摘要
本研究揭示了一种新型的合成方法——超声法在快速合成阴离子型金属有机框架(MOF)材料方面的应用。采用扩散法制备了一种新型的阴离子型MOF材料:CuTaOF_(5)-bpy(其中,bpy为4,4-联吡啶)的单晶,并利用超声法在15min内快速合成了粉末样品。X-射线单晶衍射结果显示,该材料为4,4-联吡啶、Cu^(2+)和阴离子TaOF_(5)^(2-)自组装而成的阴离子柱撑型微孔MOF材料。通过超声快速合成法制备的粉末样品与单晶具有一致的晶体结构,且具有优异的结晶性。随着超声时间的延长,样品的结晶性呈现出先增强后减弱的趋势,在15min时具有最高的结晶性。气体吸附结果表明,超声快速合成法合成的样品与单晶样品具有相近的CO_(2)吸附性能。巨正则蒙特卡洛(GCMC)模拟结果显示,阴离子TaOF_(5)^(2-)为CO_(2)的优先吸附位点,说明阴离子的引入有利于增强MOF材料对CO_(2)的吸附能力。
This study revealed the application of ultrasonic method in the rapid preparation of anionic metal-organic frameworks(MOFs).The single-crystal of a new type of anionic metal organic framework:CuTaOF_(5)-bpy(in which,bpy is 4,4-bipyridine)was prepared by diffusion method,and the powder-like sample was prepared through an ultrasonic method in 15 minutes.Single-crystal X-ray diffraction revealed that this MOF is a microporous anionic three-dimensional MOF self-assembled by 4,4-bipyridine,Cu^(2+) and anion TaOF_(5)^(2-).And the powder sample prepared by the ultrasonic method possess the same crystal structure with the single crystal and excellent crystallinity.When prolonging the ultrasonic time,the crystallinity of the sample showed a tendency to increase first and then decrease,with the highest crystallinity at 15 minutes.CO_(2)adsorption experiments show that the sample synthesized by the ultrasonic method has the same pore structure as well as the similar CO_(2)adsorption performance with the single crystal sample.Grand canonical Monte Carlo(GCMC)simulation results show that the TaOF_(5)^(2-)anions are the preferential adsorption site for CO_(2),indicating that the introduction of anions is beneficial to enhance the CO_(2)adsorption in MOFs.
作者
张付昭
许文莉
李良军
赵学波
张奎同
邢涛
Zhang Fuzhao;Xu Wenli;Li Liangjun;Zhao Xuebo;Zhang Kuitong;Xing Tao(College of New Energy,China University of Petroleum(East China),Shandong,266580;Shandong Energy Group Co.,Ltd.,Shandong,250014)
出处
《当代化工研究》
2022年第20期55-57,共3页
Modern Chemical Research
基金
山东省重大科技创新工程项目“氢能技术-工业副产氢能利用与纯化技术研究与应用”(项目编号:2020CXGC010402)
山东省自然科学基金项目“基于MOF的仿生分级超结构的构筑及气体分离性能的研究”(项目编号:ZR2021MB084)。
关键词
金属-有机框架材料
阴离子柱撑体
超声合成
二氧化碳捕获
蒙特卡洛模拟
metal-organic frameworks
anions-pillared framework
ultrasonic synthesis method
carbon dioxide capture
Monte-Carlo simulations
