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化学进展 2021, Vol. 33 Issue (4): 670-677 DOI: 10.7536/PC200459 前一篇   后一篇

• 综述 •

氧化石墨烯分离膜机械性能调控

朱彬彬1,2, 郑晓慧2,*(), 杨光2, 曾旭1,2(), 邱伟1,2, 徐斌1,*   

  1. 1 北京化工大学有机-无机复合材料国家重点实验室 材料电化学过程与技术北京市重点实验室 北京 100029
    2 军事科学院防化研究院 国民核生化灾害防护国家重点实验室 北京 100191
  • 收稿日期:2020-04-29 修回日期:2020-08-31 出版日期:2021-04-20 发布日期:2020-10-15
  • 通讯作者: 郑晓慧, 徐斌
  • 基金资助:
    国家自然科学基金项目(51572011)
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Mechanical Property Regulation of Graphene Oxide Separation Membranes

Binbin Zhu1,2, Xiaohui Zheng2(), Guang Yang2, Xu Zeng1,2(), Wei Qiu1,2, Bin Xu1   

  1. 1 State Key Laboratory of Organic-Inorganic Composites, Beijing Key Laboratory of Electrochemical Process and Technology for Materials, Beijing University of Chemical Technology,Beijing 100029, China
    2 State Key Laboratory of NBC Protection for Civilian, Research Institute of Chemical Defense, Academy of Military Sciences, Beijing 100191, China
  • Received:2020-04-29 Revised:2020-08-31 Online:2021-04-20 Published:2020-10-15
  • Contact: Xiaohui Zheng, Bin Xu
  • Supported by:
    the National Natural Science Foundation of China(51572011)

氧化石墨烯(Graphene oxide, GO)片层组装制备的分离膜,具有可调控的纳米通道和独特的分离性能,是一种很有前景的分离材料,但较差的机械性能制约了其实际应用。将活性分子、阳离子等粒子引入到GO膜的片层间,利用其与GO形成的稳定键合可提高GO膜的机械性能。本文综述了国内外在GO膜机械性能调控方面的研究进展。依据引入的粒子与GO成键的类型可分为共价键法和非共价键法,其中共价键法又分为大分子共价键法和小分子共价键法,非共价键法分为氢键法、π-π键法和离子键法。无论共价键法还是非共价键法都能显著提升GO膜的机械性能,其中共价键法对GO复合膜的增强效果优于非共价键法,大分子共价键法优于小分子共价键法。最后,阐述了现有方法存在的问题,并对未来的发展前景做出了展望。

关键词： 氧化石墨烯膜, 机械性能, 共价键, 非共价键

Due to the controllable nanoscale channels and unique separation performance, the separation films assembled from graphene oxide(GO) nanosheets are promising separation materials, but the unsatisfactory mechanical properties restrict their practical application. Introducing particles such as active molecules and cations between the GO nanosheets can improve the mechanical properties of the GO membranes due to the formation of the stable bonding. In this review, the recent progress on the methods for improving the mechanical properties of GO membranes is summarized. According to the bonding mode between GO and the introduced particles, these methods can be divided into two types, covalent bonding and non-covalent bonding. Furthermore, covalent bonding methods can be divided into macromolecular covalent bonding and small molecule covalent bonding, while noncovalent bonding methods include hydrogen bonding, π-π bonding and ionic bonding. Both covalent bonding and noncovalent bonding can significantly improve the mechanical properties of the GO films, while the covalent bonding methods are more effective. Among the covalent bonding methods, the macromolecule covalent bonding is superior to the small molecule covalent bonding. Finally, the major problems of the current methods for enhancing the mechanical property of GO are discussed, and the future prospects is proposed.

Content:

