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

Accepted version
Peer-reviewed

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Type

Article

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Authors

Gao, Lijun 
Herou, Servann JA 
Griffiths, James T 

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).

Description

Keywords

0302 Inorganic Chemistry, 0303 Macromolecular and Materials Chemistry

Journal Title

Nat Commun

Conference Name

Journal ISSN

2041-1723
2041-1723

Volume Title

10

Publisher

Springer Science and Business Media LLC
Sponsorship
Engineering and Physical Sciences Research Council (EP/N004272/1)
EPSRC (1566990)
European Research Council (280078)
Engineering and Physical Sciences Research Council (EP/L011700/1)
Engineering and Physical Sciences Research Council (EP/L015889/1)
EPSRC Centre for Doctoral Training in Sensor Technologies and Applications (EP/L015889/1); EPSRC Centre for Doctoral Training in Sensor Technologies and Applications (1566990); EPSRC grants (EP/L011700/1); EPSRC grants (EP/N004272/1); Isaac Newton Trust [Minute 13.38(k)]; European Research Council (ERC) EMATTER (# 280078); National Natural Science Foundation of China (No. 21688102); National Natural Science Foundation of China (No. 21825203); Ministry of Science and Technology of China (No. 2016YFA0200200); Strategic Priority Research Program of the Chinese Academy of Sciences (No. XDB17020000); Ras Al Khaimah Center for Advanced Materials (RAK-CAM); China Scholarship Council (CSC);