Chen Yundan, Ge Xiaofei, Li Jun, Zhang Zishuai Bill, Li Zhenshan
The Key Laboratory of Water and Sediment Sciences, Ministry of Education, College of Environmental Sciences and Engineering, Peking University, Beijing, China.
Frontiers Science Center for Transformative Molecules, Shanghai Jiao tong University, Shanghai, China.
Nat Commun. 2025 Aug 13;16(1):7509. doi: 10.1038/s41467-025-62930-4.
Ferrate (Fe(VI)) is a prospective green oxidant owing to producing highly reactive Fe(IV)/Fe(V) for micropollutant degradation. However, the performance is significantly compromised by the severe side reaction of Fe(VI) self-decay with HO, generating HO byproduct that quickly quenches Fe(IV)/Fe(V). In this study, we synthesized a single-ruthenium-atom catalyst (RuGN) to activate Fe(VI) to selectively produce Fe(IV)/Fe(V)/Ru(V) for antibiotic degradation, with record-fast ciprofloxacin (CIP) degradation kinetics (~18.7 min g L). Since Fe(VI) preferentially reacts with RuGN rather than HO, RuGN inhibits Fe(VI) self-decay, thus decreasing the HO production. Moreover, RuGN consumes HO (that quenches Fe(IV)/Fe(V)/Ru(V)) in the reaction system, which significantly improves the Fe(VI) utilization rate. Compared with other typical transition metal single-atom catalysts, RuGN exhibits moderate interactions with Fe(VI) and thus facilitates the electron transfer via Ru-O-Fe coordination to activate Fe(VI) for efficient CIP degradation. The RuGN/Fe(VI) system resists interference from background substances coexisting in water, achieving efficient CIP degradation under complex water chemistry conditions and in real water samples. The system can also efficiently degrade CIP in continuous-flow reactors. This work develops a promising strategy for improving Fe(VI) activation via regulating the interaction between the metal site and Fe(VI), holding immense potential for deep wastewater purification.
高铁酸盐（Fe(VI)）是一种有前景的绿色氧化剂，因为它能产生高活性的Fe(IV)/Fe(V)用于微污染物降解。然而，Fe(VI)与HO的严重自衰变副反应会显著损害其性能，产生的HO副产物会迅速淬灭Fe(IV)/Fe(V)。在本研究中，我们合成了一种单钌原子催化剂（RuGN）来活化Fe(VI)，以选择性地产生Fe(IV)/Fe(V)/Ru(V)用于抗生素降解，其环丙沙星（CIP）降解动力学创纪录地快（~18.7 min g L）。由于Fe(VI)优先与RuGN反应而非HO，RuGN抑制了Fe(VI)的自衰变，从而减少了HO的产生。此外，RuGN消耗了反应体系中淬灭Fe(IV)/Fe(V)/Ru(V)的HO，这显著提高了Fe(VI)的利用率。与其他典型的过渡金属单原子催化剂相比，RuGN与Fe(VI)表现出适度的相互作用，因此通过Ru-O-Fe配位促进电子转移以活化Fe(VI)实现高效的CIP降解。RuGN/Fe(VI)体系能抵抗水中共存背景物质的干扰，在复杂的水化学条件下和实际水样中实现高效的CIP降解。该体系还能在连续流反应器中高效降解CIP。这项工作通过调节金属位点与Fe(VI)之间的相互作用，开发了一种改善Fe(VI)活化的有前景策略，在深度废水净化方面具有巨大潜力。