1 Introduction

2 Covalent bonding method

2.1 Small molecule covalent bonding method

2.2 Macromolecular covalent bonding method

3 Noncovalent bonding method

3.1 Ionic bonding method

3.2 Hydrogen bonding method

3.3 π-π bonding method

4 Conclusion and prospect

Key words: 670/img_1.png509.95253.9graphene oxide membranes, mechanical properties, covalent bonding, noncovalent bonding
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图1 (a)大分子共价键法的交联反应图;(b)小分子共价键法的交联反应图;(c)离子键法的交联反应图;(d)氢键法的交联反应图;(e)π-π键法的交联反应图
Fig.1 (a) Cross-linking reaction diagram of macromolecular covalent bonding method;(b) Cross-linking reaction diagram of small molecule covalent bonding method;(c) Cross-linking reaction diagram of ion bonding method;(d) Cross-linking reaction diagram of hydrogen bonding method;(e) Cross-linking reaction diagram of π-π bonding method
图2 纯GO膜与小分子改性GO膜的力学性能:(a)典型的拉伸应力应变曲线;(b)试件的模量和强度总结;(c)典型的蠕变恢复曲线[19]
Fig.2 Mechanical properties of raw material GO and modified GO:(a) typical tensile stress-strain curve;(b) summary of modulus and strength of the specimen;(c) typical creep recovery curve[19]
图3 硼酸盐交联的复合膜的表征测试:(a)未改性(绿色)与硼酸盐改性(蓝色)GO薄膜的应力应变曲线;(b) 未改性GO薄膜(黑色)、硼酸盐改性GO膜(红色,0.08 wt% B)及无序硼酸盐改性GO膜(绿色,6.32 wt% B)的XRD表征结果[11]
Fig.3 Characterization tests of borate crosslinked composite films :(a) stress-strain curves of unmodified(green) and borate modified(blue) GO films;(b) XRD characterization results of unmodified GO film(black), borate modified GO film(red, 0.08 wt% B) and disordered borate modified GO film(green, 6.32 wt% B)[11]
图4 循环加载实验中得到的GO膜的应力应变曲线:(a)未改性GO膜循环加载实验中应力应变曲线原图;(b) 漂洗Ca2+改性GO复合膜循环加载实验中应力应变曲线原图;(c)未改性GO膜循环加载实验中放大的初始区域;(d)改性后循环加载实验中放大的初始区域[43]
Fig.4 Stress-strain curve of GO membrane obtained in cyclic loading experiment:(a) original diagram of stress and strain curve in cyclic loading experiment of unmodified GO film;(b) the original stress-strain curve of the rinsing Ca2+ modified GO composite membrane under cyclic loading;(c) the enlarged initial region in the cyclic loading experiment of unmodified GO film;(d) the enlarged initial area in the cyclic loading experiment after modification[43]
图5 (a) 水含量对GO层间距的影响(C10O1(OH)1(红色)和C10O2(OH)2(绿色));(b) 氢氧键能随键间距的变化[51]
Fig.5 (a) influence of water content on GO layer spacing(C10O1(OH)1(red) and C10O2(OH)2(green));(b) Hydrogen and oxygen bond energies vary with bond spacing[51]
图6 (a)以水为溶剂制备的PVA-GO复合膜的杨氏模量和拉伸强度;(b)以DMF为溶剂制备的PMMA-GO复合膜的杨氏模量和拉伸强度[52]
Fig.6 (a) Young’s modulus and tensile strength of GO composite membrane based on PVA prepared in water;(b) Young’s modulus and tensile strength of GO composite membrane based on PMMA prepared in DMF[52]
表1 GO复合膜机械性能改性情况汇总表
Table 1 Summary of mechanical properties modification of GO composite membrane
number GO matrix composite Bonding mode Tensile strength(MPa) Toughness(MJ ·m -3) ref
1 GO-PVA Covalent bond 360 1.4 62
2 GO-MXene-GO Covalent bond 226.3 6.2 54
3 GO/PAA Covalent bond 92 0.2 38
4 GO/PEI Covalent bond 210 0.4 55
5 GO/GA Covalent bond 101 0.3 19
6 GO/Borate Covalent bond 170 0.1 43
7 GO-PDA Covalent bond 175 1.5 39
8 GO-PCDO Covalent bond 106.6 2.52 29
9 GO-PAH Covalent bond 128.2 0.82 56
10 GO-PMMA Hydrogen bonding 148.3 2.35 52
11 GO-CNC Hydrogen bonding 490 3.9 57
12 GO-Ca2+ Ionic bond 125.8 0.31 45
13 GO-Mg2+ Ionic bond 80.6 0.13 58
14 GO-Al3+ Ionic bond 100.5 0.23 58
15 GO-AA-SCMC π-π bond+Hydrogen bonding 305.0 8.2 59
16 Al2O3/GO-PVA Covalent bond+Hydrogen bonding 143.0 9.2 60
17 GO-MMT-SPVA Covalent bond+Hydrogen bonding 250 2.7 61
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摘要

氧化石墨烯分离膜机械性能调控