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Highly active, stable oxidized platinum clusters as electrocatalysts for the hydrogen evolution reaction
Cheng, Xing1; Li, Yonghe2; Zheng, Lirong3; Yan, Yong4,5; Zhang, Yuefei2; Chen, Ge1; Sun, Shaorui1; Zhang, Jiujun6,7
刊名Energy & environmental science
2017-11-01
卷号10期号:11页码:2450-2458
ISSN号1754-5692
DOI10.1039/c7ee02537h
通讯作者Chen, ge(chenge@bjut.edu.cn) ; Sun, shaorui(sunsr@bjut.edu.cn) ; Zhang, jiujun(jiujun@shaw.ca)
英文摘要In the present work, we synthesized and characterized an electrocatalyst consisting of sub-nanometric pt clusters uniformly dispersed on a tio2 support. x-ray photoelectron spectra (xps) and x-ray adsorption fine structure (xafs) data demonstrate that these sub-nanometric pt clusters are in a highly oxidized state and possess two localized pt-o coordination structures. the pt-o bonds between the oxidized pt clusters and the tio2 give rise to a strong metal-support interaction (smsi). when applied to the hydrogen evolution reaction (her), this catalyst exhibits significantly enhanced catalytic activity (increased by a factor of up to 8.4) and enhanced stability compared with the state-of-the-art commercial pt/c catalysts. particularly, the additional xps and xafs characterizations of the catalyst after long-term electrolysis demonstrate the absence of metallic pt species, confirming that the catalytic active site comes from the oxidized pt clusters rather than from the the metallic pt species. this improved performance is considered to be induced by the unique electronic structure of the oxidized pt clusters and by the smsi. based on the results of density functional theory calculations, the 5d orbital of the oxidized pt cluster atoms appears to hybridize with the h 1s orbital to form weak pt-h valence bonds, leading to a dg (relative free energy) value of approximately zero ev for h* absorption. this effect explains the mechanism responsible for the excellent catalytic activity of these oxidized pt clusters for the her. this work therefore provides important insights into the role of oxidized pt clusters as an her electrocatalyst. the evident stabilization of the oxidized pt clusters on tio2 supports via the charge-transfer mechanism provides a useful approach for improving the durability of electrocatalysts that may be applicable to other noble metal/support systems.
WOS关键词METAL-SUPPORT INTERACTION ; CO OXIDATION ; SINGLE-ATOM ; OXYGEN REDUCTION ; CATALYSTS ; NANOPARTICLES ; EFFICIENCY ; SURFACE ; NANOCLUSTERS ; STABILITY
WOS研究方向Chemistry ; Energy & Fuels ; Engineering ; Environmental Sciences & Ecology
WOS类目Chemistry, Multidisciplinary ; Energy & Fuels ; Engineering, Chemical ; Environmental Sciences
语种英语
出版者ROYAL SOC CHEMISTRY
WOS记录号WOS:000414774500018
内容类型期刊论文
URI标识http://www.corc.org.cn/handle/1471x/2176917
专题高能物理研究所
通讯作者Chen, Ge; Sun, Shaorui; Zhang, Jiujun
作者单位1.Beijing Univ Technol, Coll Environm & Energy Engn, Beijing Key Lab Green Catalysis & Separat, Beijing 100124, Peoples R China
2.Beijing Univ Technol, Inst Microstruct & Property Adv Mat, Beijing 100124, Peoples R China
3.Chinese Acad Sci, Inst High Energy Phys, Beijing Synchrotron Radiat Facil, Beijing 100049, Peoples R China
4.Nanjing Univ Sci & Technol, Minist Educ, Dept Appl Phys, Nanjing 210094, Jiangsu, Peoples R China
5.Nanjing Univ Sci & Technol, Minist Educ, Key Lab Soft Chem & Funct Mat, Nanjing 210094, Jiangsu, Peoples R China
6.Shanghai Univ, Coll Sci, Shanghai 200444, Peoples R China
7.Shanghai Univ, Inst Sustainable Energy, Shanghai 200444, Peoples R China
推荐引用方式
GB/T 7714
Cheng, Xing,Li, Yonghe,Zheng, Lirong,et al. Highly active, stable oxidized platinum clusters as electrocatalysts for the hydrogen evolution reaction[J]. Energy & environmental science,2017,10(11):2450-2458.
APA Cheng, Xing.,Li, Yonghe.,Zheng, Lirong.,Yan, Yong.,Zhang, Yuefei.,...&Zhang, Jiujun.(2017).Highly active, stable oxidized platinum clusters as electrocatalysts for the hydrogen evolution reaction.Energy & environmental science,10(11),2450-2458.
MLA Cheng, Xing,et al."Highly active, stable oxidized platinum clusters as electrocatalysts for the hydrogen evolution reaction".Energy & environmental science 10.11(2017):2450-2458.
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