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通过聚乙二醇辅助水热法和配位络合构建随机层状HKUST-1@斜发沸石用于增强CO和CH的吸附分离

Constructing Randomly Lamellar HKUST-1@Clinoptilolite through Polyethylene Glycol-Assisted Hydrothermal Method and Coordinated Complexation for Enhanced Adsorptive Separation for CO and CH.

作者信息

Zhang Mingxuan, Zhou Jiawei, Wan Chunlei, Liu Ming, Wu Xia, Sun Jihong

机构信息

Beijing Key Laboratory for Green Catalysis and Separation, Department of Chemical Engineering, Beijing University of Technology, Beijing 100124, China.

出版信息

Nanomaterials (Basel). 2023 Jun 14;13(12):1860. doi: 10.3390/nano13121860.

Abstract

Clinoptilolite (CP) was successfully synthesized via a hydrothermal route in the presence of polyethylene glycol (PEG), and it was then delaminated by washing using Zn containing acid. HKUST-1, as one kind of the Cu-based MOFs, showed a high CO adsorption capacity owing to its large pore volume and specific surface area. In the present work, we selected one of the most efficient ways for preparing the HKUST-1@CP compounds via coordination between exchanged Cu and ligand (trimesic acid). Their structural and textural properties were characterized by XRD, SAXS, N sorption isotherms, SEM, and TG-DSC profiles. Particularly, the effect of the additive PEG (average molecular weight of 600) on the induction (nucleation) periods and growth behaviors were detailed and investigated in the hydrothermal crystallization procedures of synthetic CPs. The corresponding activation energies of induction () and growth () periods during crystallization intervals were calculated. Meanwhile, the pore size of the inter-particles of HKUST-1@CP was 14.16 nm, and the BET specific area and pore volume were 55.2 m/g and 0.20 cm/g, respectively. Their CO and CH adsorption capacities and selectivity were preliminarily explored, showing 0.93 mmol/g for HKUST-1@CP at 298 K with the highest selective factor of 5.87 for CO/CH, and the dynamic separation performance was evaluated in column breakthrough experiments. These results suggested an efficient way of preparing zeolites and MOFs composites that is conducive to being a promising adsorbent for applications in gas separation.

摘要

斜发沸石(CP)在聚乙二醇(PEG)存在下通过水热法成功合成,然后用含锌酸洗涤使其分层。HKUST-1作为一种铜基金属有机框架材料,因其大的孔体积和比表面积而表现出高的CO吸附容量。在本工作中,我们选择了一种最有效的方法,通过交换的铜与配体(均苯三甲酸)之间的配位作用来制备HKUST-1@CP化合物。通过XRD、SAXS、N吸附等温线、SEM和TG-DSC曲线对其结构和织构性质进行了表征。特别地,在合成CP的水热结晶过程中,详细研究了添加剂PEG(平均分子量为600)对诱导(成核)期和生长行为的影响。计算了结晶区间内诱导期()和生长期()的相应活化能。同时,HKUST-1@CP颗粒间的孔径为14.16nm,BET比表面积和孔体积分别为55.2m/g和0.20cm/g。初步探索了它们对CO和CH的吸附容量及选择性,在298K时HKUST-1@CP对CO的吸附容量为0.93mmol/g,CO/CH的最高选择性因子为5.87,并在柱穿透实验中评估了动态分离性能。这些结果表明了一种制备沸石和金属有机框架复合材料的有效方法,这有利于其成为气体分离应用中一种有前景的吸附剂。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d768/10303906/f616f219aa3c/nanomaterials-13-01860-g001.jpg

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