Citation: Yiting Huo, Xin Zhou, Feifan Zhao, Chenbin Ai, Zhen Wu, Zhidong Chang, Bicheng Zhu. Boosting photocatalytic CO₂ methanation through TiO₂/CdS S-scheme heterojunction and fs-TAS mechanism study[J]. Acta Physico-Chimica Sinica, ;2025, 41(11): 100148. doi: 10.1016/j.actphy.2025.100148 shu

Boosting photocatalytic CO₂ methanation through TiO₂/CdS S-scheme heterojunction and fs-TAS mechanism study

Yiting Huo ^{1, 2, 3} ,
Xin Zhou ² ,
Feifan Zhao ³ ,
Chenbin Ai ³ ,
Zhen Wu ² ,
Zhidong Chang ^1,, ,
Bicheng Zhu ^3,,

1.
School of Chemistry and Biological Engineering, University of Science and Technology Beijing, Beijing, 100083, China
2.
School of Chemical Engineering, Ordos Institute of Technology, Ordos, 017000, Inner Mongolia, China
3.
Laboratory of Solar Fuel, Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430078, Hubei Province, China

Corresponding author: Zhidong Chang, zdchang@ustb.edu.cn Bicheng Zhu, zhubicheng@cug.edu.cn
Received Date: 16 July 2025
Revised Date: 30 July 2025
Accepted Date: 3 August 2025

Fund Project: the National Natural Science Foundation of China 52173065the National Natural Science Foundation of China 22469001Natural Science Foundation of Inner Mongolia Autonomous Region of China 2025QN05107Natural Science Foundation of Inner Mongolia Autonomous Region of China 2025ZDLH002

The conversion of CO₂ into value-added hydrocarbons via photocatalysis holds great promise for sustainable energy, yet achieving high activity and selectivity remains challenging. Herein, a novel TiO₂/CdS heterostructured photocatalyst exhibits exceptional performance in CO₂ photoreduction. The optimized catalyst delivers a 4.2-fold increase in CH₄ production rate compared to pristine TiO₂, with a remarkable 65.4% selectivity toward CH₄ (34.6% CO). The enhanced activity arises from the unique morphology, facilitating CO₂ adsorption and mass transfer, and the intimate S-scheme heterojunction between CdS and TiO₂, which boosts charge separation while preserving strong redox potentials. Critically, femtosecond transient absorption spectroscopy (fs-TAS) combined with in situ DRIFTS provides direct evidence for the S-scheme pathway and identifies sulfur sites on CdS as key for stabilizing *CH₃O, *CHO and *CO intermediates, steering selectivity toward CH₄. In addition, theoretical calculations based on density functional theory (DFT) further complement the experimental findings. The calculations confirm the electronic structure characteristics of the S-scheme heterojunction, revealing the energy levels and charge transfer mechanisms at the atomic scale. This not only deepens our understanding of the photocatalytic process but also provides a theoretical basis for further optimizing the photocatalyst design. Overall, our work demonstrates the outstanding performance of the TiO₂/CdS heterostructured photocatalyst in CO₂ photoreduction.
- CO₂ photoreduction,
- Methane selectivity,
- fs-TAS,
- S-scheme heterojunction
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通讯作者: 陈斌, bchen63@163.com

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沈阳化工大学材料科学与工程学院沈阳 110142

Boosting photocatalytic CO2 methanation through TiO2/CdS S-scheme heterojunction and fs-TAS mechanism study

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通讯作者: 陈斌, bchen63@163.com

Boosting photocatalytic CO₂ methanation through TiO₂/CdS S-scheme heterojunction and fs-TAS mechanism study