文献类型：期刊文献

英文题名：Direct Synthesis of Ammonia from Nitrate on Amorphous Graphene with Near 100% Efficiency

作者：Huang, Libei[1,2];Cheng, Le[1];Ma, Tinghao[3];Zhang, Jun-Jie[4,5];Wu, Haikun[1];Su, Jianjun[1];Song, Yun[1];Zhu, He[6];Liu, Qi[6];Zhu, Minghui[7];Zeng, Zhiyuan[8];He, Qiyuan[8];Tse, Man-Kit[1];Yang, Deng-tao[3];Yakobson, Boris I.[4,5];Tang, Ben Zhong[9];Ren, Yang[6,10];Ye, Ruquan[1,11]

机构：[1]City Univ Hong Kong, Dept Chem, State Key Lab Marine Pollut, Hong Kong 999077, Peoples R China;[2]Hong Kong Polytech Univ, Sch Profess Educ & Execut Dev PolyU SPEED, Div Sci Engn & Hlth Study, Hong Kong 999077, Peoples R China;[3]Northwestern Polytech Univ, Sch Chem & Chem Engn, Xian 710072, Peoples R China;[4]Rice Univ, Dept Mat Sci & Nano Engn, 6100 Main St, Houston, TX 77005 USA;[5]Rice Univ, Dept Chem, 6100 Main St, Houston, TX 77005 USA;[6]City Univ Hong Kong, Dept Phys, Hong Kong 999077, Peoples R China;[7]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[8]City Univ Hong Kong, Dept Mat Sci & Engn, Hong Kong 999077, Peoples R China;[9]Chinese Univ Hong Kong, Shenzhen Inst Aggregate Sci & Technol, Sch Sci & Engn, Shenzhen 518172, Guangdong, Peoples R China;[10]Argonne Natl Lab, X Ray Sci Div, 9700 S Cass Ave, Argonne, IL 60439 USA;[11]City Univ Hong Kong, Shenzhen Res Inst, Shenzhen 518057, Guangdong, Peoples R China

年份：2023

卷号：35

期号：24

外文期刊名：ADVANCED MATERIALS

收录：;EI(收录号：20231814041108);WOS:【SCI-EXPANDED(收录号:WOS:000977863800001)】；

基金：The study described in this paper was partially supported by the Shenzhen Science and Technology Program (JCYJ20220818101204009), the Young Scientists Fund of the National Natural Science Foundation of China (Project No. 21905240) and the State Key Laboratory of Marine Pollution Seed Collaborative Research Fund (Grant No. SKLMP/IRF/0029). R.Y. also acknowledges the support from the Chow Sang Sang Group Research Fund (Project No. 9229060) sponsored by the Chow Sang Sang Holdings International Limited and CityU Applied Research Grant (Project No. 9667224). This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility, operated for the DOE Office of Science by the Argonne National Laboratory under Contract No. DE-AC02-06CH11357. Computational modeling work at Rice (J.-J.Z. and B.I.Y.) was supported by the Office of Naval Research (N00014-22-1-2788).

语种：英文

外文关键词：ammonia synthesis; amorphous graphene; laser induction; nitrate reduction; wastewater remediation

摘要：Ammonia is an indispensable commodity in the agricultural and pharmaceutical industries. Direct nitrate-to-ammonia electroreduction is a decentralized route yet challenged by competing side reactions. Most catalysts are metal-based, and metal-free catalysts with high nitrate-to-ammonia conversion activity are rarely reported. Herein, it is shown that amorphous graphene synthesized by laser induction and comprising strained and disordered pentagons, hexagons, and heptagons can electrocatalyze the eight-electron reduction of NO3- to NH3 with a Faradaic efficiency of approximate to 100% and an ammonia production rate of 2859 mu g cm(-2) h(-1) at -0.93 V versus reversible hydrogen electrode. X-ray pair-distribution function analysis and electron microscopy reveal the unique molecular features of amorphous graphene that facilitate NO3- reduction. In situ Fourier transform infrared spectroscopy and theoretical calculations establish the critical role of these features in stabilizing the reaction intermediates via structural relaxation. The enhanced catalytic activity enables the implementation of flow electrolysis for the on-demand synthesis and release of ammonia with >70% selectivity, resulting in significantly increased yields and survival rates when applied to plant cultivation. The results of this study show significant promise for remediating nitrate-polluted water and completing the NOx cycle.