Insight into Hydrogenation Selectivity of the Electrocatalytic Nitrate-to-Ammonia Reduction Reaction via Enhancing the Proton Transport

doi:10.1002/cssc.202102450

GIEC OpenIR

	Insight into Hydrogenation Selectivity of the Electrocatalytic Nitrate-to-Ammonia Reduction Reaction via Enhancing the Proton Transport
	Xu, Yan-Tong 1; Peng, Zhigang 1,2; Han, Ying1,4 ; Zhong, Huiqiong1 ; Yang, Jun 2; Cao, Yan 1,3
	2022-01-31
发表期刊	CHEMSUSCHEM
ISSN	1864-5631
页码	7
通讯作者	Yang, Jun(tyangj@jnu.edu.cn) ; Cao, Yan(caoyan@ms.giec.ac.cn)
摘要	The electrocatalytic nitrate-to-ammonia reduction reaction route (NARR) is one of the emerging routes toward green ammonia synthesis, and its conversion efficiency is controlled mainly by the hydrogenation selectivity. This study proposed a likely NARR route feasible and effective even in a neutral condition. Its high catalytic selectivity and efficiency were achieved by a switch of the sulfate solution to the phosphate buffer solution (PBS), while conditions of NO3- concentration, pH, and applied potential were maintained unchanged. Specifically, the faradaic efficiencies toward NH3 (FENH3) in Na2SO4 were as low as 9.8, 19.8, and 11.4 % versus remarkably jumping to 82.8, 90.5, and 89.5 % in PBS under -0.75, -1.0, and -1.25 V, respectively. The corresponding faradaic efficiencies toward NO2- (FENO2-), 77.0, 69.2, and 73.7 % in Na2SO4, significantly dropped to10.8, 7.4, and 4.4 % in PBS, evidencing an unexpected selectivity reversal of the nitrate reduction from NO2- to NH3. This insight was further revealed by the visualization of the pH gradient near the electrode surface during NARR and confirmed by density functional theory calculations; PBS notably facilitated the proton transport and active mitigation over the proton transfer barrier. The use of PBS resulted in a maximal partial current density toward NH3 (J(NH3)) and NH3 formation rate (r(NH3)) up to 133.5 mA cm(-2) and 1.74 x 10(-7) mol s(-1) cm(-2) in 1.0 m KNO3 at -1.25 V.
关键词	ammonia synthesis electrocatalysis hydrogenation nitrate reduction pH gradient
DOI	10.1002/cssc.202102450
关键词[WOS]	REMOVAL
收录类别	SCI
语种	英语
资助项目	NSFC[22178339] ; China Postdoctoral Science Foundation[2021M690151] ; Special Research Assistant Program of the Chinese Academy of Sciences[1190000058] ; Hundred Talents Program (A) of Chinese Academy of Sciences ; Guangdong Provincial Key Laboratory of New and Renewable Energy Research and Development[2021000037] ; Basic Research Program of Guangzhou City[202102020866]
WOS研究方向	Chemistry ; Science & Technology - Other Topics
项目资助者	NSFC ; China Postdoctoral Science Foundation ; Special Research Assistant Program of the Chinese Academy of Sciences ; Hundred Talents Program (A) of Chinese Academy of Sciences ; Guangdong Provincial Key Laboratory of New and Renewable Energy Research and Development ; Basic Research Program of Guangzhou City
WOS类目	Chemistry, Multidisciplinary ; Green & Sustainable Science & Technology
WOS记录号	WOS:000748603200001
出版者	WILEY-V C H VERLAG GMBH
引用统计	被引频次：12[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.giec.ac.cn/handle/344007/35736
专题	中国科学院广州能源研究所
通讯作者	Yang, Jun; Cao, Yan
作者单位	1.Chinese Acad Sci, Guangzhou Inst Energy Convers, Guangdong Prov Key Lab New & Renewable Energy Res, Guangzhou 510640, Peoples R China 2.Jinan Univ, Coll Chem & Mat Sci, Guangzhou 510632, Peoples R China 3.Anhui Univ, Coll Chem & Chem Engn, Hefei 230601, Peoples R China 4.Univ Sci & Technol China, Nano Sci & Technol Inst, Suzhou 215123, Peoples R China
第一作者单位	中国科学院广州能源研究所
推荐引用方式 GB/T 7714	Xu, Yan-Tong,Peng, Zhigang,Han, Ying,et al. Insight into Hydrogenation Selectivity of the Electrocatalytic Nitrate-to-Ammonia Reduction Reaction via Enhancing the Proton Transport[J]. CHEMSUSCHEM,2022:7.
APA	Xu, Yan-Tong,Peng, Zhigang,Han, Ying,Zhong, Huiqiong,Yang, Jun,&Cao, Yan.(2022).Insight into Hydrogenation Selectivity of the Electrocatalytic Nitrate-to-Ammonia Reduction Reaction via Enhancing the Proton Transport.CHEMSUSCHEM,7.
MLA	Xu, Yan-Tong,et al."Insight into Hydrogenation Selectivity of the Electrocatalytic Nitrate-to-Ammonia Reduction Reaction via Enhancing the Proton Transport".CHEMSUSCHEM (2022):7.