Multiatom activation of single-atom electrocatalysts via remote coordination for ultrahigh-rate two-electron oxygen reduction

doi:10.1016/j.jechem.2022.10.015

IMR OpenIR

	Multiatom activation of single-atom electrocatalysts via remote coordination for ultrahigh-rate two-electron oxygen reduction
	Liu, Xiaoqing 1; Chen, Rui 1; Peng, Wei 1; Yin, Lichang 2; Yang, De'an 1; Hou, Feng 1; Wang, Liqun 3; Liang, Ji 1
通讯作者	Liang, Ji(liangji@tju.edu.cn)
	2023
发表期刊	JOURNAL OF ENERGY CHEMISTRY
ISSN	2095-4956
卷号	76 页码:622-630
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.
关键词	Hydrogen peroxide Oxygen reduction reaction Two-electron pathway Remote coordination Electrocatalysis
资助者	National Natural Science Foun-dation of China
DOI	10.1016/j.jechem.2022.10.015
收录类别	SCI
语种	英语
资助项目	National Natural Science Foun-dation of China ; [22179093] ; [21905202]
WOS研究方向	Chemistry ; Energy & Fuels ; Engineering
WOS类目	Chemistry, Applied ; Chemistry, Physical ; Energy & Fuels ; Engineering, Chemical
WOS记录号	WOS:000892138100003
出版者	ELSEVIER
引用统计	被引频次：23[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/176020
专题	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.