Tuning the p-Orbital Electron Structure of s-Block Metal Ca Enables a High-Performance Electrocatalyst for Oxygen Reduction

doi:10.1002/adma.202107103

	Tuning the p-Orbital Electron Structure of s-Block Metal Ca Enables a High-Performance Electrocatalyst for Oxygen Reduction
	Lin, Zhiyu 1; Huang, Hao 1; Cheng, Ling 1; Hu, Wei 1; Xu, Pengping 1; Yang, Yang 1; Li, Jianmin 2; Gao, Feiyue 1; Yang, Kang 1; Liu, Shuai 1
刊名	ADVANCED MATERIALS
	2021-10-11
关键词	active center oxygen reduction p-orbital electron structure s-block metal Ca single atom
ISSN号	0935-9648
DOI	10.1002/adma.202107103
通讯作者	Wang, Hui(hw39@hmfl.ac.cn) ; Chen, Qianwang(cqw@ustc.edu.cn)
英文摘要	Most previous efforts are devoted to developing transition metals as electrocatalysts guided by the d-band center model. The metals of the s-block of the periodic table have so far received little attention in the application of oxygen reduction reactions (ORR). Herein, a carbon catalyst with calcium (Ca) single atom coordinated with N and O is reported, which displays exceptional ORR activities in both acidic condition (E-1/2 = 0.77 V, 0.1 m HClO4) and alkaline condition (E-1/2 = 0.90 V, 0.1 m KOH). The Ca-N, O/C exhibits remarkable performance in zinc-air battery with a maximum power density of 218 mW cm(-2), superior to a series of catalysts reported so far. X-ray absorption near-edge structure (XANES) characterization confirms the formation of N- and O-atom-coordinated Ca in the carbon matrix. Density functional theory (DFT) calculations reveal that the high catalytic activity of main-group Ca is ascribed to the fact that its p-orbital electron structure is regulated by N and O coordination so that the highest peak (E-P) of the projected density of states (PDOS) for the Ca atom is moved close to the Fermi level, thereby facilitating the adsorption of ORR intermediates and electron transfer.
资助项目	National Natural Science Foundation (NSFC)[51772283] ; National Key R&D 229 Program of China[2016YFA0401801]
WOS关键词	GRAPHENE OXIDE ; HYDROGEN EVOLUTION ; ACTIVE-SITES ; FUEL-CELL ; CARBON ; CATALYST ; NITROGEN ; NANOPARTICLES ; DESIGN ; IRON
WOS研究方向	Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics
语种	英语
出版者	WILEY-V C H VERLAG GMBH
WOS记录号	WOS:000705985400001
资助机构	National Natural Science Foundation (NSFC) ; National Key R&D 229 Program of China
内容类型	期刊论文
源URL	[http://ir.hfcas.ac.cn:8080/handle/334002/125525]
专题	中国科学院合肥物质科学研究院
通讯作者	Wang, Hui; Chen, Qianwang
作者单位	1.Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Dept Mat Sci & Engn, Natl Synchrotron Radiat Lab, Hefei 230026, Peoples R China 2.Chinese Acad Sci, Inst High Energy Phys, Beijing Synchrotron Radiat Facil BSRF, Beijing 100049, Peoples R China 3.Chinese Acad Sci, Hefei Inst Phys Sci, High Field Magnet Lab, Anhui Key Lab Condensed Mater Phys Extreme Condit, Hefei 230031, Peoples R China
推荐引用方式 GB/T 7714	Lin, Zhiyu,Huang, Hao,Cheng, Ling,et al. Tuning the p-Orbital Electron Structure of s-Block Metal Ca Enables a High-Performance Electrocatalyst for Oxygen Reduction[J]. ADVANCED MATERIALS,2021.
APA	Lin, Zhiyu.,Huang, Hao.,Cheng, Ling.,Hu, Wei.,Xu, Pengping.,...&Chen, Qianwang.(2021).Tuning the p-Orbital Electron Structure of s-Block Metal Ca Enables a High-Performance Electrocatalyst for Oxygen Reduction.ADVANCED MATERIALS.
MLA	Lin, Zhiyu,et al."Tuning the p-Orbital Electron Structure of s-Block Metal Ca Enables a High-Performance Electrocatalyst for Oxygen Reduction".ADVANCED MATERIALS (2021).