石墨烯基材料在CO2分离膜领域的研究进展

doi:10.16085/j.issn.1000-6613.2022-0164

摘要/Abstract

摘要：

节能高效的CO₂分离技术的开发具有重要的现实及长远意义，膜法CO₂分离在该领域备受关注，具有优异传质特性的新型分离膜材料对膜分离过程有决定性的影响。近年来，石墨烯及其衍生材料因独特的单原子层厚度、亚纳米级别的孔道结构以及优异的机械、化学和热稳定性，成为气体分离膜领域的研究热点，膜的加工难度、技术成本、大面积制备、工作稳定性等问题是限制其实际应用的关键因素。石墨烯基CO₂分离膜主要有三种形式：纳米孔石墨烯膜、层状结构氧化石墨烯膜、基于石墨烯及其衍生材料的混合基质膜。本文综述了石墨烯基CO₂分离膜领域的突破性研究进展，重点介绍了气体的跨膜传质机理和膜的构性关系，总结了膜性能的优化思路和原理，梳理了石墨烯基CO₂分离膜发展面临的挑战，提出了潜在的研究方向。分析表明，进行系统的理论研究，采用先进的表征手段，以建立膜构性关系的理论模型，指导膜结构设计是未来研究的重点。此外，进一步降低膜加工成本，充分研究膜在实际工作环境中的稳定性也至关重要。

关键词: 二维材料, 二氧化碳分离, 界面调控, 混合基质膜

Abstract:

The development of CO₂ separation technologies with high efficiency and energy effectiveness has practical and long-term significance. Membrane based CO₂ separation has become a promising approach owing to its low energy consumption, easy operation, small footprint and cost effectiveness. Currently, the focus of membrane research is searching for novel membrane materials with excellent transport characteristics. Graphene and its derivatives have gained great attention in the field of gas separation because of the atomic thickness, sub-nano pore size and excellent mechanical, thermal and chemical stability. The limiting factors for the practical applications include the difficulties in processing, technological cost, large-area fabrication and membrane working stability. Graphene-based CO₂ separation membranes can be categorized as: nanoporous graphene, lamellar graphene oxide membranes and mixed matrix membranes with graphene and its derivatives as the nanofillers. The review summarized outstanding breakthroughs regarding graphene-based CO₂ separation membranes, emphasizing the gas transport mechanisms and structure-property relationships. Optimization strategies based on rational design and the underlying mechanisms discussed. Challenges analyzed and the potential research directions proposed. Systematic theoretical research should be conducted combined with advanced characterization methods to establish structure-property relationship of membranes. In addition, the cost-effectiveness and working stability vital for the practical applications.

Key words: two-dimensional materials, carbon dioxide separation, interface regulation, mixed matrix membrane

中图分类号:

赵国珂, 潘国元, 张杨, 于浩, 赵慕华, 唐功庆, 刘轶群. 石墨烯基材料在CO₂分离膜领域的研究进展[J]. 化工进展, 2022, 41(11): 5896-5911.

ZHAO Guoke, PAN Guoyuan, ZHANG Yang, YU Hao, ZHAO Muhua, TANG Gongqing, LIU Yiqun. Recent advances in graphene-based membranes for CO₂ separation[J]. Chemical Industry and Engineering Progress, 2022, 41(11): 5896-5911.

图/表 11

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膜材料	制备方法	分离物系	测试条件	CO₂渗透通量/GPU	选择因子	参考文献
纳米孔石墨烯膜	聚焦离子束轰击	H₂/CO₂	室温，2bar	6.4×10⁶	4.69	［30］
PEI修饰的纳米孔石墨烯	氧等离子体刻蚀	CO₂/N₂	30℃，2bar	6180	22.5	［31］
GO膜	喷涂法	H₂/CO₂	25℃，1bar	3.88	20.9	［33］
GO膜	真空抽滤法	H₂/CO₂	20℃，1bar	0.09	3400	［39］
GO膜	真空抽滤法	H₂/CO₂	室温，Ar吹扫	11.4	35.3	［41］
GO膜	真空抽滤法	H₂/CO₂	室温，Ar吹扫	4.25	240	［44］
哌嗪修饰的GO膜	真空抽滤法	CO₂/N₂	室温，He吹扫	1020	680	［46］
乙二胺修饰的GO膜	真空抽滤法	CO₂/N₂	75℃，He吹扫	660	500	［47］
硼酸盐修饰的GO膜	真空抽滤法	CO₂/CH₄	30℃，1bar	650	75	［48］
Zn²⁺修饰的GO膜	真空抽滤法	CO₂/CH₄	30℃，1.5bar	175	19.1	［49］
离子液体修饰的GO膜	真空抽滤法	CO₂/N₂	室温，1bar	68.5	382	［53］

膜材料	制备方法	分离物系	测试条件	CO₂渗透通量/GPU	选择因子	参考文献
纳米孔石墨烯膜	聚焦离子束轰击	H₂/CO₂	室温，2bar	6.4×10⁶	4.69	［30］
PEI修饰的纳米孔石墨烯	氧等离子体刻蚀	CO₂/N₂	30℃，2bar	6180	22.5	［31］
GO膜	喷涂法	H₂/CO₂	25℃，1bar	3.88	20.9	［33］
GO膜	真空抽滤法	H₂/CO₂	20℃，1bar	0.09	3400	［39］
GO膜	真空抽滤法	H₂/CO₂	室温，Ar吹扫	11.4	35.3	［41］
GO膜	真空抽滤法	H₂/CO₂	室温，Ar吹扫	4.25	240	［44］
哌嗪修饰的GO膜	真空抽滤法	CO₂/N₂	室温，He吹扫	1020	680	［46］
乙二胺修饰的GO膜	真空抽滤法	CO₂/N₂	75℃，He吹扫	660	500	［47］
硼酸盐修饰的GO膜	真空抽滤法	CO₂/CH₄	30℃，1bar	650	75	［48］
Zn²⁺修饰的GO膜	真空抽滤法	CO₂/CH₄	30℃，1.5bar	175	19.1	［49］
离子液体修饰的GO膜	真空抽滤法	CO₂/N₂	室温，1bar	68.5	382	［53］

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石墨烯基材料在CO₂分离膜领域的研究进展

Recent advances in graphene-based membranes for CO₂ separation

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