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Coordination-controlled single-atom tungsten as a non-3d-metal oxygen reduction reaction electrocatalyst with ultrahigh mass activity
Chen, Zhigang1,2; Gong, Wenbin2; Liu, Zhibo3; Cong, Shan1,2; Zheng, Zuhui1,2; Wang, Zhen1,2; Zhang, Wei4; Ma, Jingyuan5; Yu, Haisheng5; Li, Guihang6; Lu, Weibang1,2; Ren, Wencai3; Zhao, Zhigang1,2,7
Corresponding AuthorZhao, Zhigang(zgzhao2011@sinano.ac.cn)
2019-06-01
Source PublicationNANO ENERGY
ISSN2211-2855
Volume60Pages:394-403
AbstractTransition metal-nitrogen-carbon (M-N-C) catalysts have emerged as the most promising alternatives to their costly platinum-based counterparts for oxygen reduction reaction (ORR) catalysis, which are critical to renewable energy conversion and storage technologies. However, thus far, only 3d transition metals (Co, Fe, Ni, Mn, etc.) have often been good choices for the metal elements in such M-N-C catalysts, while other non-3d transition metals-based catalysts such as 5d tungsten (W) usually afford much inferior ORR activities in both bulk and nanoparticle form. Here, we report the atomically dispersed tungsten on nitrogen-doped carbon nanosheets with controlled W-N coordination numbers as efficient catalysts for ORRs, which are only formed through the deliberate modulation of the synthesis parameters, such as the pyrolysis atmosphere, temperature, and time, within a very narrow range. Instead of being considered to be almost inactive towards ORR, the single-atom tungsten electrocatalysts show remarkable, durable and coordination number-sensitive ORR catalytic ability. It is shown that single-atom tungsten with a W-N coordination number of 5 exhibits markedly high ORR catalytic activity in 0.1 M KOH with onset potential ( similar to 1.01 V), half-wave potential (0.88 V) and a mass activity of 0.63 A/mg (at 0.9 V versus RHE), which even surpasses those of commercial Pt/C. Meanwhile, the WN5 catalyst catalyzes the ORR with a onset potential of 0.87 V and a half-wave potential of 0.77V in 0.1 M HClO4, both of which are nearly comparable to the benchmark Pt/C. In contrast, the single-atom tungsten electrocatalysts with W-N coordination numbers of 3 and 4 exhibit relatively poor ORR activity in both acidic and alkaline electrolytes. The DFT calculations suggest that the sharp increase in the ORR activity of the single-atom tungsten catalysts can be attributed to the moderate interaction between OH- and the single W atoms, which is probably caused by the optimal dz(2)-pz orbital hybridization and re-distribution of the charges.
KeywordMetal-nitrogen-carbon catalysts Single-atom tungsten Electrocatalytic oxygen reduction Coordination environment
Funding OrganizationNational Natural Science Foundation of China ; Outstanding Youth Fund of Jiangsu Province ; National Key Research and Development Program of China ; Youth Innovation Promotion Association, CAS ; Natural Science Foundation of Jiangxi Province ; Science and Technology Project of Nanchang
DOI10.1016/j.nanoen.2019.03.045
Indexed BySCI
Language英语
Funding ProjectNational Natural Science Foundation of China[51572286] ; National Natural Science Foundation of China[21503266] ; National Natural Science Foundation of China[51772319] ; National Natural Science Foundation of China[51772320] ; Outstanding Youth Fund of Jiangsu Province[BK20160011] ; National Key Research and Development Program of China[2016YFA0203301] ; Youth Innovation Promotion Association, CAS[2018356] ; Natural Science Foundation of Jiangxi Province[20181ACB20011] ; Science and Technology Project of Nanchang[2017-SJSYS-008]
WOS Research AreaChemistry ; Science & Technology - Other Topics ; Materials Science ; Physics
WOS SubjectChemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied
WOS IDWOS:000467774100044
PublisherELSEVIER SCIENCE BV
Citation statistics
Cited Times:34[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.imr.ac.cn/handle/321006/133608
Collection中国科学院金属研究所
Corresponding AuthorZhao, Zhigang
Affiliation1.Univ Sci & Technol China, Sch Nano Technol caul Nano Bion, Hefei 230026, Anhui, Peoples R China
2.Chinese Acad Sci, Suzhou Inst Nanotech & Nanobion, Key Lab Nanodevices & Applicat, Suzhou 215123, Peoples R China
3.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Liaoning, Peoples R China
4.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai 201800, Peoples R China
5.Chinese Acad Sci, Shanghai Inst Appl Phys, SSRF, Shanghai 201204, Peoples R China
6.Univ Sci & Technol China, NSRL, Hefei 230029, Anhui, Peoples R China
7.Chinese Acad Sci, Suzhou Inst Nanotech & Nanobion, Div Nanomat, Nanchang 330200, Jiangxi, Peoples R China
Recommended Citation
GB/T 7714
Chen, Zhigang,Gong, Wenbin,Liu, Zhibo,et al. Coordination-controlled single-atom tungsten as a non-3d-metal oxygen reduction reaction electrocatalyst with ultrahigh mass activity[J]. NANO ENERGY,2019,60:394-403.
APA Chen, Zhigang.,Gong, Wenbin.,Liu, Zhibo.,Cong, Shan.,Zheng, Zuhui.,...&Zhao, Zhigang.(2019).Coordination-controlled single-atom tungsten as a non-3d-metal oxygen reduction reaction electrocatalyst with ultrahigh mass activity.NANO ENERGY,60,394-403.
MLA Chen, Zhigang,et al."Coordination-controlled single-atom tungsten as a non-3d-metal oxygen reduction reaction electrocatalyst with ultrahigh mass activity".NANO ENERGY 60(2019):394-403.
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