Rational approach to guest confinement inside MOF cavities for low-temperature catalysis

Tiesheng Wang, Lijun Gao, Jingwei Hou, Servann J. A. Herou, James T. Griffiths, Weiwei Li, Jinhu Dong, Song Gao, Maria-Magdalena Titirici, R. Vasant Kumar, Anthony K. Cheetham, Xinhe Bao, Qiang Fu () and Stoyan K. Smoukov ()
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Tiesheng Wang: University of Cambridge
Lijun Gao: Chinese Academy of Sciences
Jingwei Hou: University of Cambridge
Servann J. A. Herou: Queen Mary University of London
James T. Griffiths: University of Cambridge
Weiwei Li: University of Cambridge
Jinhu Dong: Chinese Academy of Sciences
Song Gao: The University of New South Wales
Maria-Magdalena Titirici: Queen Mary University of London
R. Vasant Kumar: University of Cambridge
Anthony K. Cheetham: University of Cambridge
Xinhe Bao: Chinese Academy of Sciences
Qiang Fu: Chinese Academy of Sciences
Stoyan K. Smoukov: University of Cambridge

Nature Communications, 2019, vol. 10, issue 1, 1-9

Abstract: Abstract Geometric or electronic confinement of guests inside nanoporous hosts promises to deliver unusual catalytic or opto-electronic functionality from existing materials but is challenging to obtain particularly using metastable hosts, such as metal–organic frameworks (MOFs). Reagents (e.g. precursor) may be too large for impregnation and synthesis conditions may also destroy the hosts. Here we use thermodynamic Pourbaix diagrams (favorable redox and pH conditions) to describe a general method for metal-compound guest synthesis by rationally selecting reaction agents and conditions. Specifically we demonstrate a MOF-confined RuO2 catalyst (RuO2@MOF-808-P) with exceptionally high catalytic CO oxidation below 150 °C as compared to the conventionally made SiO2-supported RuO2 (RuO2/SiO2). This can be caused by weaker interactions between CO/O and the MOF-encapsulated RuO2 surface thus avoiding adsorption-induced catalytic surface passivation. We further describe applications of the Pourbaix-enabled guest synthesis (PEGS) strategy with tutorial examples for the general synthesis of arbitrary guests (e.g. metals, oxides, hydroxides, sulfides).

Date: 2019
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DOI: 10.1038/s41467-019-08972-x

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