Highly active and stable single iron site confined in graphene nanosheets for oxygen reduction reaction

doi:10.1016/j.nanoen.2016.12.056

	Highly active and stable single iron site confined in graphene nanosheets for oxygen reduction reaction
	Yu, Liang 1; Wang, Suheng 2; Deng, Dehui 1,2; Bao, Xinhe 1; Chen, Xiaoqi 1
刊名	NANO ENERGY
	2017-02-01
卷号	32 页码:353-358
关键词	Oxygen Reduction Reaction Non-precious Metals Graphene Single Iron Site Dft Calculations
ISSN号	2211-2855
DOI	10.1016/j.nanoen.2016.12.056
文献子类	Article
英文摘要	Exploring high performance non-precious metal catalysts to substitute Pt for oxygen reduction reaction (ORR) has stimulated wide research interest recently, but it remains a great challenge. Herein, we report a single iron site confined in graphene catalyst via 4N atoms, forming flat FeN4 structure in the matrix of graphene. The optimized catalyst shows a high ORR activity, almost coming up to the activity of commercial 40% Pt/C catalyst, but a significantly higher stability and tolerance to SOx, NOx and methanol with respect to 40% Pt/C. This well-defined structure provides an ideal model to study the catalytic origin of iron-based catalysts. DFT calculations indicate that the high ORR activity origins from highly dispersed and high-density coordinatively unsaturated Fe centers, and the excellent stability origins from the unique confinement of the graphene matrix via 4N atoms. This reaction can proceed easily to H2O via a four electron transfer path way on the single iron site, which is further confirmed by the experiment. This experimental and theoretical study provides a further insight into the nature of the Fe/N/C catalyst and also introduces a reference for designing high efficient catalysts in electrocatalysis.
WOS关键词	INITIO MOLECULAR-DYNAMICS ; DENSITY-FUNCTIONAL THEORY ; HIGH ELECTROCATALYTIC ACTIVITY ; TOTAL-ENERGY CALCULATIONS ; AUGMENTED-WAVE METHOD ; FUEL-CELL CATHODE ; CARBON NANOTUBES ; ALKALINE-MEDIUM ; DOPED GRAPHENE ; BASIS-SET
WOS研究方向	Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics
语种	英语
出版者	ELSEVIER SCIENCE BV
WOS记录号	WOS:000397003700043
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/169456]
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	Deng, Dehui; Bao, Xinhe
作者单位	1.Chinese Acad Sci, Dalian Inst Chem Phys, iChEM, State Key Lab Catalysis, Zhongshan Rd 457, Dalian 116023, Peoples R China 2.Xiamen Univ, Coll Chem & Chem Engn, iChEM, Xiamen 361005, Peoples R China
推荐引用方式 GB/T 7714	Yu, Liang,Wang, Suheng,Deng, Dehui,et al. Highly active and stable single iron site confined in graphene nanosheets for oxygen reduction reaction[J]. NANO ENERGY,2017,32:353-358.
APA	Yu, Liang,Wang, Suheng,Deng, Dehui,Bao, Xinhe,&Chen, Xiaoqi.(2017).Highly active and stable single iron site confined in graphene nanosheets for oxygen reduction reaction.NANO ENERGY,32,353-358.
MLA	Yu, Liang,et al."Highly active and stable single iron site confined in graphene nanosheets for oxygen reduction reaction".NANO ENERGY 32(2017):353-358.