强韧化聚合物网络的结构设计策略★

doi:10.6023/A25050157

化学学报 ›› 2025, Vol. 83 ›› Issue (9): 1103-1118.DOI: 10.6023/A25050157 上一篇

综述

强韧化聚合物网络的结构设计策略^★

王源浩, 张照明^*(), 颜徐州^*()

化学生物协同物质创制全国重点实验室上海交通大学化学化工学院教育部变革性分子前沿科学中心上海 200240

投稿日期:2025-05-11 发布日期:2025-07-07

作者简介:

王源浩, 博士生, 就读于上海交通大学化学化工学院, 主要研究方向为机械互锁聚合物的制备和构效关系研究.

张照明, 2019年在日本北海道大学获得博士学位, 随后加入上海交通大学, 先后担任博士后、助理研究员及副研究员等职. 研究领域聚焦超分子聚合物、机械互锁聚合物及智能高分子材料的开发与应用. 以(共同)第一或通讯作者发表J. Am. Chem. Soc.、Nat. Commun.、Angew. Chem. Int. Ed.、Acc. Chem. Res.等学术论文34篇, 论文引用1600余次. 主持国家自然科学基金面上项目、青年项目在内的5项科研项目.

颜徐州, 上海交通大学化学化工学院研究员, 博士生导师. 2014年获得浙江大学博士学位, 2014~2018年分别在美国犹他大学和斯坦福大学从事博士后研究, 2018年9月入职上海交通大学开展独立研究工作. 入选上海市高校特聘教授(东方学者, 2018)和曙光学者(2022)计划, 2021年获得国家自然科学基金优秀青年科学基金资助. 主要研究方向为机械互锁聚合物和动态高分子材料.

^★ “中国青年化学家”专辑.

基金资助:
国家自然科学基金(22471164); 国家自然科学基金(22475128); 国家自然科学基金(52421006); 聚烯烃催化技术与高性能材料全国重点实验室、上海市聚烯烃催化技术重点实验室资助(SKL-LCTP-202301)

Strategies for Structural Design in Strengthening and Toughening Polymer Networks^★

Yuanhao Wang, Zhaoming Zhang^*(), Xuzhou Yan^*()

State Key Laboratory of Synergistic Chem-Bio Synthesis, School of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules, Shanghai Jiao Tong University, Shanghai 200240, China

Received:2025-05-11 Published:2025-07-07
Contact: * E-mail: zhangzhaoming@sjtu.edu.cn;xzyan@sjtu.edu.cn
About author:
^★ For the VSI “Rising Stars in Chemistry”.
Supported by:
National Natural Science Foundation of China(22471164); National Natural Science Foundation of China(22475128); National Natural Science Foundation of China(52421006); State Key Laboratory of Polyolefins and Catalysis and Shanghai Key Laboratory of Catalysis Technology for Polyolefins(SKL-LCTP-202301)

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摘要/Abstract

聚合物材料在现代工业和科技领域占据重要地位, 但传统工业的聚合物改性方法往往面临着强度和韧性调节不可控制的难题, 限制了材料的高端应用. 为解决这一问题, 研究者们通过聚合物的结构优化以实现宏观性能的调控. 因此, 本综述以网络结构设计为切入点, 根据能量耗散途径的不同, 将聚合物改性的机制分为氢键作用、配位作用、主客体作用、力敏基团、机械互锁结构和其他作用六个方面. 随后, 分类综述了各个方面近年来具有代表性和创新性的工作, 通过结构分析和性能理解, 重点阐释了不同作用对于增强增韧聚合物材料的影响机制. 最后, 根据现有的研究内容, 指出了未来聚合物材料机械性能提升所面临的关键问题和重要挑战.

