Preparation of free-standing graphene carbon membrane for gas separation

doi:10.11949/j.issn.0438-1157.20160591

CIESC Journal ›› 2016, Vol. 67 ›› Issue (10): 4225-4230.DOI: 10.11949/j.issn.0438-1157.20160591

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Preparation of free-standing graphene carbon membrane for gas separation

ZHANG Shengyi, LI Lin, WANG Chunlei, ZHENG Tianfu, SUN Yaming, WANG Tonghua

School of Chemical Engineering, Dalian University of Technology, Dalian 116085, Liaoning, China

Received:2016-05-04 Revised:2016-06-17 Online:2016-10-05 Published:2016-10-05
Supported by:
supported by the National Natural Science Foundation of China (21436009, 21576035, 21506020, 21376037), the China Postdoctoral Science Foundation (2014M561232) and the Fundamental Research Funds for the Central Universities (DUT16RC(4)05).

自支撑石墨烯炭膜的制备及气体分离性能

张生义, 李琳, 王春雷, 郑天赋, 孙亚明, 王同华

大连理工大学化工学院, 辽宁大连 116085

通讯作者: 王同华
基金资助:
国家自然科学基金项目（21436009，21576035，21506020，21376037）；中国博士后第56批科学基金项目（2014M561232）；中央高校基本科研业务费专项资金项目（DUT16RC(4)05）。

Abstract

Abstract:

Free-standing graphene carbon membrane with conch nacre structure was prepared via carbonizing composite membrane of graphene oxide (GO) and polyamide acid (PAA) obtained by solvent evaporation method at 600℃. The morphology and structure were characterized by XRD and SEM. The permeation performance of CO₂ and CH₄ of free-standing graphene carbon membrane with different PAA solid content was investigated. The results indicated that GO was thermally reduced to graphene in graphene carbon membrane after carbonization, in which graphene layers were lamellar stacked and gaps between layers were filled with holes and carbon residue. Both CO₂ permeability and ideal selectivity for the CO₂/CH₄ of graphene carbon membranes were enhanced with increasing PAA solid content. The CO₂ flux of graphene carbon membrane was up to 824 barrer and the CO₂/CH₄ ideal selectivity reached 38.9 simultaneously. The gas permeation channels of graphene carbon membrane were attributed to the lamellar stacked of graphene and carbon molecule sieve in graphene carbon membrane. This study opened up new opportunities to prepare the flexible free-standing graphene carbon membrane for gas separation.

Key words: membrane, molecular sieve, gas separation, graphene, carbon membrane, free-standing

摘要：

通过溶剂蒸发法得到聚酰胺酸（PAA）与氧化石墨烯（GO）的复合石墨烯膜，并经600℃炭化制备了具有良好柔韧性的仿贝壳珍珠层结构的自支撑石墨烯炭膜。通过X射线衍射和场发射扫描电镜对薄膜微观结构进行表征，并测试不同PAA固含量制备的石墨烯炭膜对CO₂和CH₄的分离性能。结果表明，炭化后，GO被还原成石墨烯，呈层状堆叠，堆叠的层间填充了空穴和残炭；石墨烯炭膜的CO₂渗透通量和CO₂/CH₄分离理想选择性随PAA加入量增加，CO₂通量最高可达824 barrer，此时CO₂/CH₄理想选择性达38.9。石墨烯层骨架和碳分子筛构成石墨烯炭膜的气体传输通道，本研究成果为柔性自支撑气体分离炭膜的制备开辟了新思路。

关键词: 膜, 分子筛, 气体分离, 石墨烯, 炭膜, 自支撑

CLC Number:

TQ028.8

ZHANG Shengyi, LI Lin, WANG Chunlei, ZHENG Tianfu, SUN Yaming, WANG Tonghua. Preparation of free-standing graphene carbon membrane for gas separation[J]. CIESC Journal, 2016, 67(10): 4225-4230.

张生义, 李琳, 王春雷, 郑天赋, 孙亚明, 王同华. 自支撑石墨烯炭膜的制备及气体分离性能[J]. 化工学报, 2016, 67(10): 4225-4230.

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Preparation of free-standing graphene carbon membrane for gas separation

自支撑石墨烯炭膜的制备及气体分离性能

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