酞菁铁/MXene复合阴极的制备及电芬顿降解磺胺间二甲氧嘧啶  

Preparation of FePc/MXene Composite Cathode and Electro-Fenton Degradation of Sulfadimethoxine

作　　者：刘会来 李志豪 孔德峰 陈星 LIU Huilai;LI Zhihao;KONG Defeng;CHEN Xing(School of Resources and Environmental Engineering,Hefei University of Technology,Hefei 230009,China;Institute of Industry and Equipment Technology,Hefei University of Technology,Hefei 230009,China)

机构地区：[1]合肥工业大学资源与环境工程学院,合肥230009 [2]合肥工业大学工业与装备技术研究院,合肥230009

出　　处：《无机材料学报》2025年第1期61-69,I0006,I0007,共11页Journal of Inorganic Materials

基　　金：国家重点研发计划(2019YFC0408500);安徽生态文明研究院重点实验室(中心)开放基金(W2023JSKF0152)。

摘　　要：研发具有高活性和高稳定的电极材料,是实现电芬顿体系高效降解磺胺类抗生素污染物的关键。本工作以MXene材料作为载体负载酞菁铁(Fe Pc),制备了Fe Pc/MXene纳米复合材料,并利用其作为阴极催化剂构建的电芬顿体系对磺胺间二甲氧嘧啶(SDM)进行降解。负载Fe Pc后,纳米复合材料依然保持手风琴状的片层结构,并且表面略粗糙,层间间距变小;Fe Pc/MXene中Fe Nx的配位数约为4,且Fe Pc与MXene之间的相互作用促进了电极表面的电子转移。在构建的电芬顿体系中,Fe Pc/MXene电极在50 min内对SDM的降解率达到97.2%,且在较宽的p H范围内表现出优异的催化性能和稳定性。降解性能显著提高主要归因于复合材料中引入Fe N4增强了O_(2)电催化还原为H_(2)O_(2)的活性。电芬顿体系主要通过自由基(·OH和·O_(2)^(–))与非自由基(1O_(2))共同降解SDM。利用前沿轨道理论和Fukui函数阐明了SDM被不同活性物种攻击的位点,降解途径主要有苯环的羟基化、苯环上氨基的氧化、C–S和S–N键断裂。此外,循环和离子浸出实验证明所制备的阴极催化剂具有优异的稳定性。Development of electrode materials with high activity and stability is a key issue to achieve efficient degradation of sulfonamide pollutants by electro-Fenton(EF)system.In this work,FePc/MXene nanocomposites were prepared by using MXene material as carrier to load iron phthalocyanine(FePc)and employed as cathodic catalyst to construct EF system for the degradation of sulfadimethoxine(SDM).After loading FePc,the nanomaterials retained accordion-like lamellar structure with slightly roughened surface and narrowed interlayer spacing.Coordination number of FeNx in FePc/MXene was about 4,in which the interaction between FePc and MXene was favorable to promote the electron transfer at the electrode surface.In the EF system,the FePc/MXene electrode achieved a 97.2% degradation rate of SDM within 50 min,showing excellent catalytic performance and stability over wide pH range.The significant improvement in degradation performance was mainly attributed to the enhanced activity of O_(2) electrocatalytic reduction to H_(2)O_(2) by the introduction of FeN_(4) in the composites.Free radical(·OH and·O_(2)^(–))and non-radical(1O_(2))pathways were co-operative in the degradation of SDM by EF system.Frontier orbital theory and Fukui function theoretically elucidated the sites where SDM was attacked by different reactive oxygen species,primarily degrading through hydroxylation of the benzene ring,oxidation of the amino group on the benzene ring,and cleavage of C–S and S–N bonds.In addition,cycling and ion leaching experiments demonstrated the excellent stability of the prepared cathode catalysts.

关 键 词：电芬顿 FePc/MXene 磺胺间二甲氧嘧啶 活性氧物种 降解路径 

分 类 号：X52[环境科学与工程—环境工程]