Metal-Free C_(3)N_(4) with plentiful nitrogen vacancy and increased specific surface area for electrocatalytic nitrogen reduction

作     者：Ziming Zhao Yu Long Sha Luo Yutong Luo Ming Chen Jiantai Ma Ziming Zhao;Yu Long;Sha Luo;Yutong Luo;Ming Chen;Jiantai Ma

作者机构：State Key Laboratory of Applied Organic Chemistry(SKLAOC)College of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou 730000GansuChina 

出 版 物：《Journal of Energy Chemistry》 (能源化学（英文版）)

年 卷 期：2021年第30卷第9期

页      面：546-555页

核心收录：

学科分类：0820[工学-石油与天然气工程] 081702[工学-化学工艺] 0808[工学-电气工程] 081705[工学-工业催化] 0817[工学-化学工程与技术] 08[工学] 0807[工学-动力工程及工程热物理] 0827[工学-核科学与技术] 080502[工学-材料学] 0805[工学-材料科学与工程（可授工学、理学学位）] 0703[理学-化学] 

基　　金：funded by the National Natural Science Foundation of China (21802058 and 21872066) the Fundamental Research Funds for the Central Universities (China, lzujbky-2020-42) the Natural Science Foundation of Gansu Province (20JR5RA225) 

主　　题：2D C_(3)N_(4)-NV Larger specific surface area Nitrogen vacancy Electrocatalyst NRR 

摘      要：As a substitute for synthetic ammonia under mild condition, electrocatalytic nitrogen reduction reaction(NRR) provides a hopeful approach for the development of ammonia. Nevertheless, the current development of NRR electrocatalysts is far from enough and a systematic research is needed to gain a better improvement. This article presents that 2 D C_(3)N_(4)-NV with a large specific surface area and abundant nitrogen vacancies is prepared by a simple and feasible method, and used as a metal-free catalyst for electrocatalytic NRR. Experiment result and density functional theory(DFT) calculation reveal that nitrogen vacancies in 2 D C_(3)N_(4)-NV can act as an efficient active site for catalytic NRR, which is conducive to capturing and activating N_(2), lowering Gibbs free energy(DG) in reaction and inhibiting hydrogen evolution reaction(HER) at the same time. In addition, the larger specific surface area also makes more active site exposed, which is good for the contact between the electrolyte and the active site, thus enhancing its NRR activity. The electrocatalyst shows an excellent catalytic activity for NRR in 0.1 M HCl, including Faradaic efficiency of 10.96%, NH_(3) yields of 17.85 lg h^(-1) mg_(cat)^(-1)., and good stability(over 20 h).