光催化
制氢
双功能
氧化还原
材料科学
异质结
催化作用
氢
化学工程
载流子
分解水
析氧
光化学
降级(电信)
纳米技术
半导体
再分配(选举)
化学
化学反应工程
氢燃料
太阳能
量子效率
选择性
光催化分解水
人工光合作用
作者
Haida Zhu,Hui Wang,Yuzhan Luo,Luping Tian,Zhaofeng Chang,Xiaohong Chen,Yiduo Chen,Yaohong Zhong,Zhiqun Xie,Zhiwei Jiang,Shujing Ye,Zongsu Wei,Kai Yan,Anqi Wang
标识
DOI:10.1016/j.gee.2026.04.011
摘要
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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