the brushes in the presence of chaotropic anions with the increase of ionic strength. In SPR studies, the change of resonance unit (ARU) with ionic strength is determined by the balance between the increase of thickness and the decrease of refractive index of the brushes. ΔRU is insensitive to the coupled water molecules inside the brushes so that no anion specificity is observed in the SPR measurements. For the control of protein adsorption/desorption, our studies show that the brushes can more effectively resist the protein adsorption in the presence of a more chaotropic anion and a more chaotropic anion can also more effectively induce the protein desorption from the surface of the brushes.
(1)我们通过浊度法与差示扫描量热法系统研究了PNIPAM在水-甲醇混合溶剂中reentrant行为的离子特异性效应。研究结果表明SCN-与ClO4-离子能够抑制reentrant行为,而其它离子则能突显这一行为。当离子逐步从chaotrope过渡到kosmotrope, PNIPAM的最低相转变温度逐渐降低,并且其所对应的甲醇体积分数逐渐增加。阴离子特异性效应是由于阴离子影响水-甲醇络合物结构造成的。阳离子特异性效应则是其与PNIPAM链的相互作用强弱不同导致的。随着甲醇含量增加,离子特异性效应被逐渐放大。DSC结果表明不同盐溶液中PNIPAM发生相转变时的焓变基本相同,说明离子特异性效应可能为熵效应所主导。
(2)我们利用耗散测量型石英晶体微天平(QCM-D)研究了PSSNa刷在水-甲醇混合溶剂中构象行为的离子特异性效应。随着甲醇体积分数从0%增加到100%, PSSNa刷逐步塌缩,表明溶剂质量随着甲醇的加入逐渐变差。在不同的甲醇含量下,随着NaCl浓度的增加,PSSNa刷在塌缩过程中形成松散结构,并随着塌缩的继续,松散结构最终又变得较为致密均一。当加入CsCl时,除去上述的构象变化过程,PSSNa刷在高盐浓度时会呈现再溶胀的过程,且这一转变随甲醇含量增加而不断改变。当加入MgCl2时,这一塌缩再溶胀的过程随甲醇含量的增加变得更加明显。
(3)我们利用QCM-D与表面等离子体共振仪(SPR)研究了PSBMA刷构象行为的离子特异性效应。研究结果表明阴离子能够减弱链内／间吸引相互作用,使接枝链水化程度随离子强度的增加而增加。在低离子强度区,从kosmotrope到chaotrope,阴离子减弱链内／间偶极-偶极相互作用能力逐渐增强,然而在高离子强度区,阴离子序列发生反转。同时,PSBMA刷在chaotrope型阴离子存在下,在水化过程呈现不均匀的结构。SPR结果中没有观察到明显的离子特异性效应,这是因为SPR信号变化对链的水化不敏感导致的。此外,chaotrope型阴离子能促使PSBMA刷更有效地阻抗蛋白质吸附。同样,chaotrope型阴离子能够更加有效地使蛋白质分子从PSBMA刷表面解吸附。
In this thesis, we will present the investigations on the specific ion effect in different polymer systems including netural PNIPAM system, negtively charged PSSNa system, and ziwtterionic PSBMA system. The main results are as follows:
(1) We have systematically investigated the ion specific reentrant behavior of PNIPAM in water-methanol mixtures. Turbidity measurements demonstrate that SCN-and ClO4-depress the reentrant transition, whereas other anions enhance the transition. As the anion changes from chaotropic to kosmotropic, the minimum critical phase transition temperature (Tmin) decreases and the corresponding volume fraction of methanol (XM) shifts to a larger value. Our results demonstrate that anion specificity is due to the anionic structure making/breaking effect on water/methanol complexes. Cations are found to have a lesser but still significant effect on the reentrant transition and as Tmin decreases the corresponding XM also shifts to larger values as with the anions. Our studies show that cation specificity is induced by specific interactions between cations and PNIPAM chains. Furthermore, both anion and cation specificities are amplified as XM is increased due to the formation of additional water/methanol complexes. Calorimetry measurements demonstrate that the ion specificity is dominated by changes in entropy.
(2) We have studied the salt effects on the conformational behavior of PSSNa brushes in the water-methanol mixtures using a quartz crystal microbalance with dissipation (QCM-D). As the methanol fraction increases, PSSNa brushes become more collapsed, indicating that the addition of methanol leads to a poorer solvent for PSSNa chains. When NaCl is introduced, as the salt concentration increases, the extended PSSNa brushes first shrink into an inhomogeneous structure, followed by the formation of a denser and homogeneous polymer layer with the further increase of salt concentration. When CsCl is introduced, besides abovermentioned conformational change, the PSSNa chains will be recharged again at high salt concentrations accompanied by the stretching of grafted chians. PSSNa brushes in the presence of MgCl2exhibit a similar conformational change to that in the presence of CsCl, but the reentrant behavior of conformational change becomes more obvious with the methanol fraction.
(3) By use of QCM-D and surface plasmon resonance (SPR), we have systematically investigated the conformational behavior of poly(sulfobetaine methacrylate)(PSBMA) brushes as a function of ionic strength in the presence of different ions. The frequency change demonstrates that the effectiveness of anions to weaken the inter-/intrachain association and to enhance the hydration of the grafted chains increases from kosmotrope to chaotrope in the low ionic strength regime, but the ordering of anions is almost reversed at the high ionic strengths. The dissipation change indicates that some heterogeneous structures are formed inside the brushes in the presence of chaotropic anions with the increase of ionic strength. In SPR studies, the change of resonance unit (ARU) with ionic strength is determined by the balance between the increase of thickness and the decrease of refractive index of the brushes. ΔRU is insensitive to the coupled water molecules inside the brushes so that no anion specificity is observed in the SPR measurements. For the control of protein adsorption/desorption, our studies show that the brushes can more effectively resist the protein adsorption in the presence of a more chaotropic anion and a more chaotropic anion can also more effectively induce the protein desorption from the surface of the brushes.
引文
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1. Zhang, Y. J.; Cremer, P. S. Proc. Natl. Acad. Sci.2009,106,15249-15253.
2. Salis, A.; Bhattacharyya, M. S.; Monduzzi, M. J. Phys. Chem. B 2010,114,7996-8001.
3. Chen, X.; Flores, S. C.; Lim, S. M.; Zhang, Y. J.; Yang, T. L.; Kherb, J.; Cremer, P. S. Langmuir 2010,26,16447-16454.
4. Schelero, N.; Hedicke, G.; Linse, P.; Klitzing, R. V. J. Phys. Chem. B 2010,114,15523-15529.
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