Metal-organic framework membranes with single-atomic centers for photocatalytic CO2 and O2 reduction

Yu-Chen Hao, Li-Wei Chen, Jiani Li, Yu Guo, Xin Su, Miao Shu, Qinghua Zhang, Wen-Yan Gao, Siwu Li, Zi-Long Yu, Lin Gu, Xiao Feng, An-Xiang Yin (), Rui Si (), Ya-Wen Zhang, Bo Wang () and Chun-Hua Yan
Additional contact information
Yu-Chen Hao: Beijing Institute of Technology
Li-Wei Chen: Beijing Institute of Technology
Jiani Li: Beijing Institute of Technology
Yu Guo: Peking University
Xin Su: Beijing Institute of Technology
Miao Shu: Chinese Academy of Sciences
Qinghua Zhang: Chinese Academy of Sciences
Wen-Yan Gao: Beijing Institute of Technology
Siwu Li: Beijing Institute of Technology
Zi-Long Yu: Beijing Institute of Technology
Lin Gu: Chinese Academy of Sciences
Xiao Feng: Beijing Institute of Technology
An-Xiang Yin: Beijing Institute of Technology
Rui Si: Chinese Academy of Sciences
Ya-Wen Zhang: Peking University
Bo Wang: Beijing Institute of Technology
Chun-Hua Yan: Peking University

Nature Communications, 2021, vol. 12, issue 1, 1-11

Abstract: Abstract The demand for sustainable energy has motivated the development of artificial photosynthesis. Yet the catalyst and reaction interface designs for directly fixing permanent gases (e.g. CO2, O2, N2) into liquid fuels are still challenged by slow mass transfer and sluggish catalytic kinetics at the gas-liquid-solid boundary. Here, we report that gas-permeable metal-organic framework (MOF) membranes can modify the electronic structures and catalytic properties of metal single-atoms (SAs) to promote the diffusion, activation, and reduction of gas molecules (e.g. CO2, O2) and produce liquid fuels under visible light and mild conditions. With Ir SAs as active centers, the defect-engineered MOF (e.g. activated NH2-UiO-66) particles can reduce CO2 to HCOOH with an apparent quantum efficiency (AQE) of 2.51% at 420 nm on the gas-liquid-solid reaction interface. With promoted gas diffusion at the porous gas-solid interfaces, the gas-permeable SA/MOF membranes can directly convert humid CO2 gas into HCOOH with a near-unity selectivity and a significantly increased AQE of 15.76% at 420 nm. A similar strategy can be applied to the photocatalytic O2-to-H2O2 conversions, suggesting the wide applicability of our catalyst and reaction interface designs.

Date: 2021
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DOI: 10.1038/s41467-021-22991-7

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