Quantum-dot–mediated dual-defect interfaces enable high-efficiency solar purification coupled with hydrogen recovery

Photocatalytic hydrogen evolution and pollutant degradation are both promising strategies for clean energy production and environmental remediation, yet their integration for synchronous wastewater-to-energy conversion is fundamentally hindered by inefficient charge utilization and severe interfacial redox competition. Herein, a quantum-dot-bridged dual-defect interface engineering strategy is developed to synchronize photocatalytic oxidation and hydrogen evolution for wastewater-to-energy conversion. As a result, a hierarchical S-type heterostructure was constructed by integrating Ti 3 C 2 MXene quantum dots with electron-storage capability, sulfur-vacancy-rich MoS 2 , and oxygen-deficient CeO 2 (TMMC), which effectively accelerated interfacial charge transport. The optimized catalyst achieves a hydrogen evolution rate of 12.17 mmol g -1 h -1 with 98.6% norfloxacin removal and maintains high stability under continuous operation. In pollutant-containing systems, hydrogen production reaches 274.35 μmol g -1 h -1 and further increases to 405.93 μmol g -1 h -1 upon low-dose peroxymonosulfate addition. Mechanistically, Ce-O-Mo interfacial coupling induces asymmetric charge redistribution and a built-in electric field for directional carrier separation, while spatially separated sulfur and oxygen vacancies regulate proton reduction and oxidant activation, respectively, mitigating interfacial redox competition. This work establishes defect-coordinated interfacial engineering as a general paradigm for regulating charge utilization and reaction selectivity in integrated photocatalytic systems. A bifunctional TMMC photocatalyst with excellent photoelectrical properties is developed for the simultaneous oxidation of pollutants and hydrogen evolution under visible light. The corresponding charge-transfer pathway and photocatalytic mechanism are illustrated in TOC figure. • Constructing MXene quantum-dot-mediated dual-vacancy architectures via interfacial engineering. • Enabling spatially decoupled oxidation and reduction through vacancy-guided S-scheme charge transfer. • Boosting H 2 production to 405.93 μmol g -1 h -1 alongside 98.6% norfloxacin removal via low PMS addition. • Establishing a photo-Fenton-like platform integrating advanced oxidation with hydrogen recovery. • LCA confirms reduced environmental burdens and costs for sustainable wastewater-to-energy conversion.

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Publication Details

Journal
Green Energy & Environment
Published
2026-05-01
DOI
https://doi.org/10.1016/j.gee.2026.04.011
Primary Topic
Advanced Photocatalysis Techniques
Type
article
Field-Weighted Citation Impact
0.00

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article

Quantum-dot–mediated dual-defect interfaces enable high-efficiency solar purification coupled with hydrogen recovery

Zhaofeng Chang, Haida Zhu, Shujing Ye, Luping Tian et al.
Green Energy & Environment
Advanced Photocatalysis Techniques
article

Quantum-dot–mediated dual-defect interfaces enable high-efficiency solar purification coupled with hydrogen recovery

Zhaofeng Chang, Haida Zhu, Shujing Ye, Luping Tian, Zhiwei Jiang, Yaohong Zhong, Hui Wang, Yiduo Chen, Anqi Wang, Kai Yan, Yuzhan Luo, Zongsu Wei, Xiaohong Chen, Zhiqun Xie
article en

Abstract

Photocatalytic hydrogen evolution and pollutant degradation are both promising strategies for clean energy production and environmental remediation, yet their integration for synchronous wastewater-to-energy conversion is fundamentally hindered by inefficient charge utilization and severe interfacial redox competition. Herein, a quantum-dot-bridged dual-defect interface engineering strategy is developed to synchronize photocatalytic oxidation and hydrogen evolution for wastewater-to-energy conversion. As a result, a hierarchical S-type heterostructure was constructed by integrating Ti 3 C 2 MXene quantum dots with electron-storage capability, sulfur-vacancy-rich MoS 2 , and oxygen-deficient CeO 2 (TMMC), which effectively accelerated interfacial charge transport. The optimized catalyst achieves a hydrogen evolution rate of 12.17 mmol g -1 h -1 with 98.6% norfloxacin removal and maintains high stability under continuous operation. In pollutant-containing systems, hydrogen production reaches 274.35 μmol g -1 h -1 and further increases to 405.93 μmol g -1 h -1 upon low-dose peroxymonosulfate addition. Mechanistically, Ce-O-Mo interfacial coupling induces asymmetric charge redistribution and a built-in electric field for directional carrier separation, while spatially separated sulfur and oxygen vacancies regulate proton reduction and oxidant activation, respectively, mitigating interfacial redox competition. This work establishes defect-coordinated interfacial engineering as a general paradigm for regulating charge utilization and reaction selectivity in integrated photocatalytic systems. A bifunctional TMMC photocatalyst with excellent photoelectrical properties is developed for the simultaneous oxidation of pollutants and hydrogen evolution under visible light. The corresponding charge-transfer pathway and photocatalytic mechanism are illustrated in TOC figure. • Constructing MXene quantum-dot-mediated dual-vacancy architectures via interfacial engineering. • Enabling spatially decoupled oxidation and reduction through vacancy-guided S-scheme charge transfer. • Boosting H 2 production to 405.93 μmol g -1 h -1 alongside 98.6% norfloxacin removal via low PMS addition. • Establishing a photo-Fenton-like platform integrating advanced oxidation with hydrogen recovery. • LCA confirms reduced environmental burdens and costs for sustainable wastewater-to-energy conversion.

Green Energy & Environment
Karlsruhe Institute of Technology (DE), Kunming University of Science and Technology (CN), Guangxi University (CN), Sun Yat-sen University (CN), Aarhus University (DK), Dongguan University of Technology (CN), Helmholtz-Institute Ulm (DE)
National Natural Science Foundation of China, Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology
Openalex Percentile: Top 15%
Advanced Photocatalysis Techniques
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