Volume 137, Issue 30 e202505244
Forschungsartikel

Tailoring Oxygen Vacancies with Atomically Dispersed Cu Sites for Stable and Efficient Photothermal CO2 Conversion

Xueying Wan

Xueying Wan

School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui, 230026 China

State Key Laboratory of Bioinspired Interfacial Materials Science, Sustainable Energy and Environmental Materials Innovation Center, School of Nano Science and Technology, Suzhou Institute for Advanced Research, University of Science and Technology of China, Suzhou, Jiangsu, 215123 China

These authors contributed equally to this work.

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Yilin Zhao

Yilin Zhao

School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui, 230026 China

State Key Laboratory of Bioinspired Interfacial Materials Science, Sustainable Energy and Environmental Materials Innovation Center, School of Nano Science and Technology, Suzhou Institute for Advanced Research, University of Science and Technology of China, Suzhou, Jiangsu, 215123 China

These authors contributed equally to this work.

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Yifan Li

Corresponding Author

Yifan Li

Vacuum Interconnected Nanotech Workstation, Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences, Suzhou, 215123 China

These authors contributed equally to this work.

E-mail: [email protected], [email protected], [email protected]

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Jun Ma

Jun Ma

School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui, 230026 China

State Key Laboratory of Bioinspired Interfacial Materials Science, Sustainable Energy and Environmental Materials Innovation Center, School of Nano Science and Technology, Suzhou Institute for Advanced Research, University of Science and Technology of China, Suzhou, Jiangsu, 215123 China

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Yadi Gu

Yadi Gu

School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui, 230026 China

State Key Laboratory of Bioinspired Interfacial Materials Science, Sustainable Energy and Environmental Materials Innovation Center, School of Nano Science and Technology, Suzhou Institute for Advanced Research, University of Science and Technology of China, Suzhou, Jiangsu, 215123 China

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Caiyi Liu

Caiyi Liu

School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui, 230026 China

State Key Laboratory of Bioinspired Interfacial Materials Science, Sustainable Energy and Environmental Materials Innovation Center, School of Nano Science and Technology, Suzhou Institute for Advanced Research, University of Science and Technology of China, Suzhou, Jiangsu, 215123 China

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Yan Luo

Yan Luo

School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui, 230026 China

State Key Laboratory of Bioinspired Interfacial Materials Science, Sustainable Energy and Environmental Materials Innovation Center, School of Nano Science and Technology, Suzhou Institute for Advanced Research, University of Science and Technology of China, Suzhou, Jiangsu, 215123 China

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Guang Yang

Guang Yang

Vacuum Interconnected Nanotech Workstation, Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences, Suzhou, 215123 China

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Yi Cui

Yi Cui

Vacuum Interconnected Nanotech Workstation, Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences, Suzhou, 215123 China

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Dong Liu

Corresponding Author

Dong Liu

School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui, 230026 China

State Key Laboratory of Bioinspired Interfacial Materials Science, Sustainable Energy and Environmental Materials Innovation Center, School of Nano Science and Technology, Suzhou Institute for Advanced Research, University of Science and Technology of China, Suzhou, Jiangsu, 215123 China

E-mail: [email protected], [email protected], [email protected]

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Yujie Xiong

Corresponding Author

Yujie Xiong

School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui, 230026 China

State Key Laboratory of Bioinspired Interfacial Materials Science, Sustainable Energy and Environmental Materials Innovation Center, School of Nano Science and Technology, Suzhou Institute for Advanced Research, University of Science and Technology of China, Suzhou, Jiangsu, 215123 China

E-mail: [email protected], [email protected], [email protected]

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First published: 15 April 2025

Abstract

Photothermal catalysis under mild conditions represents a promising and sustainable approach for CO2 conversion into high-value chemicals, thereby enabling efficient carbon recycling. However, precise manipulation of active sites and their coordination environments at the atomic level to enhance catalyst performance still remains a challenge. Here, we present a single-atom doping strategy for oxygen vacancy engineering to facilitate efficient CO2 conversion. Specifically, an In2O3-based catalyst with abundant oxygen vacancies induced by homogeneously dispersed Cu single atoms is constructed, exhibiting a competent CO2 reduction performance in photothermal reverse water-gas shift reaction. The optimal Cu-In2O3 catalyst achieves a CO yield rate of 46.17 mol gCu−1 h−1 with near-unity selectivity (>99%) and demonstrates stability over 450 h under 3 W cm−2 full-spectrum light illumination. Comprehensive spectroscopic characterization and computational simulations elucidate that the Cu single atoms synergistically interact with oxygen vacancies to promote H2 dissociation and CO2 activation under photoexcitation. This work provides insights into the design of photothermal catalysts, emphasizing the transformative potential of atomic-site engineering for efficient CO2 conversion and sustainable energy technologies.

Conflict of Interests

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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