冰模板技术仿生构筑层状高分子纳米复合材料的研究进展★

doi:10.6023/A23050207

化学学报 ›› 2023, Vol. 81 ›› Issue (9): 1231-1239.DOI: 10.6023/A23050207 上一篇下一篇

所属专题：庆祝《化学学报》创刊90周年合辑

综述

冰模板技术仿生构筑层状高分子纳米复合材料的研究进展^★

王华高^a, 程群峰^a^,^b^,^c^,^*()

a 北京航空航天大学化学学院仿生智能界面科学与技术教育部重点实验室北京 100191
b 中国科学技术大学化学与材料学院合肥 230026
c 中国科学技术大学苏州高等研究院苏州 215123

投稿日期:2023-05-05 发布日期:2023-06-27

作者简介:

王华高, 北京航空航天大学材料物理与化学专业在读博士研究生, 主要从事仿生层状高分子纳米复合材料研究.

程群峰, 北京航空航天大学化学学院, 教授, 博士生导师, 国家杰出青年科学基金获得者. 主要从事高分子纳米复合材料的研究工作, 发现了二维碳纳米复合材料“孔隙缺陷”的新现象, 发展了一系列消除孔隙缺陷的新技术和新策略, 创制了兼具高力学、电学和电磁屏蔽性能的碳纳米复合材料, 为碳纳米复合材料在航空航天领域的应用奠定了理论基础. 获北京市科学技术奖-杰出青年中关村奖、茅以升科学技术奖-北京青年科技奖、中国化学会青年化学奖等. 担任中国复合材料学会纳米复合材料分会常务副主任以及Chin. Chem. Lett., Biomater. Adv., Giant, 2D Materials等期刊编委; Interdiscip. Mater.学术编辑. 以通讯作者在Science, Nat. Mater., Nat. Commun., PNAS等期刊发表论文100余篇, 引用8000余次, H因子51, 授权中国发明专利35项.

^★庆祝《化学学报》创刊90周年.

基金资助:
国家重点研发计划(2021YFA0715700); 国家杰出青年科学基金(52125302); 国家自然科学基金(22075009); 111引智计划(B14009)

Recent Advances in the Nacre-inspired Layered Polymer Nanocomposites by Ice Templating Technique^★

Huagao Wang^a, Qunfeng Cheng^a^,^b^,^c()

a Key Laboratory of Bio-inspired Smart Interfacial Science and Technology of Ministry of Education, School of Chemistry, Beihang University, Beijing 100191
b School of Chemistry and Materials Science, University of Science and Technology of China, Hefei 230026
c Suzhou Institute for Advanced Research, University of Science and Technology of China, Suzhou 215123

Received:2023-05-05 Published:2023-06-27
Contact: *E-mail: cheng@buaa.edu.cn
About author:
^★Dedicated to the 90th anniversary of Acta Chimica Sinica.
Supported by:
The National Key Research and Development Program of China(2021YFA0715700); The National Science Fund for Distinguished Young Scholars(52125302); The National Natural Science Foundation of China(22075009); The 111 Project(B14009)

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摘要/Abstract

冰模板技术也称为定向冷冻铸造技术, 是指将基本组装单元、溶剂和添加剂均匀分散或溶解, 利用溶剂的“液-固-气”的相转变构筑层状多孔材料的新颖技术. 受贝壳珍珠层“砖-泥”层状结构的启发, 通过对层状骨架密实化处理, 可构筑仿贝壳珍珠层复合材料. 对冰模板技术构筑的层状高分子纳米复合材料的前沿进展进行了系统的归纳和总结. 首先, 根据冰模板技术构筑不同厚度“砖”致密化策略进行分类, 分为骨架填充高分子、骨架热压处理和骨架矿化三种策略, 通过实例解读每种策略构筑的典型层状高分子纳米复合材料及其性能. 随后, 对冰模板技术构筑的层状高分子纳米复合材料的设计与功能特性进行了分析和讨论, 如调控微观结构、引入功能基元材料和提高界面相互作用等, 不仅改善了层状高分子纳米复合材料的力学性能, 同时赋予了纳米复合材料电磁屏蔽、导热和结构完整自监测等功能. 最后, 对冰模板技术仿生构筑的层状高分子纳米复合材料的结构设计、性能优化和应用拓展等未来的发展方向及存在的挑战进行了展望.

