Volume 64, Issue 28 e202423471
Research Article

Dopant and Exfoliation Induced Simultaneous Modification of Charge Density and C─C Coupling Sites for Efficient CO2 Photoreduction to Ethylene

Dr. Kousik Das

Dr. Kousik Das

New Chemistry Unit, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur, Bangalore, 560064 India

School of Advanced Materials, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur, Bangalore, 560064 India

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Subhajit Chakraborty

Subhajit Chakraborty

New Chemistry Unit, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur, Bangalore, 560064 India

School of Advanced Materials, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur, Bangalore, 560064 India

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Dr. Siddhi Kediya

Dr. Siddhi Kediya

New Chemistry Unit, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur, Bangalore, 560064 India

School of Advanced Materials, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur, Bangalore, 560064 India

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Dr. Ashutosh Kumar Singh

Dr. Ashutosh Kumar Singh

School of Advanced Materials, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur, Bangalore, 560064 India

Chemistry and Physics of Materials Unit, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur, Bangalore, 560064 India

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Dr. Risov Das

Dr. Risov Das

New Chemistry Unit, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur, Bangalore, 560064 India

School of Advanced Materials, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur, Bangalore, 560064 India

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Dr. Soumi Mondal

Dr. Soumi Mondal

New Chemistry Unit, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur, Bangalore, 560064 India

School of Advanced Materials, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur, Bangalore, 560064 India

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Dr. Mohd Riyaz

Dr. Mohd Riyaz

New Chemistry Unit, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur, Bangalore, 560064 India

School of Advanced Materials, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur, Bangalore, 560064 India

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Dr. Devender Goud

Dr. Devender Goud

New Chemistry Unit, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur, Bangalore, 560064 India

School of Advanced Materials, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur, Bangalore, 560064 India

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Nilutpal Dutta

Nilutpal Dutta

New Chemistry Unit, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur, Bangalore, 560064 India

School of Advanced Materials, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur, Bangalore, 560064 India

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Dr. Chathakudath P. Vinod

Dr. Chathakudath P. Vinod

Catalysis and Inorganic Chemistry Division, CSIR-National Chemical Laboratory, Dr. Homi Bhabha Road, Pune, 410008 India

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Prof. Dr. Sebastian C. Peter

Corresponding Author

Prof. Dr. Sebastian C. Peter

New Chemistry Unit, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur, Bangalore, 560064 India

School of Advanced Materials, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur, Bangalore, 560064 India

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

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First published: 05 May 2025

Graphical Abstract

The photocatalytic conversion of CO2 into higher carbon products demands precise catalyst engineering. In this study, we implemented a dual doping strategy in AgBiP₂S₆ to optimize charge density and enhance active sites for C─C coupling. This approach successfully enabled the synthesis of ethylene through the photoreduction of CO2, showcasing the effectiveness of the modified catalyst design.

Abstract

The photochemical conversion of CO2 into C2+ products has emerged as an attractive method for synthesizing valuable chemicals and fuels using abundant solar energy. However, the challenge lies in enhancing the efficiency and selectivity of C2+ product formation. In this study, we employed a heteroatom doping strategy to optimize the photocatalytic parameters and achieve excellent efficiency and selectivity in the photocatalytic CO2 reduction to C2+ product formation. Our experimental analysis revealed that the local electronic structure of the catalyst, modified by In-doping, enables enhanced efficiency. Additionally, the incorporation of Cu facilitates the coupling of C1 intermediates, resulting in excellent selectivity towards C2+ products. The CO2 reduction performance is further enhanced through exfoliation, which increases the exposure of active sites and extends the charge carrier lifetime by reducing the charge diffusion length. We report that the rate of formation of C2H4 reached 54.3 µmol·h−1·g−1 with an outstanding selectivity of 91% over the exfoliated CuIn-doped AgBiP2S6 catalyst. By elucidating the role of heteroatom doping and exfoliation in enhancing both the efficiency and selectivity of C2+ product formation, our study contributes to advancing the development of sustainable and efficient photocatalytic CO2 conversion 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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