沸石咪唑盐骨架
材料科学
金属有机骨架
微型多孔材料
无定形固体
咪唑酯
环境压力
多形性
猝灭(荧光)
拉曼光谱
相图
化学工程
多孔性
化学物理
软化
相(物质)
热力学
结晶学
物理化学
吸附
化学
复合材料
有机化学
工程类
物理
光学
荧光
量子力学
作者
Remo N. Widmer,Giulio I. Lampronti,Simone Anzellini,Romain Gaillac,Stefan Farsang,Chao Zhou,Ana M. Belenguer,Craig Wilson,H.K. Palmer,Annette K. Kleppe,Michael T. Wharmby,Xia Yu,Seth M. Cohen,Shane G. Telfer,Simon A. T. Redfern,François‐Xavier Coudert,Simon MacLeod,Thomas D. Bennett
出处
期刊:Nature Materials
[Springer Nature]
日期:2019-03-18
卷期号:18 (4): 370-376
被引量:121
标识
DOI:10.1038/s41563-019-0317-4
摘要
Metal-organic frameworks (MOFs) are microporous materials with huge potential for chemical processes. Structural collapse at high pressure, and transitions to liquid states at high temperature, have recently been observed in the zeolitic imidazolate framework (ZIF) family of MOFs. Here, we show that simultaneous high-pressure and high-temperature conditions result in complex behaviour in ZIF-62 and ZIF-4, with distinct high- and low-density amorphous phases occurring over different regions of the pressure-temperature phase diagram. In situ powder X-ray diffraction, Raman spectroscopy and optical microscopy reveal that the stability of the liquid MOF state expands substantially towards lower temperatures at intermediate, industrially achievable pressures and first-principles molecular dynamics show that softening of the framework coordination with pressure makes melting thermodynamically easier. Furthermore, the MOF glass formed by melt quenching the high-temperature liquid possesses permanent, accessible porosity. Our results thus imply a route to the synthesis of functional MOF glasses at low temperatures, avoiding decomposition on heating at ambient pressure.
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