Efficient photocatalytic CO2 reduction to CH4 via electric field-regulated d-band center on Ga2S3/CuS S-type heterojunction interface structures

Sun, Yuxin; Lai, Kezhen; Li, Ning; Gao, Yangqin; Ge, Lei

doi:10.1016/j.apcatb.2024.124302

Applied Catalysis B: Environment and Energy

2024

DOI: 10.1016/j.apcatb.2024.124302

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Efficient photocatalytic CO2 reduction to CH4 via electric field-regulated d-band center on Ga2S3/CuS S-type heterojunction interface structures

Yuxin Sun,

Kezhen Lai,

Ning Li

et al.

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Cited by 14 publications

References 62 publications

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Photocatalytic CO₂‐to‐CH₄ Conversion with Ultrahigh Selectivity of 95.93% on S‐Vacancy Modulated Spatial In₂S₃/In₂O₃ Heterojunction

Lai,

Sun,

et al. 2024

Adv Funct Materials

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Photocatalytic conversion of CO2 to methane faces challenges due to the stability of CO2, unpredictable intermediates, and complex electron transfer steps. Herein, a spatial In2S3/In2O3 heterojunction with abundant S vacancies (ISIO(VS)) is obtained through facile Polyvinylpyrrolidone (PVP) treatment to reach a methane yield of 16.52 µmol·g−1·h−1 with a selectivity of 95.93%, which is the highest among reported In2S3 and In2O3 based catalysts. The work function (Wf), differential charge density, and Kelvin Probe Force Microscopy (KPFM) results confirm that S vacancies strengthen the built‐in electric field (BEF) of In2S3/In2O3 (ISIO) heterojunctions, improving carrier separation. Density functional theory (DFT) calculations reveal that S vacancies induce electron redistribution, facilitating adsorption and activation of CO2 and *CO intermediate, thus promoting hydrogenation to yield *CHO. The reaction pathway of photocatalytic CO2 reduction is revealed by in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and Gibbs free energy (ΔG). The S vacancies modify electronic orbitals and the highest occupied molecular orbital (HOMO) of In atom, resulting in a stronger interaction between the catalyst and *CHO, which reduces ΔG*CHO and regulates the selectivity of CH4. This study paves a new avenue for the design of photocatalysts with highly selective reduction of CO2 to CH4 through defect engineering.

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Photocatalytic CO₂‐to‐CH₄ Conversion with Ultrahigh Selectivity of 95.93% on S‐Vacancy Modulated Spatial In₂S₃/In₂O₃ Heterojunction

Lai,

Sun,

et al. 2024

Adv Funct Materials

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Controlling Carrier Separation by Ag2S Decoration on P-CdS Nanorods for Enhanced Photocatalytic Hydrogen Evolution

Yang,

2024

Catal Lett

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Regulating metal cation Cu vacancies on ZnIn2S4/Cu1.81S to achieve high selectivity for the photocatalytic reduction of CO2 to CH4

Sun,

Lai,

Shi

et al. 2025

Applied Catalysis B: Environment and Energy

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Efficient photocatalytic CO2 reduction to CH4 via electric field-regulated d-band center on Ga2S3/CuS S-type heterojunction interface structures

Cited by 14 publications

References 62 publications

Photocatalytic CO₂‐to‐CH₄ Conversion with Ultrahigh Selectivity of 95.93% on S‐Vacancy Modulated Spatial In₂S₃/In₂O₃ Heterojunction

Photocatalytic CO₂‐to‐CH₄ Conversion with Ultrahigh Selectivity of 95.93% on S‐Vacancy Modulated Spatial In₂S₃/In₂O₃ Heterojunction

Controlling Carrier Separation by Ag2S Decoration on P-CdS Nanorods for Enhanced Photocatalytic Hydrogen Evolution

Regulating metal cation Cu vacancies on ZnIn2S4/Cu1.81S to achieve high selectivity for the photocatalytic reduction of CO2 to CH4

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Efficient photocatalytic CO2 reduction to CH4 via electric field-regulated d-band center on Ga2S3/CuS S-type heterojunction interface structures

Cited by 14 publications

References 62 publications

Photocatalytic CO2‐to‐CH4 Conversion with Ultrahigh Selectivity of 95.93% on S‐Vacancy Modulated Spatial In2S3/In2O3 Heterojunction

Photocatalytic CO2‐to‐CH4 Conversion with Ultrahigh Selectivity of 95.93% on S‐Vacancy Modulated Spatial In2S3/In2O3 Heterojunction

Controlling Carrier Separation by Ag2S Decoration on P-CdS Nanorods for Enhanced Photocatalytic Hydrogen Evolution

Regulating metal cation Cu vacancies on ZnIn2S4/Cu1.81S to achieve high selectivity for the photocatalytic reduction of CO2 to CH4

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Product

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About

Photocatalytic CO₂‐to‐CH₄ Conversion with Ultrahigh Selectivity of 95.93% on S‐Vacancy Modulated Spatial In₂S₃/In₂O₃ Heterojunction

Photocatalytic CO₂‐to‐CH₄ Conversion with Ultrahigh Selectivity of 95.93% on S‐Vacancy Modulated Spatial In₂S₃/In₂O₃ Heterojunction