Structuring of Polyelectrolyte (NaPSS) Solutions in Bulk and under Confinement as a Function of Concentration and Molecular Weight
Structuring of Polyelectrolyte (NaPSS) Solutions in Bulk and under Confinement as a Function of Concentration and Molecular Weight
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散装和封闭条件下聚电解质 (NaPSS) 溶液的结构与浓度和分子量的函数关系
DOI：
10.1021/ma201466a
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发表时间：
2011
期刊：
影响因子：
5.5
通讯作者：
R. von Klitzing
中科院分区：
文献类型：
--
作者：
C. Üzüm;S. Christau;R. von Klitzing
本论文给出了一个更深入的了解在水溶液中的聚合度和聚合物浓度的函数的几何约束下的链有序。胶体探针原子力显微镜（CP-AFM）和小角X射线散射（SAXS）被用来比较聚（苯乙烯磺酸盐）（NaPSS）链之间的两个固体界面和散装，分别。振荡力距离曲线从CP-AFM以及散射峰从SAXS表明近距离有序的结构参数，如链间距离，相关长度，和订购的强度的双链。CP-AFM（约束）和SAXS（体）的这些特征长度在相同的范围内。在约束条件下，链间距离最多小20%，相关长度最多高20%，这表明在约束条件下，双链有轻微的压缩和更强的反凝聚。聚合度N为20 ~ 155时，链间距与单体单元浓度成正比，分别表示稀态和半稀态;聚合度N为367和10690时，链间距与单体单元浓度成正比，分别表示稀态和半稀态。从稀态到半稀态的转变与粘度测量中发现的转变和理论概念吻合得很好。在固定的单体浓度下，d在稀溶液中取决于链长，而在半稀溶液中与分子量无关。实验intercoil distancedin稀制度吻合以及从线圈数密度，这是反过来基于一个理论模型的计算。讨论了计算链间距离的其他模型。有序的相关长度随着分子量的增加而增加，表明反式缩合的增加。由于熵的原因，有序化的强度随着聚合度的增加而增加。
The present paper gives a deeper insight into the chain ordering in aqueous polyelectrolyte solutions under geometrical confinement as a function of degree of polymerization and polymer concentration. Colloidal probe atomic force microscopy (CP-AFM) and small-angle X-ray scattering (SAXS) are used to compare the poly(styrenesulfonate) (NaPSS) chain ordering between two solid interfaces and in bulk, respectively. Oscillatory force–distance curves from CP-AFM as well as the scattering peaks from SAXS indicate a near range ordering of polyelectrolyte chains with structural parameters such as interchain distance, correlation length, and the strength of ordering. These characteristic lengths from CP-AFM (confinement) and SAXS (bulk) are in the same range. The interchain distance is up to 20% smaller and the correlation length is up to 20% higher under confinement, indicating a slight compression of the polyelectrolyte chains and a stronger counterion condensation under confinement. The interchain distancedscales with the monomer unit concentrationcasd∼c–1/3for a degree of polymerizationNfrom 20 to 155 and asd∼c–1/2forN= 367 and 10 690, indicating a dilute and semidilute regime, respectively. The transition from dilute to semidilute regime is in good agreement with the one found in viscosity measurements and with theoretical concepts. At a fixed monomer concentration,ddepends on the chain length in the dilute regime while it is independent of the molecular weight in the semidilute regime. The experimental intercoil distancedin the dilute regime coincides well with the one calculated from the coil number density, which is based in turn on a theoretical model. Other models for calculating the interchain distance are discussed. The correlation length of the ordering increases with increasing molecular weight, indicating an increase in counterion condensation. The strength of ordering increases with the degree of polymerization due to entropic reasons.
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