关键词: 贝壳珍珠层, 冰模板技术, 层状纳米复合材料, 力学性能, 功能应用

Ice templating, known as directional freeze casting, is a novel technique for constructing laminar porous materials by homogeneously dispersing or dissolving the building blocks, solvents and additives and using the “liquid-solid-gas” phase transition of the solvent. Inspired by the “brick-mortar” layered structure, the lamellar scaffold prepared from ice templating can be densified to construct nacre-like composite. This work presents a timely and systematic investigation and summary of frontier progresses of layered polymer nanocomposites constructed by the ice templating technique. Firstly, the densification strategies are classified according the different thickness of “brick” into three strategies: lamellar scaffold-filled polymer, hot-pressing treatment and mineralization. And typical layered polymer nanocomposites constructed by each strategy and their properties are also presented with classical examples. Subsequently, the design and functional applications of layered polymer nanocomposites are analyzed and discussed, such as the modulation of microstructures, introduction of functional building blocks, and enhancement of interfacial interactions, which not only improve the mechanical properties of layered polymer nanocomposites, but also endow them with functional applications, such as electromagnetic shielding, thermal conductivity and self-monitoring of structural integrity. Finally, we provide an outlook on the future directions and challenges of the structural design, performance optimization and application expansion of nacre-inspired layered polymer nanocomposites constructed by the ice templating technique.

Key words: natural nacre, ice template, layered polymer nanocomposites, mechanical property, functional application

引用此文

王华高, 程群峰. 冰模板技术仿生构筑层状高分子纳米复合材料的研究进展^★[J]. 化学学报, 2023, 81(9): 1231-1239.

Huagao Wang, Qunfeng Cheng. Recent Advances in the Nacre-inspired Layered Polymer Nanocomposites by Ice Templating Technique^★[J]. Acta Chimica Sinica, 2023, 81(9): 1231-1239.

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图/表 9

图1. 贝壳珍珠层的组成、多级结构及力学性能 (a)碳酸钙纳米颗粒和蛋白质与几丁质组成珍珠层; (b)文石片层间的界面相互作用: 矿物桥的连接、表面的纳米凸起抑制非弹性变形、粘弹性有机层和片层间形成的互锁结构; (c)珍珠层的扫描电子显微镜(SEM)照片, 表现出典型的“砖-泥”层状结构[1]; (d)珍珠层的抗裂纹扩展的R曲线[7]; (e)珍珠层的断裂表面SEM照片; (f)珍珠层裂纹扩展过程中的增韧机理, 显示出裂纹偏转、裂纹桥连和“砖”的滑移等[11]

Figure 1. Composition, hierarchical structure and properties of natural nacre (a) Calcium carbonate nanoparticles and proteins with chitin to form natural nacre; (b) Interfacial interaction between aragonite tablets: mainly including mineral bridges, surface protrusion to inhibit deformation, cohesive organic layer and plate interlocking; (c) SEM image of a natural nacre, showing a typical “brick-mortar” layered structure[1] (Copyright 2015 Springer Nature); (d) Crack resistance curves for natural nacre[7] (Copyright 2007 Springer Nature); (e) SEM image of the fracture surface of the nacre[1] (Copyright 2015 Springer Nature); (f) Toughening mechanisms during crack extension in natural nacre, showing crack deflection, crack bridge and tablets sliding[11] (Copyright 2016 AAAS)

图2. 冰模板技术仿生构筑层状高分子纳米复合材料的机理和过程 (a)浆料、悬浮液或分散液的制备; (b)通过定向冷冻使水凝结, 基元材料被排挤到片层冰晶之间; (c)冷冻干燥去除冰晶, 保留层状骨架; (d)骨架密实化处理制备层状高分子纳米复合材料[13,15]

