Qin Yu, Xu Li, Liu Liying, Deng Xiaoyu, Gao Yucheng, Ding Zhongwei
Beijing Key Laboratory of Membrane Science and Technology, College of Chemical Engineering, Beijing University of Chemical Technology Beijing 100029 China
RSC Adv. 2021 Aug 27;11(46):28863-28875. doi: 10.1039/d1ra04801e. eCollection 2021 Aug 23.
A novel gas separation approach is proposed in this work by combining an amine-based solid adsorbent with a zeolitic imidazolate framework-8 (ZIF-8) membrane. This was achieved by incorporating the amine-based solid adsorbent during the fabrication of the ZIF-8 membrane on a macroporous substrate. An amine-based solid adsorbent was prepared using porous ZIF-8-3-isocyanatopropyltrimethoxysilane (IPTMS) and -[(3-trimethoxysilyl)propyl]diethylenetriamine (3N-APS) amine compounds. The as-prepared porous amine-based solid adsorbent (denoted as ZIF-8-IPTMS-3N-APS) possessed excellent adsorptive CO/N and CO/CH separation performances. As the adsorbent needs to be regenerated, this could indicate that the CO adsorption separation process cannot be continuously operated. In this work, an amine-based solid adsorbent was applied during the preparation of the ZIF-8 membranes owing to the following reasons: (i) gas separation by the membrane can be operated continuously; (ii) the amino group provides a heterogeneous nucleation site for ZIF-8 to grow; and (iii) the reparation of surface defects on the macroporous substrate can be performed prior to the growth of the ZIF-8 membrane. Herein, the ZIF-8 membrane was successfully fabricated, and it possessed excellent CO/CH, CO/N, and H/CH separation performances. The 0.6 μm ultrathin ZIF-8 membrane demonstrated a high CO permeance of 4.75 × 10 mol m s Pa at 35 °C and 0.1 MPa, and ideal CO/N and CO/CH selectivities of 4.67 and 6.02, respectively. Furthermore, at 35 °C and 0.1 MPa, the ideal H/CH selectivity of the ZIF-8 membrane reached 31.2, and a significantly high H permeance of 2.45 × 10 mol m s Pa.
本工作提出了一种将胺基固体吸附剂与沸石咪唑酯骨架-8(ZIF-8)膜相结合的新型气体分离方法。这是通过在大孔基材上制备ZIF-8膜的过程中加入胺基固体吸附剂来实现的。使用多孔ZIF-8-3-异氰酸丙基三甲氧基硅烷(IPTMS)和-[(3-三甲氧基甲硅烷基)丙基]二乙烯三胺(3N-APS)胺化合物制备了胺基固体吸附剂。所制备的多孔胺基固体吸附剂(表示为ZIF-8-IPTMS-3N-APS)具有优异的吸附CO/N和CO/CH分离性能。由于吸附剂需要再生,这可能表明CO吸附分离过程无法连续运行。在本工作中,由于以下原因,在制备ZIF-8膜的过程中应用了胺基固体吸附剂:(i)膜的气体分离可以连续运行;(ii)氨基为ZIF-8的生长提供了异质成核位点;(iii)可以在ZIF-8膜生长之前对大孔基材上的表面缺陷进行修复。在此,成功制备了ZIF-8膜,其具有优异的CO/CH、CO/N和H/CH分离性能。0.6μm的超薄ZIF-8膜在35℃和0.1MPa下表现出4.75×10 mol m s Pa的高CO渗透率,以及分别为4.67和6.02的理想CO/N和CO/CH选择性。此外,在35℃和0.1MPa下,ZIF-8膜的理想H/CH选择性达到31.2,H渗透率显著高达2.45×10 mol m s Pa。