文献类型：期刊文献

英文题名：Selective conversion of nitrate to nitrogen by CuNi alloys embedded mesoporous carbon with breakpoint chlorination

作者：Yao, Xinyun[1,2];Yu, Bei[3];Xue, Yinghao[3];Ran, Xianqiang[3];Zuo, Jiaqi[4];Qiu, Kaipei[1,4,5]

机构：[1]State Environm Protect Key Lab Environm Risk Asse, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem & Mol Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China;[3]Tongji Univ, Sch Environm Sci & Engn, State Key Lab Pollut Control, Shanghai 200092, Peoples R China;[4]East China Univ Sci & Technol, Sch Resources & Environm Engn, Shanghai Environm Protect Key Lab Environm Stand, 130 Meilong Rd, Shanghai 200237, Peoples R China;[5]Shanghai Inst Pollut Control & Ecol Secur, Shanghai 200092, Peoples R China

年份：2021

卷号：42

外文期刊名：JOURNAL OF WATER PROCESS ENGINEERING

收录：;WOS:【SCI-EXPANDED(收录号:WOS:000677557200008)】；

基金：This work was supported by National Natural Science Foundation of China (Grant Nos. 21972041, 22006037, 51878472) , Shanghai Sailing Program (Grant No. 19YF1410400) , and State Key Laboratory of Pollution Control and Resource Reuse Foundation (Grant No. PCRRF20001) .

语种：英文

外文关键词：Electrocatalytic nitrate reduction; CuNi alloys; Nitrogen-doped mesoporous carbon; 100% dinitrogen selectivity; DFT calculations

摘要：The electrocatalytic reduction of nitrate, a common contaminant in surface and ground water, to the harmless nitrogen gas is a promising technology that can be potentially energy efficient and environmentally friendly. The bottleneck hindering its large-scale implementation is mainly attributed to the unsatisfactory selectivity toward the final product N2. To solve this challenge, a two-step strategy was applied here, in which the NO3- was first reduced to NH4+ at the cathode, followed with a rapid non-electrochemical oxidation to N2 by the ClO- generated from anodic breakpoint chlorination. Note that the formation of ClO- may be easily controlled and enhanced by the dosage of Cl- ions, the overall nitrate removal efficiency for the above process was determined by its NO3- to NH4+ activity. The high-performance copper-nickel alloys embedded mesoporous carbon electrocatalysts were therefore rationally designed, which exhibited a complete conversion of NO3- in the absence of Cl-, and furthermore, a 100% N2 selectivity with the addition of Cl- . Using density functional theory calculations, it was verified that the incorporation of Ni atoms into Cu interface significantly enhanced the adsorption of *NHOH and *NH2OH intermediates, lowering the barrier of *NOH hydrogenation to *NH3 (NH4+). Besides, the nitrogencontaining ordered mesoporous carbon support not only facilitated the synthesis of uniformly distributed CuNi nanoparticles (ca. 20 nm), but also ensured the sufficient mass and charge transfer, as well as the high durability.