Direct ammonia synthesis from the air via gliding arc plasma integrated with single atom electrocatalysis

被引:94
作者
Wu, Angjian [1 ]
Yang, Ji [2 ,4 ]
Xu, Bo [3 ]
Wu, Xiao-Yu [5 ]
Wang, Yuhang [6 ]
Lv, Xingjie [1 ]
Ma, Yichen [7 ]
Xu, Aoni [1 ]
Zheng, Jiageng [1 ]
Tan, Qinhuai [1 ]
Peng, Yaqi [1 ]
Qi, Zhifu [1 ]
Qi, Haifeng [2 ]
Li, Jianfeng [4 ]
Wang, Yaolin [7 ]
Harding, Jonathan [7 ]
Tu, Xin [7 ]
Wang, Aiqin [2 ]
Yan, Jianhua [1 ]
Li, Xiaodong [1 ]
机构
[1] Zhejiang Univ, Dept Energy Engn, State Key Lab Clean Energy Utilizat, Hangzhou 310027, Peoples R China
[2] Chinese Acad Sci, Collaborat Innovat Ctr Chem Energy Mat iChEM, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
[3] Washington State Univ, Dept Civil & Environm Engn, Pullman, WA 99164 USA
[4] Xiamen Univ, Coll Chem & Chem Engn, State Key Lab Phys Chem Solid Surfaces, iChEM, Xiamen 361005, Peoples R China
[5] Univ Waterloo, Dept Mech & Mechatron Engn, Waterloo, ON N2L 3G1, Canada
[6] Soochow Univ, Inst Funct Nano & Soft Mat FUNSOM, Jiangsu Key Lab Carbon Based Funct Mat & Devices, Suzhou 215123, Peoples R China
[7] Univ Liverpool, Dept Elect Engn & Elect, Liverpool L69 3GJ, Merseyside, England
基金
中国国家自然科学基金;
关键词
Ammonia synthesis; Plasma-electrocatalysis; Co single atom; Reaction mechanism; NITROGEN-FIXATION; HABER-BOSCH; REDUCTION; CATALYSTS; IDENTIFICATION;
D O I
10.1016/j.apcatb.2021.120667
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Industrial ammonia synthesis revolutionized global agriculture and industry, but it consumes significant amounts of energy and releases vast quantities of CO2. One alternative, electrocatalytic nitrogen reduction generally suffers from a low ammonia yield rate and poor selectivity. Here, a tandem "plasma-electrocatalysis" strategy was proposed to harvest ammonia from the air. An ammonia yield rate (similar to 1.43 mg(NH3 )cm(-2) h(-1)) with almost 100% faradaic efficiency was achieved during over 50 hours of stable operation at -0.33 V vs. RHE. The ammonia yield rate reached up to similar to 3.0 mg(NH3) cm(-2) h(-1) with a faradaic efficiency of similar to 62% at -0.63 V vs. RHE. This marked performance is achieved by separating activation of stable nitrogen molecules via non-thermal plasma, followed by selective ammonia synthesis via a cobalt single-atom electrocatalyst. This strategy may rival the Haber-Bosch process and the aspirational electrochemical nitrogen reduction at a distributed small-size ammonia production based on a techno-economic analysis.
引用
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页数:10
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