Breaking Long-Range Order in Iridium Oxide by Alkali Ion for Efficient Water Oxidation

doi:10.1021/jacs.8b11456

	Breaking Long-Range Order in Iridium Oxide by Alkali Ion for Efficient Water Oxidation
	Xiao, Hai 2; Huang, Yanqiang 4; Liu, Bin 1; Gao, Jiajian 1; Xu, Cong-Qjao 2; Hung, Sung-Fu 3; Liu, Wei 4; Cai, Weizheng 1; Zeng, Zhiping 1; Jia, Chunmiao 1
刊名	JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
	2019-02-20
卷号	141 期号:7 页码:3014-3023
ISSN号	0002-7863
DOI	10.1021/jacs.8b11456
通讯作者	Li, Jun(junli@tsinghua.edu.cn) ; Huang, Yanqiang(yqhuang@dicp.ac.cn) ; Liu, Bin(liubin@ntu.edu.sg)
英文摘要	Oxygen electrochemistry plays a critical role in clean energy technologies such as fuel cells and electrolyzers, but the oxygen evolution reaction (OER) severely restricts the efficiency of these devices due to its slow kinetics. Here, we show that via incorporation of lithium ion into iridium oxide, the thus obtained amorphous iridium oxide (Li-IrOx) demonstrates outstanding water oxidation activity with an OER current density of 10 mA/cm(2) at 270 mV overpotential for 10 h of continuous operation in acidic electrolyte. DFT calculations show that lithium incorporation into iridium oxide is able to lower the activation barrier for OER X-ray absorption characterizations indicate that both amorphous Li-IrOx and rutile IrO2 own similar [IrO6] octahedron units but have different [IrO6] octahedron connection modes. Oxidation of iridium to higher oxidation states along with shrinkage in the Ir-O bond was observed by in situ X-ray absorption spectroscopy on amorphous Li-IrOx, but not on rutile IrO2 under OER operando conditions. The much more "flexible" disordered [IrO6] octahedrons with higher oxidation states in amorphous Li-IrOx as compared to the periodically interconnected "rigid" [IrO6] octahedrons in crystalline IrO2 are able to act as more electrophilic centers and thus effectively promote the fast turnover of water oxidation.
资助项目	Singapore Ministry of Education Academic Research Fund (AcRF) Tier 1[RG10/16] ; Singapore Ministry of Education Academic Research Fund (AcRF) Tier 1[RG111/15] ; National Key R&D Program of China[2016YFA0202804] ; National Natural Science Foundation of China[21590792] ; National Natural Science Foundation of China[91645203] ; National Natural Science Foundation of China[21521091] ; Singapore Ministry of Education Academic Research Fund (AcRF) Tier 2[MOE2016-T2-2-004]
WOS关键词	OXYGEN EVOLUTION REACTION ; TOTAL-ENERGY CALCULATIONS ; ELECTRONIC-STRUCTURE ; TAFEL LINES ; IRO2 ; ELECTROCATALYSTS ; MECHANISM ; KINETICS ; NANOPARTICLES ; CATALYSTS
WOS研究方向	Chemistry
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000459642000035
资助机构	Singapore Ministry of Education Academic Research Fund (AcRF) Tier 1 ; Singapore Ministry of Education Academic Research Fund (AcRF) Tier 1 ; National Key R&D Program of China ; National Key R&D Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Singapore Ministry of Education Academic Research Fund (AcRF) Tier 2 ; Singapore Ministry of Education Academic Research Fund (AcRF) Tier 2 ; Singapore Ministry of Education Academic Research Fund (AcRF) Tier 1 ; Singapore Ministry of Education Academic Research Fund (AcRF) Tier 1 ; National Key R&D Program of China ; National Key R&D Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Singapore Ministry of Education Academic Research Fund (AcRF) Tier 2 ; Singapore Ministry of Education Academic Research Fund (AcRF) Tier 2 ; Singapore Ministry of Education Academic Research Fund (AcRF) Tier 1 ; Singapore Ministry of Education Academic Research Fund (AcRF) Tier 1 ; National Key R&D Program of China ; National Key R&D Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Singapore Ministry of Education Academic Research Fund (AcRF) Tier 2 ; Singapore Ministry of Education Academic Research Fund (AcRF) Tier 2 ; Singapore Ministry of Education Academic Research Fund (AcRF) Tier 1 ; Singapore Ministry of Education Academic Research Fund (AcRF) Tier 1 ; National Key R&D Program of China ; National Key R&D Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Singapore Ministry of Education Academic Research Fund (AcRF) Tier 2 ; Singapore Ministry of Education Academic Research Fund (AcRF) Tier 2
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/165998]
专题	大连化学物理研究所_中国科学院大连化学物理研究所
通讯作者	Huang, Yanqiang; Liu, Bin; Li, Jun
作者单位	1.Nanyang Technol Univ, Sch Chem & Biomed Engn, 62 Nanyang Dr, Singapore 637459, Singapore 2.Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China 3.Natl Taiwan Univ, Dept Chem, Taipei 106, Taiwan 4.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, 457 Zhongshan Rd, Dalian 116023, Peoples R China 5.Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Peoples R China
推荐引用方式 GB/T 7714	Xiao, Hai,Huang, Yanqiang,Liu, Bin,et al. Breaking Long-Range Order in Iridium Oxide by Alkali Ion for Efficient Water Oxidation[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2019,141(7):3014-3023.
APA	Xiao, Hai.,Huang, Yanqiang.,Liu, Bin.,Gao, Jiajian.,Xu, Cong-Qjao.,...&Li, Jun.(2019).Breaking Long-Range Order in Iridium Oxide by Alkali Ion for Efficient Water Oxidation.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,141(7),3014-3023.
MLA	Xiao, Hai,et al."Breaking Long-Range Order in Iridium Oxide by Alkali Ion for Efficient Water Oxidation".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 141.7(2019):3014-3023.