Figure 2. Mechanisms and processes for constructing layered polymer nanocomposites by the ice templating technique (a) Preparation of slurry, solution or dispersion; (b) condensation of water by directional freezing and exclusion of building blocks between lamellar ice crystals; (c) freeze-drying to remove ice crystals and retain the lamellar scaffold; (d) densification of the lamellar scaffold to fabricate layered polymer nanocomposites[13,15]

图3. 冰模板技术制备层状高分子纳米复合材料的策略 (a)填充策略[41]; (b)热压策略[35]; (c)矿化生长策略[22]; (d)发展历程和代表性层状高分子纳米复合材料[19?????????????????????????-45]

Figure 3. Strategies for preparation of layered polymer nanocomposites by the ice templating technique (a) Filling strategy[41] (Copyright 2023 Wiley-VCH Verlag GmbH); (b) Hot-pressing strategy[35] (Copyright 2021 AAAS. http://creativecommons.org/ licenses/by /4.0/); (c) Mineralization strategy[22] (Copyright 2016 AAAS); (d) Development and representative layered polymer nanocomposites[19?????????????????????????-45]

图4. 骨架填充策略构筑仿珍珠层高分子纳米复合材料 (a)制备流程示意图; (b)仿珍珠层纳米复合材料的断面SEM照片(插图为实物照片)[24]; (c)人造材料与人类牙本质和牙釉质的硬度比较; (d)断裂韧性KJc随裂纹长度的变化曲线; (e)仿生层状纳米复合材料从锐化后尖端萌生的裂纹在扩展中的三维X射线断层渲染图[36]

Figure 4. Filling strategy for constructing nacre-like layered polymer nanocomposites (a) Schematic diagram of the constructing process; (b) SEM image of the nacre-like layered polymer nanocomposites (inset is an optical photograph)[24] (Copyright 2016 Wiley-VCH Verlag GmbH); (c) Comparison of the hardness of the artificial material with that of human dentin and enamel; (d) Rising crack-extension resistance curves; (e) XRT volume rendering of crack propagation initiated from a sharpened notch tip in the nacre-like layered polymer nanocomposites[36] (Copyright 2019 Wiley-VCH Verlag GmbH)

图5. 仿生层状高分子纳米复合材料 (a)长程有序层状纳米复合材料的显微计算机断层(micro-CT)扫描照片; (b)长程有序层状结构纳米复合材料的SEM照片[43]; (c)冷冻速率与层厚度之间的关系[29]; (d)交叉层状仿海螺壳高分子纳米复合材料[44]

Figure 5. Nacre-like layered polymer nanocomposites (a) Micro-computed tomography (micro-CT) scans of long-range layered nanocomposites; (b) SEM image of nanocomposites with long-range align structures[43] (Copyright 2020 AAAS. http://creativecommons.org/licenses/by/ 4.0/); (c) relationship between freezing rate and layer thickness[29] (Copyright 2019 Wiley-VCH Verlag GmbH); (d) polymer nanocomposites with cross- layered conch shell-like structures[44] (Copyright 2022 Wiley-VCH Verlag GmbH)

图6. 少量基元材料构筑的仿珍珠层高分子纳米复合材料 (a)层状石墨烯骨架的SEM照片; (b)层状石墨烯/环氧树脂纳米复合材料的SEM照片; (c)层状石墨烯/环氧树脂的断裂韧性KJc随裂纹长度的变化曲线[47]; (d)层状MXene/环氧树脂纳米复合材料的SEM照片; (e)层状MXene/环氧树脂纳米复合材料的界面作用示意图; (f)层状MXene/环氧树脂的断裂韧性KJc随裂纹长度的变化曲线[41]; (g)层状MMT/PDMS纳米复合材料的力学性能; (h)层状MMT/PDMS纳米复合材料的共聚焦荧光显微镜(CFM)照片; (i)层状MMT/PDMS纳米复合材料裂纹扩展过程中的CFM照片[34]

