In this study, we designed an integrated electrochemical filtration system for catalytic activation of peroxymonosulfate (PMS) and degradation of aqueous microcontaminants. Composites of carbon nanotube (CNT) and nanoscale zero valence copper (nZVC) were developed to serve as high-performance catalysts, electrode and filtration media simultaneously. We observed both radical and nonradical reaction pathways, which collectively contributed to the degradation of model pollutants. Congo red was completely removed via a single-pass through the nZVCCNT filter (τ <2 s) at neutral pH. The rapid kinetics of Congo red degradation were maintained across a wide pH range (from 3.0–7.0), in complicated matrixes (e.g., tap water and lake water), and for the degradation of a wide array of persistent organic contaminants. The superior activity of nZVCCNT stems from the boosted redox cycles of Cu²⁺/Cu⁺ in the presence of an external electric field. The flow-through design remarkably outperformed the conventional batch system due to the convection-enhanced mass transport. Mechanism studies suggested that the carbonyl group and electrophilic oxygen of CNT served as electron donor and electron acceptor, respectively, to activate PMS to generate •OH and ¹O₂ via one-electron transport. The electron-deficient Cu atoms are prone to react with PMS via surface hydroxyl group to produce reactive intermediates (Cu²⁺-O-O-SO₃⁻), and then ¹O₂ will be generated by breaking the coordination bond of the metastable intermediate. The study will provide a green strategy for the remediation of organic pollution by a highly efficient and integrated system based on catalytic oxidation, electrochemistry, and nano-filtration techniques.

在这项研究中，我们设计了一个集成的电化学过滤系统，用于过氧化单硫酸盐（PMS）的催化活化和水性微污染物的降解。碳纳米管（CNT）和纳米级零价铜（nZVC）的复合材料被开发出来，可以同时用作高性能催化剂，电极和过滤介质。我们观察到自由基和非自由基的反应途径，共同促进了模型污染物的降解。在中性pH值下，通过单次通过nZVC CNT过滤器（τ<2 s）将刚果红完全去除。在复杂的基质（例如：，自来水和湖水），以及用于降解各种持久性有机污染物。nZVC CNT的卓越活性源于在外部电场存在下Cu ²⁺ / Cu ⁺的增强的氧化还原循环。由于对流增强了传质，流通设计明显优于传统的批处理系统。机理研究表明，CNT的羰基和亲电子氧分别充当电子给体和电子受体，以激活PMS通过单电子传输生成•OH和¹ O ₂ 。缺电子的铜原子易于通过PMS与PMS反应表面羟基基团，以产生活性中间体（铜²⁺ -OO-SO ₃ ^- ），然后¹ Ò ₂将通过打破亚稳中间体的配位键而产生。该研究将为基于催化氧化，电化学和纳米过滤技术的高效集成系统提供绿色策略，以补救有机污染。