强熵效应与大分子体系的熵调控

戴晓彬; 张轩钰; 高丽娟; 燕立唐

doi:10.11777/j.issn1000-3304.2021.21044

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强熵效应与大分子体系的熵调控

专论 | 更新时间：2023-05-22

- 强熵效应与大分子体系的熵调控
- Superentropy Effect and Macromolecular Entropy Control Strategy
- 高分子学报 2021年52卷第9期页码：1076-1099
- 作者机构：
  
  清华大学化学工程系北京 100084
- 作者简介：
  
  E-mail: ltyan@mail.tsinghua.edu.cn
- 基金信息：
  
  国家自然科学基金(基金号 ┣22025302);21873053┫
- DOI：10.11777/j.issn1000-3304.2021.21044
  中图分类号：
- 纸质出版日期：2021-09-20，
  
  网络出版日期：2021-06-24，
  
  收稿日期：2021-02-08，
  
  修回日期：2021-03-02，
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戴晓彬,张轩钰,高丽娟等.强熵效应与大分子体系的熵调控[J].高分子学报,2021,52(09):1076-1099.

Dai Xiao-bin,Zhang Xuan-yu,Gao Li-juan,et al.Superentropy Effect and Macromolecular Entropy Control Strategy[J].ACTA POLYMERICA SINICA,2021,52(09):1076-1099.
戴晓彬,张轩钰,高丽娟等.强熵效应与大分子体系的熵调控[J].高分子学报,2021,52(09):1076-1099. DOI： 10.11777/j.issn1000-3304.2021.21044.

Dai Xiao-bin,Zhang Xuan-yu,Gao Li-juan,et al.Superentropy Effect and Macromolecular Entropy Control Strategy[J].ACTA POLYMERICA SINICA,2021,52(09):1076-1099. DOI： 10.11777/j.issn1000-3304.2021.21044.

摘要

在大分子体系中，以链的构象熵为主的熵效应对体系的微观结构和宏观性能都起着至关重要的作用. 然而，熵的统计本质使其远不像焓作用那么直观，甚至会导致反直觉的现象出现. 因此，探寻大分子体系中的熵效应，对于深入揭示此类体系纷繁复杂现象背后物理机制的重要性来说是不言而喻的，已成为高分子与软凝聚态物理学以及生命科学等多学科相交叉的重要前沿研究领域. 如何在阐释熵效应的独特作用规律基础上，有效地调控熵以实现对体系微观结构的熵调控进而发展新型功能体系，是该领域一个亟需解决的重要科学问题. 本文总结了我们在提出并发展熵调控策略方面的研究进展. 首先，剖析了熵效应的一些基本作用规律，涵盖熵致有序和熵力等，并进一步提出了强熵效应的概念. 其次，阐述了熵调控策略的必要性、基本原理以及调控途径. 同时，举例介绍了熵调控策略在大分子体系中的应用，涵盖高分子纳米复合体系、凝胶网络、生命大分子体系以及大分子胶体体系等. 最后，简明扼要地展望了该领域的未来发展趋势以及面临的关键问题，以期为其以后的发展提供些许有益的启迪.

Abstract

Entropy

one of the elementary parameters in thermodynamics

is a central concept in statistical mechanics. In macromolecular systems

entropic effects

predominantly from the conformational entropy of a chain

play an essential role in both microstructural organization and macroscopic properties. In striking contrast to enthalpic interactions

entropic effects seem to be elusive and even lead to counterintuitive performance due to the statistical nature of entropy. Thus

exploring the entropic effects in macromolecular systems is of significant importance in elucidating the physical origin behind many complex phenomena

and has become one of the most important directions in the interdisciplinary fields covering polymer physics and soft matter physics. One particular aspect lies in how to manipulate entropic effects to tune the structural organization and thereby develop new functional systems

based on a fundamental understanding of the rules governing the ectopic effects. Here

we summarize our recent progress in proposing and developing entropic strategy in the structural control of macromolecular systems. Firstly

we elucidate the unique rules of the entropic effects

including entropic ordering and entropic forces

and propose the concept of superentropic effect. The significance

principles

and approaches regarding the entropic strategy are then described. Some applications of entropic strategy in various macromolecular systems

such as polymer nanocomposites

polymer gel networks

and biological macromolecules

are also presented. We finally seek to discuss future directions and identify open problems regarding the future progress of the entropic strategy. We hope that this article will promote further efforts toward fundamental research and the wide applications of entropic strategy in elucidating physical mechanisms

developing new types of functional materials

and beyond.

关键词

熵调控强熵效应高分子链构象统计熵力软凝聚态物理

Keywords

Entropic strategySuperentropic effectConformation statistics of polymer chainEntropic forceSoft matter physics

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Xu Z, Zhu G, Chen P, Dai X, Yan L T. Nanoscale, 2019, 11(46): 22305-22315. doi:10.1039/c9nr07337jhttp://dx.doi.org/10.1039/c9nr07337j

Xu Z, Yang Y, Zhu G, Chen P, Huang Z, Dai X, Hou C, Yan L T. Adv Theo Simul, 2019, 2(2): 1800160. doi:10.1002/adts.201800160http://dx.doi.org/10.1002/adts.201800160

Hou X S, Zhu G L, Ren L J, Huang Z H, Zhang R B, Ungar G, Yan L T, Wang W. J Am Chem Soc, 2018, 140(5): 1805-1811. doi:10.1021/jacs.7b11324http://dx.doi.org/10.1021/jacs.7b11324

Huang Z, Zhu G, Chen P, Hou C, Yan L T. Phys Rev Lett, 2019, 122(19): 198002. doi:10.1103/physrevlett.122.198002http://dx.doi.org/10.1103/physrevlett.122.198002

Ma C, Wu H, Huang Z H, Guo R H, Hu M B, Kübel C, Yan L T, Wang W. Angew Chem Int Ed, 2015, 54(52): 15699-15704. doi:10.1002/anie.201507237http://dx.doi.org/10.1002/anie.201507237

Huang Zihan(黄子涵), Dong Bojun(董伯骏), Chen Pengyu(陈鹏宇), Yang Ye(杨烨), Zhu Guolong(朱国龙), Yan Litang(燕立唐). Acta Polymerica Sinica(高分子学报), 2016, (8): 979-991. doi:10.11777/j.issn1000-3304.2016.16055http://dx.doi.org/10.11777/j.issn1000-3304.2016.16055

Guo R, Liu Z, Xie X M, Yan L T. J Phys Chem Lett, 2013, 4(8): 1221-1226. doi:10.1021/jz4003789http://dx.doi.org/10.1021/jz4003789

Chen P, Xu Z, Zhu G, Dai X, Yan L T. Phys Rev Lett, 2020, 124(19): 198102. doi:10.1103/physrevlett.124.198102http://dx.doi.org/10.1103/physrevlett.124.198102

Rezvantalab H, Beltran-Villegas D J, Larson R G. Phys Rev Lett, 2016, 117(12): 128001. doi:10.1103/physrevlett.117.128001http://dx.doi.org/10.1103/physrevlett.117.128001

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