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作 者:叶茂 奥德 孙玉绣 顾振杰[1,4] 杨紫博 乔志华 YE Mao;AO De;SUN Yuxiu;GU Zhenjie;YANG Zibo;QIAO Zhihua(State Key Laboratory of Separation Membranes and Membrane Processes,Tiangong University,Tianjin 300387,China;School of Textile Science and Engineering,Tiangong University,Tianjin 300387,China;School of Chemical Engineering and Technology,Tiangong University,Tianjin 300387,China;School of Physical Science and Technology,Tiangong University,Tianjin 300387,China;School of Materials Science and Engineering,Tiangong University,Tianjin 300387,China;Hebei Key Laboratory of Heterocyclic Compounds,Handan University,Handan 056006,Hebei,China)
机构地区:[1]天津工业大学省部共建分离膜与膜过程国家重点实验室,天津300387 [2]天津工业大学纺织科学与工程学院,天津300387 [3]天津工业大学化学工程与技术学院,天津300387 [4]天津工业大学物理科学与技术学院,天津300387 [5]天津工业大学材料科学与工程学院,天津300387 [6]邯郸学院,河北省杂环化合物重点实验室,河北邯郸056006
出 处:《硅酸盐学报》2024年第8期2545-2552,共8页Journal of The Chinese Ceramic Society
基 金:河北省科技计划(22373709D);河北省高等学校科学研究项目(BJK2024029)。
摘 要:金属–有机骨架(MOF)材料因其较高的比表面积、丰富的化学官能团、可调的孔隙结构和良好的热化学稳定性而可作为膜材料备受关注。本工作利用液体辅助球磨法合成了沸石型咪唑酯骨架材料(ZIF-62),通过对压制的ZIF-62薄片进行热处理,得到了具有良好气体分离性能的自支撑ZIF-62玻璃膜。结果表明,热处理过程未改变ZIF-62晶体的化学键和配体组成,实现了ZIF-62晶体从晶态到无定形玻璃态的转化。通过改变ZIF-62粉末的添加量,可以得到不同厚度的自支撑ZIF-62玻璃膜,随着厚度的不断降低,制备的ZIF-62玻璃膜的CO_(2)渗透速率不断增加,CO_(2)/CH_(4)分离选择性不断降低。此外,在48 h的连续测试过程中,ZIF-62玻璃膜的气体分离性能依旧保持良好的稳定性。本工作对MOF材料在膜气体分离领域中的应用具有参考意义。Introduction MOF gas separation membranes have attracted much attention due to the large BET surface area,flexible functional groups,adjustable structure,and good thermo-chemical stability,which can significantly improve the separation efficiency and purity of the gas separation process.However,MOF gas separation membranes have unavoidable grain boundaries and are prone to non-selective defects,which greatly destroys the intrinsic separation properties of pure MOF materials,posing a serious of challenges during the preparation and application.MOF glass membranes is an emerging type of gas separation membrane with the advantages of easy processing,no grain boundary defects and permanent porosity,and have become a new access for the preparation of high-performance gas separation membranes.However,the typical MOF glass membranes are normally formed on support layers,and the presence of the supporting layers greatly limits the processability and gas permeability enhancement.In this work,a novel preparation method of self-supported MOF glass membranes is proposed,and a serious of self-supported ZIF-62 glass membranes performing excellent CO_(2)/CH_(4) gas separation property are obtained.Methods In the present work,ZIF-62 crystals were prepared according to the previous literature.Zinc hydroxide,zinc acetate dihydrate(purity 99%,manufacturers are Shanghai Aladdin Biochemistry Science and Technology Co.,Ltd.),imidazole(purity 99.5%,manufacturers are Anhui Zesheng Science and Technology Co.,Ltd.),benzimidazole(purity 96%manufacturers are Shanghai McLean Biochemistry Science and Technology Co.,Ltd.),N,N-N,N-dimethylformamide(purity of analytical purity,the manufacturers are Sinopharm Chemical Reagent Co.,Ltd.),etc were used.Then,the ZIF-62 crystals were pressed to thin pellets in specific molds,and were heat-treated by a preset heating procedure,so as to prepare the homogeneous and dense self-supported amorphous ZIF-62 glass(a_(g)ZIF-62)membranes.The difference of the properties between ZIF-62 crystals and a_(g)ZIF-62 me
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