Multiatom activation of single-atom electrocatalysts via remote coordination for ultrahigh-rate two-electron oxygen reduction
文献类型：期刊论文
| 作者 | Liu, Xiaoqing1; Chen, Rui1; Peng, Wei1; Yin, Lichang2; Yang, De'an1; Hou, Feng1; Wang, Liqun3; Liang, Ji1 |
| 刊名 | JOURNAL OF ENERGY CHEMISTRY
 |
| 出版日期 | 2023 |
| 卷号 | 76页码:622-630 |
| ISSN号 | 2095-4956 |
| 关键词 | Hydrogen peroxide Oxygen reduction reaction Two-electron pathway Remote coordination Electrocatalysis |
| DOI | 10.1016/j.jechem.2022.10.015 |
| 通讯作者 | Liang, Ji(liangji@tju.edu.cn) |
| 英文摘要 | Electrocatalytic oxygen reduction via a two-electron pathway (2e--ORR) is a promising and eco-friendly route for producing hydrogen peroxide (H2O2). Single-atom catalysts (SACs) typically show excellent selectivity towards 2e--ORR due to their unique electronic structures and geometrical configurations. The very low density of single-atom active centers, however, often leads to unsatisfactory H2O2 yield rate, significantly inhibiting their practical feasibility. Addressing this, we herein introduce fluorine as a sec-ondary doping element into conventional SACs, which does not directly coordinate with the single -atom metal centers but synergize with them in a remote manner. This strategy effectively activates the surrounding carbon atoms and converts them into highly active sites for 2e--ORR. Consequently, a record-high H2O2 yield rate up to 27 mol g-1 h-1 has been achieved on the Mo-F-C catalyst, with high Faradaic efficiency of 90%. Density functional theory calculations further confirm the very kinetically facile 2e--ORR over these additional active sites and the superiority of Mo as the single-atom center to others. This strategy thus not only provides a high-performance electrocatalyst for 2e--ORR but also should shed light on new strategies to significantly increase the active centers number of SACs.(c) 2022 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 Foun-dation of China ; [22179093] ; [21905202] |
| WOS研究方向 | Chemistry ; Energy & Fuels ; Engineering |
| 语种 | 英语 |
| 出版者 | ELSEVIER |
| WOS记录号 | WOS:000892138100003 |
| 资助机构 | National Natural Science Foun-dation of China |
| 源URL | [http://ir.imr.ac.cn/handle/321006/176019]  |
| 专题 | 金属研究所_中国科学院金属研究所 |
| 通讯作者 | Liang, Ji |
| 作者单位 | 1.Tianjin Univ, Sch Mat Sci & Engn, Key Lab Adv Ceram & Machining Technol, Minist Educ, Tianjin 300072, Peoples R China 2.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Liaoning, Peoples R China 3.Tianjin Normal Univ, Coll Phys & Mat Sci, Appl Phys Dept, Tianjin 300387, Peoples R China |
| 推荐引用方式 GB/T 7714 | Liu, Xiaoqing,Chen, Rui,Peng, Wei,et al. Multiatom activation of single-atom electrocatalysts via remote coordination for ultrahigh-rate two-electron oxygen reduction[J]. JOURNAL OF ENERGY CHEMISTRY,2023,76:622-630. |
| APA | Liu, Xiaoqing.,Chen, Rui.,Peng, Wei.,Yin, Lichang.,Yang, De'an.,...&Liang, Ji.(2023).Multiatom activation of single-atom electrocatalysts via remote coordination for ultrahigh-rate two-electron oxygen reduction.JOURNAL OF ENERGY CHEMISTRY,76,622-630. |
| MLA | Liu, Xiaoqing,et al."Multiatom activation of single-atom electrocatalysts via remote coordination for ultrahigh-rate two-electron oxygen reduction".JOURNAL OF ENERGY CHEMISTRY 76(2023):622-630. |
入库方式： OAI收割
来源：金属研究所
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