CAS OpenIR  > 中科院上海应用物理研究所2011-2018年
Identification of binuclear Co2N5 active sites for oxygen reduction reaction with more than one magnitude higher activity than single atom CoN4 site
Xiao, ML; Zhang, H; Chen, YT; Zhu, JB; Gao, LQ; Jin, Z; Ge, JJ; Jiang, Z; Chen, SL; Liu, CP; Xing, W
2018
Source PublicationNANO ENERGY
ISSN2211-2855
Volume46Pages:396-403
Subtype期刊论文
AbstractHerein, a novel binuclear active site structure, Co2NxCy, is intentionally designed and successfully fabricated to efficiently catalyze the oxygen reduction reaction (ORR), which is achieved by precisely controlling the atomic scale structure of bimetal-organic frameworks before pyrolysis. Through discovering a two-atom site with Co-Co distance at 2.1-2.2 angstrom from aberration-corrected scanning transmission electron microscopy (STEM), as well as a novel shortened Co-Co path (2.12 angstrom) from the X-ray absorption spectroscopy, we for the first time identified the binuclear Co2NX site in the pyrolyzed catalyst. Combined with density functional theory (DFT) calculation, the structure is further confirmed as Co2N5. Excitingly, the Co2N5 site performs approximately 12 times higher activity than the conventional CoN4 site and the corresponding catalyst shows unprecedented catalytic activity in acidic electrolyte with half-wave potential of 0.79 V, approaching the commercial Pt/C catalyst and presenting the best one among the Co-N-C catalysts. Theoretical density functional theory calculations reveal that the novel binuclear site exhibits considerably reduced thermodynamic barrier towards ORR, thus contributing to the much higher intrinsic activity. Our finding opens up a new path to design efficient M-N-x/C catalysts, thus pushing the fuel cell industry field one step ahead.
KeywordMetal-organic Frameworks Cytochrome-c-oxidase Fuel-cell Cathode Reaction Catalysts Fe/n/c-catalysts Acidic Media Iron Electrocatalysts Carbon Spectroscopy
DOI10.1016/j.nanoen.2018.02.025
Indexed BySCI
Language英语
WOS IDWOS:000427924000046
Citation statistics
Cited Times:24[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.sinap.ac.cn/handle/331007/29036
Collection中科院上海应用物理研究所2011-2018年
Affiliation1.Xiao, ML
2.Zhang, H
3.Chen, YT
4.Zhu, JB
5.Gao, LQ
6.Jin, Z
7.Ge, JJ
8.Jiang, Z
9.Chen, SL
10.Liu, CP
11.Xing, W
Recommended Citation
GB/T 7714
Xiao, ML,Zhang, H,Chen, YT,et al. Identification of binuclear Co2N5 active sites for oxygen reduction reaction with more than one magnitude higher activity than single atom CoN4 site[J]. NANO ENERGY,2018,46:396-403.
APA Xiao, ML.,Zhang, H.,Chen, YT.,Zhu, JB.,Gao, LQ.,...&Xing, W.(2018).Identification of binuclear Co2N5 active sites for oxygen reduction reaction with more than one magnitude higher activity than single atom CoN4 site.NANO ENERGY,46,396-403.
MLA Xiao, ML,et al."Identification of binuclear Co2N5 active sites for oxygen reduction reaction with more than one magnitude higher activity than single atom CoN4 site".NANO ENERGY 46(2018):396-403.
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