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作 者:郭丝雨 顾少轩[1] 乔昂 陶海征[1] GUO Siyu;GU Shaoxuan;QIAO Ang;TAO Haizheng(State Key Laboratory of Silicate Materials for Architectures,Wuhan University of Technology,Wuhan 430070,China)
机构地区:[1]武汉理工大学硅酸盐建筑材料国家重点实验室,武汉430070
出 处:《硅酸盐通报》2024年第11期4208-4214,共7页Bulletin of the Chinese Ceramic Society
基 金:国家自然科学基金(22175135);广东省基础应用与研究基金(2022A1515010312)。
摘 要:金属有机骨架(MOF)晶体膜能够在分子层面上实现孔结构调控,因此在气体分离领域备受关注。然而,由于MOF晶体膜晶界缺陷多、成膜困难,制备高质量的MOF气体分离膜一直是一个挑战。为此,本文利用MOF玻璃无晶界、易成形的优势,提出了制备MOF晶体-玻璃复合膜的解决方案。首先采用原位溶剂热法制备了混晶复合和双层复合的ZIF-8/ZIF-62晶体膜,随后经熔融冷却制备成晶体-玻璃复合膜。结果表明:熔融的ZIF-62液相可以有效弥合晶界缺陷,使得膜层变得致密;相比于混晶膜,以ZIF-8/ZIF-62多层复合形式制得的晶体-玻璃复合膜对H_(2)/N_(2)、H_(2)/CH_(4)、CO_(2)/N_(2)、CO_(2)/CH_(4)混合气体具有更高的气体选择性和分离效率,尤其是对于H_(2)/CH_(4)、CO_(2)/CH_(4)混合气体,其气体选择性可分别达27.7、26.5。Metal organic framework(MOF)crystal films have attracted much attention in the field of gas separation due to their pore structure regulation at molecular level.However,the preparation of high quality MOF gas separation film has always been a challenge due to many grain boundary defects and the difficulty of film formation.Therefore,a solution to prepare MOF crystal-glass composite film was proposed in this paper,taking advantages of MOF glass without grain boundary and easy forming.Firstly,ZIF-8/ZIF-62 crystal film with mixed crystal composite and double layer composite was prepared by in-situ solvothermal method,and then the crystal-glass composite film was prepared by melting and cooling.The results show that the fused ZIF-62 liquid phase can effectively bridge the grain boundary defects and make film dense.Compared with mixed crystal films,the crystal-glass composite films prepared by ZIF-8/ZIF-62 multilayer composite films have higher gas selectivity and separation efficiency for H_(2)/N_(2),H_(2)/CH_(4),CO_(2)/N_(2),and CO_(2)/CH_(4)mixed gases.Especially for H_(2)/CH_(4)and CO_(2)/CH_(4),the selectivity can reach 27.7 and 26.5,respectively.
关 键 词:ZIF-8 ZIF-62 ZIF晶体-玻璃复合膜 熔融冷却 理想气体选择性
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