Preparation of Mg-MOF-74 membranes via layer-by-layer seeding and its separation properties

doi:10.11949/j.issn.0438-1157.20140988

CIESC Journal ›› 2015, Vol. 66 ›› Issue (1): 478-485.DOI: 10.11949/j.issn.0438-1157.20140988

Preparation of Mg-MOF-74 membranes via layer-by-layer seeding and its separation properties

LI Fang¹, LI Qiming^1,2, YU Xiaofei¹, BAO Xinxia¹, LIU Haolin¹, JIA Kun¹

1 School of Chemistry, Chemical Engineering and Environmental Engineering, Liaoning Shihua University, Fushun 113001, Liaoning, China;
2 Key Laboratory of Coal to Ethylene Glycol and Its Related Technology, Chinese Academy of Sciences, Fuzhou 350002, Fujian, China

Received:2014-06-30 Revised:2014-08-27 Online:2015-01-05 Published:2015-01-05
Supported by:
supported by the National Natural Science Foundation of China (21201096), Liaoning Province Education Administration (L2010242) and the support from Key Laboratory of Coal to Ethylene Glycol and Its Related Technology, Chinese Academy of Sciences.

层层组装晶种法制备Mg-MOF-74膜及其分离性能

李芳¹, 李其明^1,2, 于晓飞¹, 鲍新侠¹, 刘浩林¹, 贾坤¹

1 辽宁石油化工大学化学化工与环境学部, 辽宁抚顺 113001;
2 中国科学院煤制乙二醇及相关技术重点实验室, 福建福州 350002

通讯作者: 李其明
基金资助:
国家自然科学基金项目(21201096);辽宁省教育厅资助项目(L2010242);中国科学院煤制乙二醇及相关技术重点实验室资助项目。

Abstract

Abstract:

Continuous and dense Mg-MOF-74 membranes were prepared through a combined layer-by-layer seeding assembling and secondary growth method based on 2, 5-dihydroxybenzoic acid and magnesium acetate solution. The adhesion between Mg-MOF-74 crystals and a-Al₂O₃ support could be considerably improved by the alternate immersion assembling of 2, 5-dihydroxybenzoic acid and magnesium acetate solution. Compared with the in-situ crystallization technique, Mg-MOF-74 membranes synthesized by four-cycle layer-by-layer method exhibited improved molecule-sieving properties due to optimized membrane continuity and density. Single gas test indicated that the best Mg-MOF-74 membrane had H₂/CO₂ ideal selectivity as high as 8.96, higher than its Knudsen diffusion selectivity. XRD measurement proved that the XRD patterns of Mg-MOF-74 membranes were consistent with those of powdered Mg-MOF-74 from published papers, which implied that our membranes were composed of randomly oriented MOF-74 crystals. SEM characterization showed that the MOF-74 crystals possessed wheat-shaped morphology and specific BET surface area as high as 1182 m²·g^-1.

Key words: membrane, microstructure, crystallization, Mg-MOF-74 membrane, layer-by-layer assembling

摘要：

以2,5-二羟基对苯二甲酸和乙酸镁溶液为原料通过交替浸渍层层组装法在a-Al₂O₃载体表面预置晶种层, 再利用二次生长法制备出连续而致密的Mg-MOF-74晶体膜。采用X射线衍射(XRD)和扫描电镜(SEM)对膜进行了表征。实验结果表明:相比于原位溶剂热合成法, 通过2, 5-二羟基对苯二甲酸和乙酸镁交替浸渍层层组装法可以增强Mg-MOF-74与氧化铝基体之间的附着效果, 提高晶体薄膜的致密性与连续性, 实验发现4次交替浸渍层层组装预置晶种可以制备出具有分子筛分性能的Mg-MOF-74晶体膜, 单组分气体渗透测试表明其H₂/CO₂的理想选择性可以达到8.96, 高于其努森扩散选择性。XRD测试表明该晶体膜的特征衍射峰与文献报告的粉末MOF-74完全一致, 表明Mg-MOF-74晶粒以无取向形式生长于氧化铝载体表面。SEM表征表明Mg-MOF-74晶粒呈麦粒状微观外形, 其BET比表面积可以达到1182 m²·g^-1。

关键词: 膜, 微观结构, 晶化, Mg-MOF-74晶体膜, 层层组装

CLC Number:

O614.241

LI Fang, LI Qiming, YU Xiaofei, BAO Xinxia, LIU Haolin, JIA Kun. Preparation of Mg-MOF-74 membranes via layer-by-layer seeding and its separation properties[J]. CIESC Journal, 2015, 66(1): 478-485.

李芳, 李其明, 于晓飞, 鲍新侠, 刘浩林, 贾坤. 层层组装晶种法制备Mg-MOF-74膜及其分离性能[J]. 化工学报, 2015, 66(1): 478-485.

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Preparation of Mg-MOF-74 membranes via layer-by-layer seeding and its separation properties

层层组装晶种法制备Mg-MOF-74膜及其分离性能

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