Volume 64, Issue 24 e202505668
Communication

Boron Doping-Induced Ultrahigh Ce3+ Ratio in Amorphous CeO2/GO Catalyst for Low-Concentration CO2 Photoreduction

Yanhong Li

Yanhong Li

School of Chemistry, Key Laboratory of Bio-Inspired Smart Interfacial Science and Technology, Beihang University, Beijing, 100191 China

These authors contributed equally to this work.

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Qian Yin

Qian Yin

School of Physics, Beihang University, Beijing, 100191 China

These authors contributed equally to this work.

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Binbin Jia

Binbin Jia

School of Materials and Chemical Engineering, Key Laboratory of Inorganic Nonmetallic Crystalline and Energy Conversion Materials, China Three Gorges University, Yichang, 443002 China

These authors contributed equally to this work.

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Huiqing Wang

Huiqing Wang

School of Materials and Chemical Engineering, Key Laboratory of Inorganic Nonmetallic Crystalline and Energy Conversion Materials, China Three Gorges University, Yichang, 443002 China

These authors contributed equally to this work.

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Hongfei Gu

Hongfei Gu

School of Chemistry, Key Laboratory of Bio-Inspired Smart Interfacial Science and Technology, Beihang University, Beijing, 100191 China

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Qi Hu

Qi Hu

School of Physics, Beihang University, Beijing, 100191 China

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Haosen Yang

Haosen Yang

School of Chemistry, Key Laboratory of Bio-Inspired Smart Interfacial Science and Technology, Beihang University, Beijing, 100191 China

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Tianqi Guo

Corresponding Author

Tianqi Guo

International Institute for Interdisciplinary and Frontiers, Beihang University, Beijing, 100191 China

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

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Pengfei Hu

Corresponding Author

Pengfei Hu

School of Chemistry, Key Laboratory of Bio-Inspired Smart Interfacial Science and Technology, Beihang University, Beijing, 100191 China

Research Institute of Aero-Engine, Beihang University, Beijing, 100191 China

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

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Lidong Li

Corresponding Author

Lidong Li

School of Chemistry, Key Laboratory of Bio-Inspired Smart Interfacial Science and Technology, Beihang University, Beijing, 100191 China

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

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Li-Min Liu

Corresponding Author

Li-Min Liu

School of Physics, Beihang University, Beijing, 100191 China

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

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Lin Guo

Corresponding Author

Lin Guo

School of Chemistry, Key Laboratory of Bio-Inspired Smart Interfacial Science and Technology, Beihang University, Beijing, 100191 China

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

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First published: 08 April 2025

Graphical Abstract

This study introduces a novel strategy to synthesize amorphous CeO2/GO with an exceptionally high Ce3+ ratio of 85.7% through B-doping. The resulting amorphous structure reduces the band gap, enhances charge separation efficiency, and significantly boosts diluted CO2 photocatalytic activity. The material achieves remarkable CO2-to-CO conversion rates of 249.33 µmol g−1 h−1(under 15% CO2) and 103.4 µmol g−1 h−1(under 1% CO2) with 100% selectivity, highlighting its potential for sustainable CO2 conversion.

Abstract

Direct utilization of diluted CO2 enables sustainable CO2 conversion into valuable products, with reduced CeO2 emerging as an attractive candidate due to its exceptional redox flexibility. The catalytic efficacy of CeO2 is intimately tied to the electronic structure of 4f, yet the persistent challenge lies in maintaining a high and stable concentration of Ce3+. In this study, we propose a symmetry-breaking-induced amorphization strategy to achieve an exceptionally high Ce3+ ratio by B doping, which facilitates the reduction of Ce4+ to Ce3+ in amorphous CeO2. First-principles calculations and infrared spectroscopy reveal that B doping with three excess electrons induces the formation of planar triangular B–O₃ units by disrupting the original high-symmetry structure of CeO2, facilitating the spontaneous transition to the amorphous phase. Electronic structure analysis confirms that even a modest 7.5% B doping can significantly elevate the Ce3+ ratio to 85.7%. The resulting amorphous B-doped CeO2/GO shows a remarkable CO2-to-CO conversion rate of 249.33 µmol g−1 h−1(under 15% CO2) and 103.4 µmol g−1 h−1(under 1% CO2), with 100% selectivity in both cases. This performance highlights how amorphization stabilizes defect states, making amorphous CeO2/GO with high Ce3+ an effective material for CO2 photoreduction and addressing key challenges in CO2 capture and utilization.

Conflict of Interests

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available in the supplementary material of this article.

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