Radial Profile of Counterion Concentration of a Single Polyelectrolyte

Shuang-jiang Luo; Pei-yuan Gao; Hong-xia Guo; Jing-fa Yang; Jiang Zhao

doi:10.11777/j.issn1000-3304.2017.17065

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Radial Profile of Counterion Concentration of a Single Polyelectrolyte

Research Article | 更新时间：2021-01-27

- Radial Profile of Counterion Concentration of a Single Polyelectrolyte
  增强出版
- Acta Polymerica Sinica Issue 9, Pages: 1479-1487(2017)
- 作者机构：
  
  中国科学院化学研究所北京 100190
- 作者简介：
- 基金信息：
- DOI：10.11777/j.issn1000-3304.2017.17065
  CLC：
- Published：2017-9，
  
  Received：30 March 2017，
  
  Revised：2 May 2017，
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Shuang-jiang Luo, Pei-yuan Gao, Hong-xia Guo, Jing-fa Yang, Jiang Zhao. Radial Profile of Counterion Concentration of a Single Polyelectrolyte. [J]. Acta Polymerica Sinica (9):1479-1487(2017)
DOI：

Shuang-jiang Luo, Pei-yuan Gao, Hong-xia Guo, Jing-fa Yang, Jiang Zhao. Radial Profile of Counterion Concentration of a Single Polyelectrolyte. [J]. Acta Polymerica Sinica (9):1479-1487(2017) DOI： 10.11777/j.issn1000-3304.2017.17065.

摘要

采用单分子荧光显微统计光谱技术，通过将pH响应型荧光探针分子精确标记于聚苯乙烯磺酸钠分子链末端，并通过不同长度的多肽链调节分子链与探针分子间的距离，有效测量了聚苯乙烯磺酸钠单分子链的抗衡离子浓度的空间分布.实验结果清晰展示了聚电解质分子链的抗衡离子云结构，并确定了抗衡离子浓度随着距离分子链末端长度的不同而发生变化的规律，为描述聚电解质抗衡离子浓度的径向分布特征提供了实验信息.

Abstract

The distribution of counterions around the charged chain of polyelectrolyte is the key aspect of its physical and chemical properties. In the current study

the spatial profile of counterion concentration along the radial direction of the molecular chain of sodium polystyrene sulfonate (NaPSS) is investigated by single molecule fluorescence technique

fluorescence correlation spectroscopy (FCS) and photon counting histogram (PCH) technique. FCS measures the diffusion coefficient (therefore the hydrodynamic radius) of a single PSS

chain while PCH measures the molecular brightness of a single fluorophore attached to the chain end. By chemical reactions

a pH responsive fluorophore (Oregon Green 488

OG488) is precisely positioned at different distances to the end of PSS

chain

using hydrophilic polypeptide chains of different length as spacers. The concentration distribution of hydronium ions at the vicinity of the PSS

chain is measured by examining the molecular brightness of OG488

by numerical fitting the PCH data using super-Poisson distribution function. The results demonstrate that the concentration of hydronium in the vicinity of the PSS

chain is 2-3 orders of magnitude higher than that in the bulk solution (at the infinite distance to the chain)

evidencing the existence of counterion cloud around the charged chain. By varying the position of the probe with the adjustment of chain length of polypeptide

the local pH value at different distances to the PSS

chain end is measured and therefore the spatial profile of counterion concentration around the direction towards away from the chain is probed. The results show that the counterion concentration decreases very sharply with the increase of the distance (within 2.0 nm) to the PSS

chain. It is further discovered that the concentration gradient decreases with the increase of the bulk pH

demonstrating the expansion of the counterion cloud as the result of the entropy effect by dilution of hydronium ions. The results clearly prove that the counterions distribution around a charged macromolecule is the result of balance of electrostatic attraction and the process of entropy maximization

. the process of counterion adsorption

instead of the conventional counterion condensation.

关键词

聚电解质抗衡离子单分子荧光

Keywords

PolyelectrolyteCounterionsSingle molecule fluorescence

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Key Laboratory of Advanced Technologies of Materials, Ministry of Education, Southwest Jiaotong University

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Jiangxi Provincial Key Laboratory of New Energy Chemistry/Institute of Polymers, Nanchang University

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