The catalyst efficiency-stability trade-off still remains the major challenge for advanced oxidation processes (AOPs). To overcome this challenge, herein, we develop a sustainable and metal-free AOP by an electrified reduced graphene oxide (rGO) membrane in the flow-through electrochemical membrane system, demonstrating efficient degradation of a broader range of water contaminants (>90%), significant reduction of the effluent toxicity (harmless effluent) via the electrochemical activation of peroxymonosulfate (PMS), and long-term stability (>50 h) even in various real water matrices. The external electric field maintains the morphology of rGO and promotes the redox cycle between C–O and C=O groups of rGO at the cathode, with the electrochemical regenerated C–O groups providing sustainable active sites for the formation of rGO-PMS∗, ensuring the long-term stability of the electrified rGO membrane. This work paves the way toward the application of cheap carbonaceous catalysts for effective and sustainable water purification and decontamination.

催化剂效率与稳定性的权衡仍然是高级氧化工艺（AOP）的主要挑战。为了克服这一挑战，我们在此通过流通式电化学膜系统中的带电还原氧化石墨烯 (rGO) 膜开发了一种可持续且无金属的 AOP ，证明可以有效降解更广泛的水污染物 ​​(>90%) ，通过过一硫酸盐 (PMS) 的电化学活化显着降低废水毒性（无害废水），并且即使在各种实际水基质中也具有长期稳定性（> 50 小时）。外部电场维持了rGO的形态，并促进了阴极rGO的C-O和C=O基团之间的氧化还原循环，电化学再生的C-O基团为rGO-PMS*的形成提供了可持续的活性位点，确保带电rGO膜的长期稳定性。这项工作为应用廉价的碳质催化剂进行有效和可持续的水净化和净化铺平了道路。