Structure and Synthesizability of Iron-Sulfur Metal-Organic Frameworks

被引:0
作者
Mao, Jianming [1 ]
Jiang, Ningxin [1 ]
Daru, Andrea [1 ]
Filatov, Alexander S. [1 ]
Burch, Jessica E. [2 ]
Hofmann, Jan [3 ]
Vornholt, Simon M. [3 ]
Chapman, Karena W. [3 ]
Anderson, John S. [1 ]
Ferguson, Andrew L. [1 ,4 ]
机构
[1] Univ Chicago, Dept Chem, Chicago, IL 60637 USA
[2] Rigaku Amer Corp, The Woodlands, TX 77381 USA
[3] SUNY Stony Brook, Dept Chem, Stony Brook, NY 11794 USA
[4] Univ Chicago, Pritzker Sch Mol Engn, Chicago, IL 60637 USA
基金
美国国家科学基金会;
关键词
LIGAND FUNCTIONALIZATION; THERMODYNAMIC STABILITY; METHANE STORAGE; ATOMIC CHARGES; FORCE-FIELD; ADSORPTION; MOFS; CRYSTAL; DESIGN; ALGORITHMS;
D O I
10.1021/jacs.4c16341
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Sulfur-based metal-organic frameworks (MOFs) and coordination polymers (CPs) are an emerging class of hybrid materials that have received growing attention due to their magnetic, conductive, and catalytic properties with potential applications in electrocatalysis and energy storage. In this work, we report a high-throughput virtual screening protocol to predict the synthesizability of candidate metal-sulfur MOFs/CPs by computing the thermodynamically stable structures resulting from a particular combination of metal cluster, linker, cation, and synthetic conditions. Free energies are computed by using all-atom classical mechanical thermodynamic integration. Low-free-energy structures are refined using ab initio density functional theory, and pair distribution functions and powder X-ray diffraction patterns are calculated to complement and guide experimental structure determination. We validate the computational approach by retrospective predictions of the stable structure produced by experimental syntheses, and a subsequent screen predicts Fe4S4-BDT-TPP as a new thermodynamically stable one-dimensional (1D) CP comprising a redox-active Fe4S4 cluster, a 1,4-benzenedithiolate (BDT) linker, and a tetraphenylphosphonium (TPP) countercation. This material is experimentally synthesized, and the 1D chain structure of the crystal is confirmed using microcrystal electron diffraction. The computational screening pipeline is generically transferable to neutral and ionic MOFs/CPs comprising arbitrary metal clusters, linkers, cations, and synthetic conditions, and we make it freely available as an open source tool to guide and accelerate the discovery and engineering of novel porous materials.
引用
收藏
页码:17651 / 17667
页数:17
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