Citation: Wenlong Wang, Wentao Hao, Lang He, Jia Qiao, Ning Li, Chaoqiu Chen, Yong Qin. Bandgap and adsorption engineering of carbon dots/TiO₂ S-scheme heterojunctions for enhanced photocatalytic CO₂ methanation[J]. Acta Physico-Chimica Sinica, ;2025, 41(9): 100116. doi: 10.1016/j.actphy.2025.100116 shu

Bandgap and adsorption engineering of carbon dots/TiO₂ S-scheme heterojunctions for enhanced photocatalytic CO₂ methanation

Wenlong Wang ^{1, 2} ,
Wentao Hao ^{2, 3} ,
Lang He ^2,, ,
Jia Qiao ² ,
Ning Li ^1,, ,
Chaoqiu Chen ^2,, ,
Yong Qin ²

1.
School of Energy and Power Engineering & State Key Laboratory of Coal and CBM Co-Mining, North University of China, Taiyuan 030051, Shanxi Province, China
2.
State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, Shanxi Province, China
3.
University of Chinese Academy of Sciences, Beijing 100049, China

Corresponding author: Lang He, helang@sxicc.ac.cn Ning Li, lnlong2834@yeah.net Chaoqiu Chen, chenchaoqiu@sxicc.ac.cn
Received Date: 27 April 2025
Revised Date: 9 June 2025
Accepted Date: 10 June 2025

Fund Project: the National Natural Science Foundation of China 22372190ICC CAS SCJC-2023-20the special fund for Science and Technology Innovation Teams of Shanxi Province 202304051001007the Postdoctoral Fellowship Program of CPSF GZC20232815China Postdoctoral Science Foundation 2024M753358China Postdoctoral Science Foundation 2024M763394

S-scheme heterojunctions have garnered significant interest in photocatalytic CO₂ conversion to valuable products (e.g., CH₄) due to their enhanced charge separation and robust redox capabilities. Carbon dots (CDs), with their tunable band structures and light absorption ranges, show particular promise in constructing efficient S-scheme photocatalytic systems. Nevertheless, the critical roles of CDs' band alignment and surface adsorption properties in determining heterojunction configuration, charge carrier kinetics, and ultimately CO₂ activation/product selectivity distribution remain insufficiently explored. Herein, we construct four CDs/TiO₂ heterojunctions using CDs synthesized from varied carbon sources, in which S-scheme heterojunctions were successfully constructed based on cost-effective coal pitch (C-GQDs, 1.75 nm), glucose (G-CQDs, 1.84 nm), and acetone (CQDs-X, 1.82 nm) carbon sources, whereas Type-Ⅰ heterojunctions were formed by carbon black based CDs (GQDs-A, 1.92 nm). Systematic investigations reveal that both the band structure and adsorption characteristics of CDs play important roles in the charge transfer path and separation efficiency, CO₂ adsorption and activation capacities, and product selectivity in photocatalytic CO₂ reduction. Remarkably, the introduction of CDs significantly broadens the photo-response range compared to fresh TiO₂, and in particular, the C-GQDs/TiO₂ exhibits exceptional performance with a CH₄ production rate of 32.7 μmol·g⁻¹·h⁻¹, surpassing TiO₂ by 6.3-fold and outperforming GQDs-A/TiO₂, CQDs-X/TiO₂, and G-CQDs/TiO₂ by factors of 3.8, 2.7, and 2.3, respectively. This heterojunction simultaneously achieves 72.6% CH₄ selectivity and 98.1% hydrocarbons selectivity (encompassing CH₄, C₂H₆, C₂H₄, and C₃H₈). In contrast, composites incorporating GQDs-A, CQDs-X, or G-CQDs exhibit substantially diminished CH₄ selectivity (< 40.0%). The high CH₄ production rate and selectivity of C-GQDs/TiO₂ can be attributed to its unique S-scheme heterojunction structure, higher reduction potential, and well-matched CO₂ and H₂O adsorption and activation capabilities. This study provides unique insights into the efficient photoreduction of CO₂ to CH₄ driven by the S-scheme heterojunction electron transfer pathway in CDs/TiO₂ photocatalysts.
- Bandgap engineering,
- Carbon dots/TiO₂,
- S-scheme heterojunctions,
- Photocatalytic CO₂ methanation,
- Coal-based carbon dots
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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

Bandgap and adsorption engineering of carbon dots/TiO2 S-scheme heterojunctions for enhanced photocatalytic CO2 methanation

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通讯作者: 陈斌, bchen63@163.com

Bandgap and adsorption engineering of carbon dots/TiO₂ S-scheme heterojunctions for enhanced photocatalytic CO₂ methanation