Achieving efficient N-2 electrochemical reduction by stabilizing the N2H* intermediate with the frustrated Lewis pairs

doi:10.1016/j.jechem.2021.09.020

CORC > 金属研究所 > 中国科学院金属研究所

	*Achieving efficient N-2 electrochemical reduction by stabilizing the N2H intermediate with the frustrated Lewis pairs**
	Chen, Zhe 4,5; Zhao, Jingxiang 2,6; Jiao, Yan 3; Wang, Tao 5; Yin, Lichang 1,4
刊名	JOURNAL OF ENERGY CHEMISTRY
	2022-03-01
卷号	66 页码:628-634
关键词	Nitrogen reduction Electrocatalysis Intermediate stabilization strategy Density functional theory
ISSN号	2095-4956
DOI	10.1016/j.jechem.2021.09.020
通讯作者	Wang, Tao(twang@westlake.edu.cn) ; Yin, Lichang(lcyin@imr.ac.cn)
英文摘要	Electrocatalytic nitrogen reduction reaction (eNRR) with sustainable energy under ambient conditions represents an attractive approach to producing ammonia, but the design of the-state-of-the-art electrocatalyst with high efficiency and selectivity still faces formidable challenges. In contrast to traditional eNRR catalyst design strategies focusing on N N triple bond activation, we herein theoretically proposed an alternative strategy to improve eNRR performance via stabilizing the N2H* intermediate using catalysts with the frustrated Lewis pairs (FLPs), i.e., transition metal (TM) atoms and boron (B) atom codoped 2D black phosphorus (TM-B@BP). Our density functional theory (DFT) results reveal that the TM atom donates electrons to the adsorbed N-2 molecule, while B atom provides empty orbital to stabilize the adsorption of N2H* intermediate. This framework successfully identifies five promising candidates (i.e., Ti-B@BP, V-B@BP, Cr-B@BP, Mn-B@BP and Fe-B@BP) with low theoretical limiting potentials (-0.60, -0.41, -0.45, -0.43 and -0.50 V, respectively) and high selectivity for eNRR. We believe that the intermediate stabilization strategy introduced in current work offers a new opportunity to achieve accelerated and cost-effective ammonia synthesis with electrocatalysis. (C) 2021 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.
资助项目	National Natural Science Foundation of China (NSFC)[51972312] ; National Natural Science Foundation of China (NSFC)[U20A20242] ; Liaon-ing Provincial Natural Science Foundation of China[2020-MS-003]
WOS研究方向	Chemistry ; Energy & Fuels ; Engineering
语种	英语
出版者	ELSEVIER
WOS记录号	WOS:000744271300003
资助机构	National Natural Science Foundation of China (NSFC) ; Liaon-ing Provincial Natural Science Foundation of China
内容类型	期刊论文
源URL	[http://ir.imr.ac.cn/handle/321006/173685]
专题	金属研究所_中国科学院金属研究所
通讯作者	Wang, Tao; Yin, Lichang
作者单位	1.Huaibei Normal Univ, Dept Phys & Elect Informat, Huaibei 235000, Anhui, Peoples R China 2.Harbin Normal Univ, Key Lab Photon & Elect Bandgap Mat, Minist Educ, Harbin 150025, Heilongjiang, Peoples R China 3.Univ Adelaide, Ctr Mat Energy & Catalysis CMEC, Sch Chem Engn & Adv Mat, Adelaide, SA 5005, Australia 4.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Liaoning, Peoples R China 5.Westlake Univ, Ctr Artificial Photosynth Solar Fuels, Sch Sci, Hangzhou 310024, Zhejiang, Peoples R China 6.Harbin Normal Univ, Coll Chem & Chem Engn, Minist Educ, Harbin 150025, Heilongjiang, Peoples R China
推荐引用方式 GB/T 7714	Chen, Zhe,Zhao, Jingxiang,Jiao, Yan,et al. Achieving efficient N-2 electrochemical reduction by stabilizing the N2H* intermediate with the frustrated Lewis pairs[J]. JOURNAL OF ENERGY CHEMISTRY,2022,66:628-634.
APA	Chen, Zhe,Zhao, Jingxiang,Jiao, Yan,Wang, Tao,&Yin, Lichang.(2022).Achieving efficient N-2 electrochemical reduction by stabilizing the N2H* intermediate with the frustrated Lewis pairs.JOURNAL OF ENERGY CHEMISTRY,66,628-634.
MLA	Chen, Zhe,et al."Achieving efficient N-2 electrochemical reduction by stabilizing the N2H* intermediate with the frustrated Lewis pairs".JOURNAL OF ENERGY CHEMISTRY 66(2022):628-634.