Self‐Assembly of Thiourea‐Crosslinked Graphene Oxide Framework Membranes toward Separation of Small Molecules

Advanced Materials - Tập 30 Số 16 - 2018
Jingjing Yang1,2, Dian Gong1,3, Guihua Li1, Gaofeng Zeng1,4, Qiyan Wang1,3, Yelei Zhang1,3, Guojuan Liu1, Ping Wu1, Evgeny I. Vovk4, Zheng Peng4, Xin‐Hui Zhou4, Yong Yang4, Zhi Liu4, Yuhan Sun1,4
1CAS Key Laboratory of Low-Carbon Conversion Science and Engineering, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 100 Haike Road, Shanghai 201210, China
2Department of Electronic Information Materials School of Materials Science and Engineering, Shanghai University, 99 Shangda Road, Shanghai, 200444 China
3School of Chemical Sciences, University of Chinese Academy of Sciences, 19A Yuquan Road, Beijing 100049, China
4School of Physical Science and Technology, ShanghaiTech University, 393 Middle Huaxia Road, Shanghai, 201210, China

Tóm tắt

AbstractThe poor mechanical strength of graphene oxide (GO) membranes, caused by the weak interlamellar interactions, poses a critical challenge for any practical application. In addition, intrinsic but large‐sized 2D channels of stacked GO membranes lead to low selectivity for small molecules. To address the mechanical strength and 2D channel size control, thiourea covalent‐linked graphene oxide framework (TU‐GOF) membranes on porous ceramics are developed through a facile hydrothermal self‐assembly synthesis. With this strategy, thiourea‐bridged GO laminates periodically through the dehydration condensation reactions via NH2 and/or SH with OCOH as well as the nucleophilic addition reactions of NH2 to COC, leading to narrowed and structurally well‐defined 2D channels due to the small dimension of the covalent TU‐link and the deoxygenated processes. The resultant TU‐GOF/ceramic composite membranes feature excellent sieving capabilities for small species, leading to high hydrogen permselectivities and nearly complete rejections for methanol and small ions in gas, solvent, and saline water separations. Moreover, the covalent bonding formed at the GO/support and GO/GO interfaces endows the composite membrane with significantly enhanced stability.

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