Bai Chang-Wei, Yang Fu-Qiao, Duan Pi-Jun, Zhang Zhi-Quan, Sun Yi-Jiao, Chen Xin-Jia, Chen Fei, Yu Han-Qing
Key Laboratory of the Three Gorges Reservoir Region's Eco-Environment, Ministry of Education, College of Environment and Ecology, Chongqing University, Chongqing, China.
CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science and Technology of China, Hefei, China.
Nat Commun. 2025 Mar 28;16(1):3019. doi: 10.1038/s41467-025-58392-3.
Developing efficient and stable heterogeneous catalysts for the continuous activation of oxidants is crucial to mitigating the global water resource crisis. Guided by computational predictions, this research achieved this goal through the synthesis of a modified graphitic carbon nitride with enhanced catalytic activity and stability. Its intrinsic activity was further amplified by dynamic in-situ reconstruction using the I/I redox mediator system during photoreactions. Impressively, this reconstructed catalyst demonstrated the capability for at least 30 regeneration cycles while maintaining high purification efficacy. The mechanism underlying the in-situ reconstruction of active sites for periodate functionalization was elucidated through theoretical calculations, coupled with semi-in-situ X-ray photoelectron spectroscopy (XPS) and electrochemical analyses. The system's capacity to detoxify recalcitrant pollutants was demonstrated through successful Escherichia coli cultivation and Zebrafish embryo experiments. The economic feasibility and environmental impacts are quantitatively assessed by the Electrical Energy per Order (EE/O) metric and Life Cycle Assessment (LCA), confirming the system's scalability and applicability in real-world scenarios. This dual-site constrained interlayer insertion, and controllable in-situ catalyst reconstruction achieve durable robustness of the photocatalyst, paving the way for the development of sustainable catalytic water purification technologies.
开发高效稳定的非均相催化剂以持续激活氧化剂对于缓解全球水资源危机至关重要。在计算预测的指导下，本研究通过合成具有增强催化活性和稳定性的改性石墨相氮化碳实现了这一目标。在光反应过程中，利用I/I氧化还原介质系统进行动态原位重构，进一步放大了其固有活性。令人印象深刻的是，这种重构催化剂在保持高净化效率的同时，展示了至少30次再生循环的能力。通过理论计算，结合半原位X射线光电子能谱（XPS）和电化学分析，阐明了用于高碘酸盐功能化的活性位点原位重构的机制。通过成功的大肠杆菌培养和斑马鱼胚胎实验，证明了该系统对难降解污染物的解毒能力。通过每阶电能（EE/O）指标和生命周期评估（LCA）对该系统的经济可行性和环境影响进行了定量评估，证实了该系统在实际场景中的可扩展性和适用性。这种双位点受限层间插入和可控的原位催化剂重构实现了光催化剂的持久稳定性，为可持续催化水净化技术的发展铺平了道路。
