2D copper-iron bimetallic metal-organic frameworks for reduction of nitrate with boosted efficiency and ammonia selectivity  

作　　者：Qian Ma Yinghao Xue Chuning Zhang Yanyan Chen Wei Teng Hua Zhang Jianwei Fan 

机构地区：[1]State Key Laboratory of Pollution Control and Resources Reuse,College of Environmental Science and Engineering,Tongji University,Shanghai 200092,China

出　　处：《Journal of Environmental Sciences》2025年第3期374-385,共12页环境科学学报(英文版)

基　　金：supported by the National Natural Science Foundation of China(NSFC)(Nos.52370044 and 21976134);the State Key Laboratory of Pollution Control and Resource Reuse Foundation(Nos.PCRRK21003 and PCRRK21001);Shanghai Scientific Research Plan Project(No.23ZR1467000);the State Key Laboratory of Treatments and Recycling for Organic Effluents by Adsorption in Petroleum and Chemical Industry(No.SDHY2206).

摘　　要：Electrocatalytic reduction of nitrate to ammonia has been considered a promising and sustainable pathway for pollutant treatment and ammonia has significant potential as a clean energy.Therefore,the method has received much attention.In this work,Cu/Fe 2D bimetallic metal-organic frameworks were synthesized by a facile method applied as cathode materials without high-temperature carbonization.Bimetallic centers(Cu,Fe)with enhanced intrinsic activity demonstrated higher removal efficiency.Meanwhile,the 2D nanosheet reduced themass transfer barrier between the catalyst and nitrate and increased the reaction kinetics.Therefore,the catalysts with a 2D structure showed much better removal efficiency than other structures(3D MOFs and BulkMOFs).Under optimal conditions,Cu/Fe-2D MOF exhibited high nitrate removal efficiency(87.8%)and ammonium selectivity(89.3%)simultaneously.The ammonium yielded up to significantly 907.2μg/(hr·mg_(cat))(7793.8μg/(hr·mg_(metal)))with Faradaic efficiency of 62.8%at an initial 100 mg N/L.The catalyst was proved to have good stability and was recycled 15 times with excellent effect.DFT simulations confirm the reduced Gibbs free energy of Cu/Fe-2D MOF.This study demonstrates the promising application of Cu/Fe-2D MOF in nitrate reduction to ammonia and provides new insights for the design of efficient electrode materials.

关 键 词：Metal-organic frameworks Electrochemical denitrification Ammonium selectivity 2D bimetal materials 

分 类 号：X701[环境科学与工程—环境工程]