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铁铜双金属界面的远程电子转移途径:连接催化机制与持久性污染物降解的可扩展应用

Long-range electron transfer pathways at FeCu bimetallic interfaces: Bridging catalytic mechanisms and scalable applications for persistent pollutant degradation.

作者信息

You Xiaoyin, Wang Chaohai, Wang Chuqiao, Xu Xing, Hu Yuying, Li Ning, Hu Fengping, Liu Wen, Peng Xiaoming

机构信息

School of Civil Engineering and Architecture, East China Jiaotong University, Nanchang 330013, PR China.

School of Municipal and Environmental Engineering, Henan University of Urban Construction, Pingdingshan 467036, PR China.

出版信息

J Hazard Mater. 2025 Aug 15;494:138682. doi: 10.1016/j.jhazmat.2025.138682. Epub 2025 May 22.

Abstract

Efficient and stable heterogeneous catalysts for peroxymonosulfate (PMS) activation are pivotal for advancing advanced oxidation processes in water treatment. However, the limited redox cycling capacity of single-metal sites often hinders their catalytic performance and durability. Here, dispersed Fe-Cu bimetallic clusters anchored on a nitrogen-sulfur codoped carbon matrix ((FeCu-SNC) were synthesized via a coordination-pyrolysis strategy. FeCu-SNC was engineered to activate peroxymonosulfate (PMS) for the degradation of bisphenol A (BPA) and structurally diverse pollutants. Combined experimental and density functional theory (DFT) analyses revealed that the Fe-Cu dual sites synergistically enhanced PMS adsorption and triggered a dominant electron transfer pathway (ETP), bypassing conventional radical-mediated mechanisms. The FeCu-SNC/PMS system achieved rapid BPA degradation (k > 0.38 min), with preferential oxidation of pollutants bearing electron-donating groups. A dynamic catalytic membrane system (DCMS) integrated with electrospinning technology enabled catalyst reuse, maintaining > 95 % BPA removal over 300 min of continuous operation. Furthermore, a scalable ETP device utilizing a salt bridge and ammeter effectively isolated sulfate ion leaching, attaining 96 % pollutant removal after 72 h while addressing secondary pollution. This work provides a dual strategy- catalyst design and process engineering-for sustainable water decontamination.

摘要

用于过一硫酸盐(PMS)活化的高效稳定多相催化剂对于推进水处理中的高级氧化过程至关重要。然而,单金属位点有限的氧化还原循环能力常常阻碍其催化性能和耐久性。在此,通过配位 - 热解策略合成了锚定在氮硫共掺杂碳基质上的分散铁 - 铜双金属簇((FeCu - SNC))。FeCu - SNC被设计用于活化过一硫酸盐(PMS)以降解双酚A(BPA)和结构多样的污染物。结合实验和密度泛函理论(DFT)分析表明,铁 - 铜双位点协同增强了PMS的吸附并触发了一条主导的电子转移途径(ETP),绕过了传统的自由基介导机制。FeCu - SNC/PMS体系实现了双酚A的快速降解(k > 0.38 min),对带有供电子基团的污染物具有优先氧化作用。与静电纺丝技术集成的动态催化膜系统(DCMS)实现了催化剂的重复使用,在连续运行300分钟内保持> 95%的双酚A去除率。此外,一种利用盐桥和电流表的可扩展ETP装置有效地隔离了硫酸根离子的浸出,在72小时后实现了96%的污染物去除率,同时解决了二次污染问题。这项工作为可持续水净化提供了一种双重策略——催化剂设计和工艺工程。

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