Figure 6. Nacre-like layered polymer nanocomposites constructed with a small amount of building blocks (a) SEM image of the layered graphene scaffold; (b) SEM image of the layered graphene/epoxy nanocomposites; (c) rising crack extension resistance curve for layered graphene/epoxy nanocomposites[47] (Copyright 2019 Elsevier); (d) SEM image of the layered MXene/epoxy nanocomposites; (e) schematic diagram of the interfacial interaction of layered MXene/epoxy nanocomposites; (f) rising crack extension resistance curve for layered MXene/epoxy nanocomposites[41] (Copyright 2023 Wiley-VCH Verlag GmbH); (g) Mechanical properties of layered MMT/PDMS nanocomposites; (h) Confocal fluorescence microscopy (CFM) image of layered MMT/PDMS nanocomposites; (i) CFM image of layered MMT/PDMS nanocomposites during crack extension[34] (Copyright 2021 Springer Nature. http://creativecommons.org/licenses/by/4.0/)

图7. 层状骨架热压策略构筑仿珍珠层复合材料 (a)热压制备仿贝壳珍珠层复合材料的示意图; (b)层状骨架的SEM照片; (c)蚕丝贝壳复合材料的SEM照片(插图为实物照片); (d)蚕丝贝壳复合材料的弯曲应力应变曲线[38]

Figure 7. Hot-pressing strategy for constructing nacre-like layered polymer nanocomposites (a) Schematic diagram of the preparation of silk nacre by hot pressing; (b) SEM image of the silk lamellar scaffold; (c) SEM image of the silk nacre (inset is an optical photograph); (d) bending stress-strain curve of the silk nacre[38] (Copyright 2022 AAAS. http://creativecommons.org/licenses/by/4.0/)

图8. 层状骨架矿化策略构筑人造贝壳珍珠层 (a)骨架矿化制备人造贝壳流程示意图; (b)人造贝壳珍珠层的实物照片; (c)人造贝壳珍珠层的SEM照片[22]; (d)人造贝壳珍珠层中磁性纳米颗粒的高分辨率透射电镜照片; (e)不同人造贝壳珍珠层的断裂韧性KJc随裂纹长度的变化曲线; (f)韧性放大因子的阿什比图[37]

Figure 8. Mineralization strategy for constructing artificial nacre (a) Fabrication scheme of the artificial nacre; (b) bulk synthetic nacre; (c) SEM image of the artificial nacre[22] (Copyright 2016 AAAS); (d) high-resolution transmission electron microscope image of magnetic nanoparticles in artificial nacre; (e) crack growth resistance curves of the artificial nacre; (f) Ashby plots of the toughness amplification factor[37] (Copyright 2022 Wiley-VCH Verlag GmbH)

图9. 仿生层状高分子纳米复合材料的代表性应用 (a)层状高分子纳米复合材料的电磁屏蔽机理[28]; (b)层状多孔PI /MXene纳米复合材料的电磁屏蔽效能[35]; (c)层状BN/PU纳米复合材料作为热界面材料的应用展示[40]; (d)和(e)层状MXene/环氧树脂复合材料的结构完整自监测[41]

Figure 9. Representative applications of layered polymer nanocomposites (a) Electromagnetic shielding mechanism of layered polymer nanocomposites[28] (Copyright 2018 American Chemical Society); (b) electromagnetic shielding effectiveness of layered porous PI/MXene nanocomposites[35] (Copyright 2021 AAAS. http://creativecommons.org/licenses/by/4.0/); (c) application demonstration of the BN/PU layered nanocomposites as a thermal interface material[40] (Copyright 2022 American Chemical Society); (d) and (e) self-monitoring of the structural integrity of layered MXene/epoxy nanocomposites[41] (Copyright 2023 Wiley-VCH Verlag GmbH)

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冰模板技术仿生构筑层状高分子纳米复合材料的研究进展^★

Recent Advances in the Nacre-inspired Layered Polymer Nanocomposites by Ice Templating Technique^★

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冰模板技术仿生构筑层状高分子纳米复合材料的研究进展★

Recent Advances in the Nacre-inspired Layered Polymer Nanocomposites by Ice Templating Technique★

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冰模板技术仿生构筑层状高分子纳米复合材料的研究进展^★

Recent Advances in the Nacre-inspired Layered Polymer Nanocomposites by Ice Templating Technique^★