关键词: 动态高分子材料, 机械自适应性, 非共价相互作用, 机械互锁结构, 能量耗散

Polymer materials play a crucial role in modern industry and technology due to their versatile properties and broad range of applications. However, conventional industrial modification strategies often suffer from an inherent inability to finely tune the balance between strength and toughness, thereby constraining their utility in high-performance applications. To address this challenge, researchers have focused on optimizing the internal structure of polymers as a means to regulate their macroscopic mechanical behavior. Among various strategies, network structure design has emerged as a particularly effective approach. This review takes network structure as a central theme and categorizes the mechanisms of polymer modification based on their energy dissipation pathways. Six major mechanisms are discussed: hydrogen bonding, coordination interactions, host-guest interactions, force-sensitive groups, mechanically interlocked structures, and other reinforcing effects. For each category, we provide overview of recent representative and innovative studies. Through detailed structural analysis and performance evaluation, we highlight how different pathways contribute to the enhancement of mechanical properties. These special structures markedly enhance the material's ability to dissipate energy upon external force. This improvement arises primarily through three synergistic pathways: (1) the reversible breaking and reformation of sacrificial bonds, which serve to absorb and redistribute applied stress; (2) energy dissipation via molecular mobility and chain segmental friction; and (3) multiscale mechanisms of stress transfer and dispersion, which effectively mitigate stress concentration and delay failure. Finally, based on the current research, we identify key unresolved questions and major challenges that must be addressed to further advance the mechanical performance of polymer materials. Looking ahead, the development of next-generation high-performance polymers is expected to converge on several critical directions: achieving sustainability in material sourcing and processing, the combination of high elasticity and high toughness, reducing economic costs, and deepening the multiscale understanding of structure-property relationships. These avenues will be pivotal in guiding the rational design of polymer systems for future technological demands.

Key words: dynamic polymer materials, mechanical adaptability, non-covalent interaction, mechanically interlocked structure, energy dissipation

引用此文

王源浩, 张照明, 颜徐州. 强韧化聚合物网络的结构设计策略^★[J]. 化学学报, 2025, 83(9): 1103-1118.

Yuanhao Wang, Zhaoming Zhang, Xuzhou Yan. Strategies for Structural Design in Strengthening and Toughening Polymer Networks^★[J]. Acta Chimica Sinica, 2025, 83(9): 1103-1118.

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图/表 14

图1. (a) IPDI-SPU和TDI-SPU的结构式; (b) IPDI-SPU和TDI-SPU的应力-应变曲线; (c) IPDI-SPU2000弹性体条(25 mg)可以举起5.0 kg的重量[50]

Figure 1. (a) Chemical structures of IPDI-SPU and TDI-SPU elastomers. (b) Stress-strain curves of IPDI-SPU and TDI-SPU elastomers. (c) Photographs showing that the IPDI-SPU2000 elastomer strip (25 mg) can lift a weight of 5.0 kg[50]

图2. (a)八重氢键[51]和(b)十二重氢键的结构示意式[52]

Figure 2. Schematic of (a) octuple hydrogen bonding[51] and (b) duodecuple hydrogen bonding[52]

图3. (a)甲硅烷保护基的裂解和随后铁络合物形成的过程, 以及在此过程中试样膨胀的展示; (b, c)铁离子处理前后的网络结构示意图; (d)不同网络的应力-应变曲线[62]. (e)聚合物主链的结构式与不同离子配位后的网络结构; (f)不同网络的应力-应变曲线; (g)不同网络的杨氏模量和韧性值[63]

Figure 3. (a) A scheme of the cleavage of the silyl protective groups and subsequent iron complex formation, and a depiction of the swelling of a test specimen during the process. Schematics of the network structure (b) before and (c) after iron treatment. (d) Stress-strain curves of different networks[62]. (e) Schematics of the polymer backbone and network structures after coordination of different ions. (f) Stress-strain curves, (g) Young's modulus and toughness values of different networks[63]

图4. (a) PBP的化学结构和示意图及通过B—N配位键形成的B—N配位超分子聚合物(BNP)的示意图; (b)通过B—O和B—N键形成超分子交联聚合物; 不同网络的(c)应力-应变曲线, (d)杨氏模量和韧性数值以及(e)其他机械性能的对比[66]

Figure 4. (a) Chemical structure and cartoon representation of PBP and the dative B—N supramolecular polymer (BNP) via dative B—N bonds. (b) Cartoon representation of the formation of the supramolecular polymer cross-linked vitrimer via dynamic B—O and B—N dative bonds. Comparison of (c) stress-strain curves, (d) Young's modulus and toughness values, (e) and other mechanical properties of different networks[66]

图5. CD基超分子水凝胶的机械性能受CD和聚合物侧链上客体分子的影响: (a)电势垒, (b) CD腔尺寸, (c)客体单元长度, (d)电荷数和(e)还原响应性[73]

Figure 5. Mechanical properties of the CD-based supramolecular hydrogels affected by CDs and guest molecule on polymer side chain: (a) electric barrier, (b) CD cavity size, (c) length of guest unit, (d) charge number, and (e) reduction responsiveness[73]

图6. (a)冠醚主体聚合物链、二级铵盐客体交联剂和超分子网络的示意图; (b)不同交联密度超分子网络的应力-应变曲线[74]; (c)穴醚主体聚合物链、百草枯客体交联剂和超分子网络的示意图; (d)不同聚合物网络的应力-应变曲线[76]

