Rational approach to guest confinement inside MOF cavities for low-temperature catalysis.
Herou, Servann JA
Griffiths, James T
Smoukov, Stoyan K
Nature Publishing Group
MetadataShow full item record
Wang, T., Gao, L., Hou, J., Herou, S. J., Griffiths, J. T., Li, W., Dong, J., et al. (2019). Rational approach to guest confinement inside MOF cavities for low-temperature catalysis.. Nature communications, 10 (1), 1340. https://doi.org/10.1038/s41467-019-08972-x
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 (RuO₂@MOF-808-P) 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).
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);
European Research Council (280078)
Embargo Lift Date
External DOI: https://doi.org/10.1038/s41467-019-08972-x
This record's URL: https://www.repository.cam.ac.uk/handle/1810/289327