Cheng Long, Yang Haonan, Chen Xingyu, Liu Guozhen, Guo Yanan, Liu Gongping, Jin Wanqin
State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, 30 Puzhu Road, Nanjing, 211816, P. R. China.
Chem Asian J. 2021 Oct 18;16(20):3162-3169. doi: 10.1002/asia.202100834. Epub 2021 Aug 23.
Graphene oxide (GO) is a promising two-dimensional building block for fabricating high-performance gas separation membranes. Whereas the tortuous transport pathway may increase the transport distance and lead to a low gas permeation rate, introducing spacers into GO laminates is an effective strategy to enlarge the interlayer channel for enhanced gas permeance. Herein, we propose to intercalate CO -philic MIL-101(Cr) metal-organic framework nanocrystals into the GO laminates to construct a 2D/3D hybrid structure for gas separation. The interlayer channels were partially opened up to accelerate gas permeation. Meanwhile, the intrinsic pores of MIL-101 provided additional transport pathways, and the affinity of MIL-101 to CO molecules resulted in higher H /CO diffusion selectivity, leading to a simultaneous enhancement in gas permeance and separation selectivity. The MIL-101(Cr)/GO membrane with optimal structures exhibited outstanding and stable mixed-gas separation performance with H permeance of 67.5 GPU and H /CO selectivity of 30.3 during the 120-h continuous test, demonstrating its potential in H purification application.
氧化石墨烯（GO）是一种用于制造高性能气体分离膜的很有前景的二维构建单元。然而，曲折的传输路径可能会增加传输距离并导致气体渗透率较低，在氧化石墨烯层压板中引入间隔物是扩大层间通道以提高气体渗透率的有效策略。在此，我们建议将亲CO的MIL-101（Cr）金属有机框架纳米晶体插入到氧化石墨烯层压板中，以构建用于气体分离的二维/三维混合结构。层间通道被部分打开以加速气体渗透。同时，MIL-101的固有孔隙提供了额外的传输路径，并且MIL-101对CO分子的亲和力导致更高的H₂/CO扩散选择性，从而导致气体渗透率和分离选择性同时提高。具有最佳结构的MIL-101（Cr）/GO膜在120小时的连续测试中表现出出色且稳定的混合气体分离性能，H₂渗透率为67.5 GPU，H₂/CO选择性为30.3，证明了其在H₂纯化应用中的潜力。
