Peracetic acid (PAA) serves as a potent and low-toxic oxidant for contaminant removal. Radical-mediated catalytic PAA oxidation processes are typically non-selective, rendering weakened oxidation efficacy under complex water matrices. Herein, we explored the usage of reduced graphene oxide (rGO) for PAA activation via a non-radical pathway. Outperforming the most catalytic PAA oxidation systems, the rGO–PAA system exhibits near-complete removal of typical micropollutants (MPs) within a short time (<2 min). Non-radical direct electron transfer (DET) from MPs to PAA plays a decisive role in the MP degradation, where accelerated DET is achieved by a higher potential of the rGO–PAA reactive surface complexes. Benefitting from DET, the rGO–PAA system shows robust removal of multiple MPs under complex water matrices and with low toxicity. Notably, in the DET regime, the electrostatic attraction of rGO to both PAA and target MP is a critical prerequisite for achieving efficient oxidation, depending on the conditions of solution pH and MP pK_a. A heatmap model building on such an electrostatic interaction is further established as guidance for regulating the performance of the DET-mediated PAA oxidation systems. Overall, our work unveils the imperative role of DET for rGO-activated PAA oxidation, expanding the knowledge of PAA-based water treatment strategies.

中文翻译：

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还原的氧化石墨烯触发过乙酸活化以强力去除微污染物：电子转移的作用

过氧乙酸 (PAA) 是一种有效且低毒的氧化剂，可用于去除污染物。自由基介导的催化 PAA 氧化过程通常是非选择性的，导致复杂水基质下的氧化效果减弱。在此，我们探索了还原氧化石墨烯 (rGO) 通过非自由基途径激活 PAA 的用途。rGO-PAA 系统的性能优于最具催化作用的 PAA 氧化系统，可在短时间内（<2 分钟）几乎完全去除典型的微污染物 (MP)。从 MP 到 PAA 的非自由基直接电子转移 (DET) 在 MP 降解中起着决定性作用，其中加速的 DET 是通过 rGO-PAA 反应性表面复合物的更高电位实现的。受益于 DET，rGO-PAA 系统显示出在复杂水基质和低毒性下对多种 MP 的稳健去除。尤其，一个。_{_} 进一步建立基于这种静电相互作用的热图模型，作为调节 DET 介导的 PAA 氧化系统性能的指导。总的来说，我们的工作揭示了 DET 对于 rGO 激活的 PAA 氧化的重要作用，扩展了基于 PAA 的水处理策略的知识。