Efficient Electrochemical N2 Reduction to NH3 on MoN Nanosheets Array under Ambient Conditions

被引:238
作者
Zhang, Ling [1 ,2 ]
Ji, Xuqiang [1 ]
Ren, Xiang [1 ]
Luo, Yonglan [1 ]
Shi, Xifeng [3 ]
Asiri, Abdullah M. [4 ,5 ]
Zheng, Baozhan [2 ]
Sun, Xuping [1 ]
机构
[1] Univ Elect Sci & Technol China, Inst Fundamental & Frontier Sci, Chengdu 610054, Sichuan, Peoples R China
[2] Sichuan Univ, Coll Chem, Chengdu 610064, Sichuan, Peoples R China
[3] Shandong Normal Univ, Coll Chem Chem Engn & Mat Sci, Jinan 250014, Shandong, Peoples R China
[4] King Abdulaziz Univ, Chem Dept, Fac Sci, POB 80203, Jeddah 21589, Saudi Arabia
[5] King Abdulaziz Univ, Ctr Excellence Adv Mat Res, POB 80203, Jeddah 21589, Saudi Arabia
基金
中国国家自然科学基金;
关键词
MoN nanosheets array; Non-noble-metal catalyst; Electrocatalysis; N-2 reduction reaction; Ambient conditions; METAL NITRIDE CATALYSTS; AMMONIA-SYNTHESIS; ATMOSPHERIC-PRESSURE; NANOWIRE ARRAYS; NITROGEN; WATER; HYDROGEN; CATHODE; ELECTROCATALYSIS; TEMPERATURE;
D O I
10.1021/acssuschemeng.8b01438
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Electrochemical N-2 reduction reaction (NRR) under ambient conditions offers us an environmentally friendly route for artificial synthesis of NH3. However, up to now, few noble-metal-free electrocatalysts with satisfactory catalytic activities have been explored. In this Letter, we demonstrate that MoN nanosheets array on carbon cloth (MoN NA/CC) acts as a high-performance NRR electrocatalyst toward NH3 electrosynthesis in 0.1 M HCl under ambient conditions. This catalyst achieves a large NH3 yield of 3.01 x 10(-10) mol s(-1) cm(-2) and a Faradaic efficiency of 1.15% at -0.3 V vs reversible hydrogen electrode with strong electrochemical durability and selectivity. Density functional theory calculations reveal that MoN NA/CC catalyzes NRR via the Mars-van Krevelen mechanism.
引用
收藏
页码:9550 / 9554
页数:9
相关论文
共 39 条
[1]   Transition Metal Nitride Catalysts for Electrochemical Reduction of Nitrogen to Ammonia at Ambient Conditions [J].
Abghoui, Younes ;
Skulasson, Egill .
INTERNATIONAL CONFERENCE ON COMPUTATIONAL SCIENCE, ICCS 2015 COMPUTATIONAL SCIENCE AT THE GATES OF NATURE, 2015, 51 :1897-1906
[2]   Electroreduction of N2 to Ammonia at Ambient Conditions on Mononitrides of Zr, Nb, Cr, and V: A DFT Guide for Experiments [J].
Abghoui, Younes ;
Garden, Anna L. ;
Howat, Jakob G. ;
Vegge, Tejs ;
Skulason, Egill .
ACS CATALYSIS, 2016, 6 (02) :635-646
[3]   Enabling electrochemical reduction of nitrogen to ammonia at ambient conditions through rational catalyst design [J].
Abghoui, Younes ;
Garden, Anna L. ;
Hlynsson, Valtyr Freyr ;
Bjorgvinsdottir, Snaedis ;
Olafsdottir, Hrefna ;
Skulason, Egill .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2015, 17 (07) :4909-4918
[4]   Electrochemical Reduction of N2 under Ambient Conditions for Artificial N2 Fixation and Renewable Energy Storage Using N2/NH3 Cycle [J].
Bao, Di ;
Zhang, Qi ;
Meng, Fan-Lu ;
Zhong, Hai-Xia ;
Shi, Miao-Miao ;
Zhang, Yu ;
Yan, Jun-Min ;
Jiang, Qing ;
Zhang, Xin-Bo .
ADVANCED MATERIALS, 2017, 29 (03)
[5]   Light-driven dinitrogen reduction catalyzed by a CdS:nitrogenase MoFe protein biohybrid [J].
Brown, Katherine A. ;
Harris, Derek F. ;
Wilker, Molly B. ;
Rasmussen, Andrew ;
Khadka, Nimesh ;
Hamby, Hayden ;
Keable, Stephen ;
Dukovic, Gordana ;
Peters, John W. ;
Seefeldt, Lance C. ;
King, Paul W. .
SCIENCE, 2016, 352 (6284) :448-450
[6]   Mechanism of molybdenum nitrogenase [J].
Burgess, BK ;
Lowe, DJ .
CHEMICAL REVIEWS, 1996, 96 (07) :2983-3011
[7]   Ammonia Electrosynthesis with High Selectivity under Ambient Conditions via a Li+ Incorporation Strategy [J].
Chen, Gao-Feng ;
Cao, Xinrui ;
Wu, Shunqing ;
Zeng, Xingye ;
Ding, Liang-Xin ;
Zhu, Min ;
Wang, Haihui .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2017, 139 (29) :9771-9774
[8]   Electrocatalytic Synthesis of Ammonia at Room Temperature and Atmospheric Pressure from Water and Nitrogen on a Carbon-Nanotube-Based Electrocatalyst [J].
Chen, Shiming ;
Perathoner, Siglinda ;
Ampelli, Claudio ;
Mebrahtu, Chalachew ;
Su, Dangsheng ;
Centi, Gabriele .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2017, 56 (10) :2699-2703
[9]   MoO3 nanosheets for efficient electrocatalytic N2 fixation to NH3 [J].
Han, Jingrui ;
Ji, Xuqiang ;
Ren, Xiang ;
Cui, Guanwei ;
Li, Lei ;
Xie, Fengyu ;
Wang, Hui ;
Li, Baihai ;
Sun, Xuping .
JOURNAL OF MATERIALS CHEMISTRY A, 2018, 6 (27) :12974-12977
[10]   A Cost-Effective 3D Hydrogen Evolution Cathode with High Catalytic Activity: FeP Nanowire Array as the Active Phase [J].
Jiang, Ping ;
Liu, Qian ;
Liang, Yanhui ;
Tian, Jingqi ;
Asiri, Abdullah M. ;
Sun, Xuping .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2014, 53 (47) :12855-12859