4.6 Article

CuSx-mediated two reaction systems enable biomimetic photocatalysis in CO2 reduction with visible light

Journal

JOURNAL OF ENERGY CHEMISTRY
Volume 65, Issue -, Pages 497-504

Publisher

ELSEVIER
DOI: 10.1016/j.jechem.2021.06.003

Keywords

CO2; Photoreduction; Bifunctional catalyst; Proton-coupled electron transfer

Funding

  1. National Key Research and Development Program of China [2018YFD1000806-01]
  2. National Natural Science Foundation of China [21822203, 21932006]
  3. Natural Science Foundation of Zhejiang Province [LR18B030002]
  4. China Postdoctoral Science Foundation [2020M671020]

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The catalytic performance of heterogeneous catalysts can be effectively improved by optimizing the catalysts through appropriate structure design. Constructing a hybrid structure with Cu2S nanoparticles on amorphous CuSx matrix can enhance the catalysis of cuprous sulfide, leading to a significantly higher CO production rate in photocatalytic CO2 reduction under visible light irradiation. This enhancement is attributed to two reaction systems, involving light reaction on the heterojunctions of Cu2S nanoparticles and CuSx matrix for proton/electron production, and dark reaction on defect-rich CuSx for CO2 reduction.
The performances of heterogeneous catalysts can be effectively improved by optimizing the catalysts via appropriate structure design. Herein, we show that the catalysis of cuprous sulfide can be boosted by constructing the hybrid structure with Cu2S nanoparticles on amorphous CuSx matrix (Cu2S/CuSx). In the photocatalytic CO2 reduction under visible light irradiation, the Cu2S/CuSx exhibited a CO production rate at 4.0 mmol h(-1) that is 12-fold higher than that of the general Cu2S catalyst. Further characterizations reveal that the Cu2S/CuSx has two reaction systems that realize the biomimetic catalysis, involving in the light reaction on the Cu2S nanoparticle-CuSx matrix heterojunctions for proton/electron production, and the dark reaction on the defect-rich CuSx for CO2 reduction. The CuSx matrix could efficiently activate CO2 and stabilize the split hydrogen species to hinder undesired hydrogen evolution reaction, which benefits the proton-electron transfer to reduce CO2, a key step for bridging the two reaction systems. (C) 2021 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.

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