文献类型：期刊文献

英文题名：Cu-Fe Synergistic Active Sites Boost Kinetics of Electrochemical Nitrate Reduction

作者：Hua, Yilong[1,2];Song, Nan[3];Wu, Ziyang[1];Lan, Yue[1];Luo, Hongxia[1];Song, Qianqian[1];Yang, Jianping[1]

机构：[1]Donghua Univ, Coll Mat Sci & Engn, State Key Lab Modificat Chem Fibers & Polymer Mat, Shanghai 201620, Peoples R China;[2]Univ South China, Sch Resource & Environm & Safety Engn, Hengyang 421001, Hunan, Peoples R China;[3]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China

年份：2024

卷号：34

期号：21

外文期刊名：ADVANCED FUNCTIONAL MATERIALS

收录：;EI(收录号：20240515481194);WOS:【SCI-EXPANDED(收录号:WOS:001154935300001)】；

基金：Y.H. and N.S. contributed equally to this work. This work was supported by the National Natural Science Foundation of China (No. 52172291, No. 52122312, and No.12375311), "Shuguang Program" supported by Shanghai Education Development Foundation and Shanghai Municipal Education Commission (22SG31), State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Donghua University.

语种：英文

外文关键词：Cu-Fe bimetallic electrode; In situ electrodeposition; rate-determining step; reaction pathway; synergistic NO3RR

摘要：Electrochemical conversion of nitrate offers an efficient solution to nitrate pollution and a sustainable strategy for ammonia generation. Cu and Fe bimetallic electrocatalysts exhibit excellent electrochemical reduction of nitrate (NO3RR) reactivity but the conventional preparation strategy is complex and time-consuming and this reaction is still suffers from unsatisfied kinetic and unidentified mechanisms. Herein, in situ electrodeposition strategy is employed to induce Cu to modify the Fe active sites of iron-based N-doping carbon nanofiber electrode (Fe/Fe3C@NCNFs) during NO3RR in Cu-contained nitrate solution. Benefiting from the synergistic effect between Cu and Fe sites of CuFe/Fe3C@NCNFs electrode, superior activity of rate-determining reaction (*NO(3 )to *NO2) and reduced energy barriers of the following deoxidation and hydrogenation steps are achieved. Compared with Fe/Fe3C@NCNFs-500, the pseudo-first-order (PFO) rate constant for NO3RR by CuFe/Fe3C@NCNFs demonstrates nearly two-fold improvement with high current efficiencies over wide pH and voltage range. Furthermore, the maximum NO3N removal capacity and N-2 selectivity of CuFe/Fe3C@NCNFs reach 15593.8 mg N g(-1) Fe and ca. 92% after twenty cycles. This work offers an avenue for highly active bimetallic electrode design, paving more insights into the interactions between active site construction and NO3RR performance.