化学
亚稳态
溶剂
多米诺骨牌
金属
金属有机骨架
羧酸盐
化学物理
多孔性
结晶学
光化学
物理化学
催化作用
立体化学
有机化学
吸附
作者
Sheng-Han Lo,Liang Feng,Kui Tan,Zhehao Huang,Shuai Yuan,Kunyu Wang,Bing-Han Li,Wan‐Ling Liu,Gregory S. Day,Songsheng Tao,Chun‐Chuen Yang,Tzuoo-Tsair Luo,Chia‐Her Lin,Sue‐Lein Wang,Simon J. L. Billinge,Kuang‐Lieh Lu,Yves J. Chabal,Xiaodong Zou,Hong‐Cai Zhou
出处
期刊:Nature Chemistry
[Springer Nature]
日期:2019-12-02
卷期号:12 (1): 90-97
被引量:107
标识
DOI:10.1038/s41557-019-0364-0
摘要
Topological transitions between considerably different phases typically require harsh conditions to collectively break chemical bonds and overcome the stress caused to the original structure by altering its correlated bond environment. In this work we present a case system that can achieve rapid rearrangement of the whole lattice of a metal–organic framework through a domino alteration of the bond connectivity under mild conditions. The system transforms from a disordered metal–organic framework with low porosity to a highly porous and crystalline isomer within 40 s following activation (solvent exchange and desolvation), resulting in a substantial increase in surface area from 725 to 2,749 m2 g–1. Spectroscopic measurements show that this counter-intuitive lattice rearrangement involves a metastable intermediate that results from solvent removal on coordinatively unsaturated metal sites. This disordered–crystalline switch between two topological distinct metal–organic frameworks is shown to be reversible over four cycles through activation and reimmersion in polar solvents. A disordered metal–organic framework converts into a more porous, crystalline phase within 40 s following solvent exchange and desolvation. The rapid domino rearrangement of the whole lattice, which involves carboxylate migration on coordinatively unsaturated metal sites, is accompanied by a substantial increase in surface area.
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