Identification of the highly active Zn-N4 sites with pyrrole/pyridine-N synergistic coordination by dz2+s-band center for electrocatalytic H2O2 production

doi:10.1016/j.jechem.2024.06.021

IMR OpenIR

	Identification of the highly active Zn-N4 sites with pyrrole/pyridine-N synergistic coordination by dz2+s-band center for electrocatalytic H2O2 production
	Chen, Rui 1; Liu, Wei 1; Sang, Zhiyuan 1; Jia, Jingjing 1; Li, Zhenxin 1; Nie, Jiahuan 1; Jiang, Qiao 1; Mao, Zixian 1; Guo, Baitong 1; Wang, Qiuying 1; Hou, Feng 1; Yin, Lichang 2; Yang, De'an 1; Liang, Ji 1
通讯作者	Sang, Zhiyuan(sangzhiyuan@tju.edu.cn) ; Yin, Lichang(lcyin@imr.ac.cn) ; Yang, De'an(dayang@tju.edu.cn) ; Liang, Ji(liangji@tju.edu.cn)
	2024-11-01
发表期刊	JOURNAL OF ENERGY CHEMISTRY
ISSN	2095-4956
卷号	98 页码:105-113
摘要	Single metal atoms anchored on nitrogen-doped carbon materials (M-N4) have been identified as effective active sites for catalyzing the two-electron oxygen reduction reaction (2e-ORR). However, the relationship between the local atomic/electronic environments of the M-N4 sites (metal atoms coordinated with different types of N species) and their catalytic activity for 2e-ORR has rarely been elaborated clearly, which imposes significant ambiguity for the rational design of catalysts. Herein, guided by the comprehensive density-functional theory calculations and predictions, a series of Zn-N4 single-atom catalysts (SACs) are designed with pyrrole/pyridine-N (NPo/NPd) synergistic coordination and prepared by controlling the pyrolysis temperature (600, 700, and 800 degrees C). Among them, the dominated Zn-N4 configurations with rationally combined NPo/NPd coordination show *OOH adsorption strength close to the optimal value, much superior to those with mono N species. Thus, the as-prepared catalyst exhibits a high H2O2 selectivity of over 90% both in neutral and alkaline environments, with a superb H2O2 yield of up to 33.63 mol g-1 h-1 in an alkaline with flow cell. More importantly, a new descriptor, dz2+s band center, has been proposed, which is especially feasible for predicting the activity for metal types with fully occupied s and d orbitals. This work thus presents clear guidance for the rational design of highly active SACs toward ORR and provides a complement to the d-band theory for more accurately predicting the catalytic activity of the materials. (c) 2024 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights are reserved, including those for text and data mining, AI training, and similar technologies.
关键词	Zinc single -atom catalysts Hydrogen peroxide Local coordination environments d plus s -Band modulation
资助者	National Natural Science Foundation of China
DOI	10.1016/j.jechem.2024.06.021
收录类别	SCI
语种	英语
资助项目	National Natural Science Foundation of China[22379111] ; National Natural Science Foundation of China[22179093]
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:001267744700001
出版者	ELSEVIER
引用统计	被引频次：10[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/321006/187963
专题	中国科学院金属研究所
通讯作者	Sang, Zhiyuan; Yin, Lichang; Yang, De'an; 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
推荐引用方式 GB/T 7714	Chen, Rui,Liu, Wei,Sang, Zhiyuan,et al. Identification of the highly active Zn-N4 sites with pyrrole/pyridine-N synergistic coordination by dz2+s-band center for electrocatalytic H2O2 production[J]. JOURNAL OF ENERGY CHEMISTRY,2024,98:105-113.
APA	Chen, Rui.,Liu, Wei.,Sang, Zhiyuan.,Jia, Jingjing.,Li, Zhenxin.,...&Liang, Ji.(2024).Identification of the highly active Zn-N4 sites with pyrrole/pyridine-N synergistic coordination by dz2+s-band center for electrocatalytic H2O2 production.JOURNAL OF ENERGY CHEMISTRY,98,105-113.
MLA	Chen, Rui,et al."Identification of the highly active Zn-N4 sites with pyrrole/pyridine-N synergistic coordination by dz2+s-band center for electrocatalytic H2O2 production".JOURNAL OF ENERGY CHEMISTRY 98(2024):105-113.