High-throughput Design of Single-atom Catalysts with Nonplanar and Triple Pyrrole-N Coordination for Highly Efficient H<sub>2</sub>O<sub>2</sub> Electrosynthesis

doi:10.1002/anie.202421864

IMR OpenIR

	High-throughput Design of Single-atom Catalysts with Nonplanar and Triple Pyrrole-N Coordination for Highly Efficient H₂O₂ Electrosynthesis
	Jia, Jingjing 1; Li, Zhenxin 1; Sang, Zhiyuan 1,2; Liu, Xiaoqing 1; Peng, Wei 1; Chen, Rui 1; Jiang, Qiao 1; Li, Xia 1; Ren, Zhizhen 3,4; Hao, Weichang 3,4; Yin, Lichang 5; Liu, Jiachen 1; Hou, Feng 1; Liang, Ji 1
通讯作者	Sang, Zhiyuan(sangzhiyuan@tju.edu.cn) ; Hao, Weichang(whao@buaa.edu.cn) ; Yin, Lichang(lcyin@imr.ac.cn) ; Liang, Ji(liangji@tju.edu.cn)
	2025-01-12
发表期刊	ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
ISSN	1433-7851
页码	12
摘要	Single-atom catalysts (SACs) with nonplanar configurations possess unique capabilities for tailoring the oxygen reduction reaction (ORR) catalytic performance compared with the ones with planar configurations, owing to the additional orbital rearrangement arising from the asymmetric coordination atoms. However, the systematic investigation of these nonplanar SACs has long been hindered by the difficulty in screening feasible nonplanar configurations and precisely controlling the coordination structures. Herein, we demonstrate a combined high-throughput screening and experimental verification of nonplanar SACs (ppy-MN3) with metal atoms triple-coordinated by pyrrole-N, for highly active and selective 2e- ORR electrocatalysis. With the additional p-orbital rearrangement of N-ligands for ppy-MN3 during catalysis, a new descriptor on the energy difference between d-band center of metal sites and p-band centers of N-ligands (Delta & varepsilon;d-p) is proposed to accurately identify the relationship between their catalytic activities and electronic structures, on top of the conventional d-band center theory. Consequently, ppy-ZnN3 is identified with excellent 2e- ORR activity (eta=0.08 eV) and selectivity, as well as a low 2e- ORR kinetic barrier under alkaline condition owing to a strong hydrogen bonding between OOH* intermediate and interfacial water, which is then experimentally verified by its high electrocatalytic H2O2 yield (43 mol g-1 h-1) and selectivity (92 %) under alkaline condition. This study thus presents a proof-of-concept demonstration of the performance-oriented and precise coordination design of nonplanar SACs for efficient H2O2 electrosynthesis, and, more importantly, provides an essential complement to the d-band theory for more accurately predicting the catalytic activities of catalysts with nonplanar configurations for series potential electrochemical processes.
资助者	the National Natural Science Foundation of China ; National Natural Science Foundation of China ; Tianjin Graduate Research Innovation Project
DOI	10.1002/anie.202421864
收录类别	SCI
语种	英语
资助项目	the National Natural Science Foundation of China[22379111] ; the National Natural Science Foundation of China[22179093] ; National Natural Science Foundation of China ; Tianjin Graduate Research Innovation Project
WOS研究方向	Chemistry
WOS类目	Chemistry, Multidisciplinary
WOS记录号	WOS:001396316300001
出版者	WILEY-V C H VERLAG GMBH
引用统计	被引频次：1[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/321006/180918
专题	中国科学院金属研究所
通讯作者	Sang, Zhiyuan; Hao, Weichang; Yin, Lichang; 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.Peking Univ, Sch Mat Sci & Engn, Beijing 100871, Peoples R China 3.Beihang Univ, Sch Phys, Beijing 100191, Peoples R China 4.Beihang Univ, Anal & Testing Ctr, Beijing 100191, Peoples R China 5.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China
推荐引用方式 GB/T 7714	Jia, Jingjing,Li, Zhenxin,Sang, Zhiyuan,et al. High-throughput Design of Single-atom Catalysts with Nonplanar and Triple Pyrrole-N Coordination for Highly Efficient H₂O₂ Electrosynthesis[J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2025:12.
APA	Jia, Jingjing.,Li, Zhenxin.,Sang, Zhiyuan.,Liu, Xiaoqing.,Peng, Wei.,...&Liang, Ji.(2025).High-throughput Design of Single-atom Catalysts with Nonplanar and Triple Pyrrole-N Coordination for Highly Efficient H₂O₂ Electrosynthesis.ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,12.
MLA	Jia, Jingjing,et al."High-throughput Design of Single-atom Catalysts with Nonplanar and Triple Pyrrole-N Coordination for Highly Efficient H₂O₂ Electrosynthesis".ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2025):12.