| Achieving efficient N-2 electrochemical reduction by stabilizing the N2H* intermediate with the frustrated Lewis pairs | |
| Chen, Zhe1,2; Zhao, Jingxiang3,4; Jiao, Yan5; Wang, Tao2; Yin, Lichang1,6 | |
| Corresponding Author | Wang, Tao(twang@westlake.edu.cn) ; Yin, Lichang(lcyin@imr.ac.cn) |
| 2022-03-01 | |
| Source Publication | JOURNAL OF ENERGY CHEMISTRY
 |
| ISSN | 2095-4956 |
| Volume | 66Pages:628-634 |
| Abstract | 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. |
| Keyword | Nitrogen reduction Electrocatalysis Intermediate stabilization strategy Density functional theory |
| Funding Organization | National Natural Science Foundation of China (NSFC) ; Liaon-ing Provincial Natural Science Foundation of China |
| DOI | 10.1016/j.jechem.2021.09.020 |
| Indexed By | SCI |
| Language | 英语 |
| Funding Project | 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 Research Area | Chemistry ; Energy & Fuels ; Engineering |
| WOS Subject | Chemistry, Applied ; Chemistry, Physical ; Energy & Fuels ; Engineering, Chemical |
| WOS ID | WOS:000744271300003 |
| Publisher | ELSEVIER |
| Citation statistics | |
| Document Type | 期刊论文 |
| Identifier | http://ir.imr.ac.cn/handle/321006/173686 |
| Collection | 中国科学院金属研究所 |
| Corresponding Author | Wang, Tao; Yin, Lichang |
| Affiliation | 1.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Liaoning, Peoples R China 2.Westlake Univ, Ctr Artificial Photosynth Solar Fuels, Sch Sci, Hangzhou 310024, Zhejiang, Peoples R China 3.Harbin Normal Univ, Coll Chem & Chem Engn, Minist Educ, Harbin 150025, Heilongjiang, Peoples R China 4.Harbin Normal Univ, Key Lab Photon & Elect Bandgap Mat, Minist Educ, Harbin 150025, Heilongjiang, Peoples R China 5.Univ Adelaide, Ctr Mat Energy & Catalysis CMEC, Sch Chem Engn & Adv Mat, Adelaide, SA 5005, Australia 6.Huaibei Normal Univ, Dept Phys & Elect Informat, Huaibei 235000, Anhui, Peoples R China |
| Recommended Citation 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. |
| Files in This Item: | There are no files associated with this item. | |||||
Items in the repository are protected by copyright, with all rights reserved, unless otherwise indicated.
Edit Comment