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

文献类型：期刊论文

作者Xu, Yan-Tong1; Peng, Zhigang1,2; Han, Ying1,4; Zhong, Huiqiong1; Yang, Jun2; Cao, Yan1,3
刊名CHEMSUSCHEM
出版日期2022-01-31
页码7
ISSN号1864-5631
关键词ammonia synthesis electrocatalysis hydrogenation nitrate reduction pH gradient
DOI10.1002/cssc.202102450
通讯作者Yang, Jun(tyangj@jnu.edu.cn) ; Cao, Yan(caoyan@ms.giec.ac.cn)
英文摘要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.
WOS关键词REMOVAL
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
语种英语
出版者WILEY-V C H VERLAG GMBH
WOS记录号WOS:000748603200001
资助机构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
源URL[http://ir.giec.ac.cn/handle/344007/35735]  
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
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.

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来源：广州能源研究所

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