Figure 6. (a) Chemical structures and schematic representations of crown ether-decorated polymer chain, secondary ammonium salts cross-linker and supramolecular network (SPN). (b) Stress-strain curves of SPNs with different cross-linking densities[74]. (c) Chemical structures and schematic representations of cryptand-decorated polymer chain, bisparaquat cross-linker and SPN. (d) Stress-strain curves of different polymer networks[76]

图7. (a)聚合反应所需的分子; (b)力敏基团和普通共价键的结构式; (c)构筑网络的不同方式; (d)力敏基团构筑的网络和(e)普通共价键构筑的网络在外力作用下的断裂示意[80]

Figure 7. (a) Molecules required for the polymerization reaction. (b) Structural formulas of force-sensitive group and normal covalent bonds. (c) Different ways of constructing the network. (d) Schematic representation of the fracture of the network constructed by force-sensitive groups and (e) normal covalent bonds upon external force[80]

图8. (a)初始网络示意图; (b)力敏基团在超声作用下的结构变化; (c)力诱导的网络交联示意图; (d)不同超声处理持续时间后样品的应力-应变曲线; (e)超声前后聚合物的紫外-可见光谱; (f)不同超声处理持续时间后样品的储能模量变化[82]

Figure 8. (a) Schematic representation of the initial network. (b) Structural changes of force-sensitive groups under sonicating. (c) Schematic representation of cross-linking behavior induced by force. (d) Stress-strain curves of the samples with different sonicating durations. (e) Ultraviolet-visible spectroscopy of the polymer with and without sonicating. (f) Storage modulus changes of the samples after different sonicating durations[82]

图9. (a)轮烷交联剂和丁苯橡胶(SBR)的化学结构及相应示意图; (b)机械互锁网络(MINs)的示意图; (c)机械互锁交联点在外力作用下的运动行为; SBR、机械互锁网络MIN和对照样品control的(d)应力−应变曲线、(e)杨氏模量和韧性值[99]

Figure 9. (a) Chemical structures and corresponding schematic representations of rotaxane cross-linker and styrene-butadiene rubber (SBR). (b) Schematic illustration of the formation of mechanically interlocked networks (MINs). (c) Molecular motion of mechanically interlocked cross-links upon external force. (d) Stress-strain curves, (e) Young’s modulus and toughness of SBR, MIN and control[99]

图10. (a)由CDs组成的可移动交联点交联的滑环凝胶. PEG的紧密堆积结构在拉伸和释放过程中形成和破坏; (b)不同聚合物网络的应力-应变曲线[101]

Figure 10. (a) Slide-ring (SR) gel with movable cross-links composed of CDs. The close-packed structure of PEG is formed and destroyed during stretching and releasing. (b) Stress-strain curves of different polymer networks[101]

图11. (a)冠醚基聚合物主链、金属环交联剂的化学结构和示意图; (b)分子项链交联形成的机械互锁网络示意图; (c)不同交联密度的聚合物网络的应力-应变曲线[105]

Figure 11. (a) Chemical structure and corresponding cartoon of crown ether-based polymer and metallacycle cross-linker. (b) Mechanically interlocked networks (MINs) cross-linked by molecular necklace. (c) Stress-strain curves of polymer networks with different cross-linking densities[105]

图12. (a)机械混合后硫化的天然橡胶(MNR)和乳液混合后硫化的天然橡胶(LNR)的网络示意图; 不同橡胶的(b)应力-应变曲线和(c)机械性能对比[116]

Figure 12. (a) Schematic illustration of the network of mechanical mixed vulcanized NR (MNR) and latex mixed vulcanized NR (LNR). (b) Stress-strain curves and (c) mechanical properties of different rubber[116]

图13. (a)通过硬−软−硬立体三嵌段共聚物it-MRxM (x=m/n)与st-PMMA的物理交联增韧TPE立体复合物; (b, c) [it-PRMA]/[it-PMMA]=4或6的立体络合全甲基丙烯酸弹性体的应力-应变曲线[117]

Figure 13. (a) Toughened TPE stereocomplex via physical cross-linking in a hard-soft-hard stereo-triblock co-polymer, it-MRxM (x=m/n), with st-PMMA. (b, c) Stress-strain curves of stereocomplexed all-methacrylic elastomers with [it-PRMA]/[it-PMMA]=4 or 6[117]

图14. (a)前体结构式和网络的形成; (b)固化后网络的示意图; (c)聚合物材料的应力-应变曲线[118]

Figure 14. (a) Chemical structure of precursors and network formation. (b) Schematic illustration of the cured network. (c) Stress-strain curve of polymer material[118]

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强韧化聚合物网络的结构设计策略^★

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强韧化聚合物网络的结构设计策略^★

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