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Enhanced proton and electron reservoir abilities of polyoxometalate grafted on graphene for high-performance hydrogen evolution
Liu, Rongji1; Zhang, Guangjin1; Cao, Hongbin1; Zhang, Suojiang1; Xie, Yongbing1; Haider, Ali2; Kortz, Ulrich2; Chen, Banghao3; Dalal, Naresh S.3; Zhao, Yongsheng4; Zhi, Linjie5; Wu, Cai-Xia6; Yan, Li-Kai6; Su, Zhongmin6; Keita, Bineta7
2016
Source PublicationENERGY & ENVIRONMENTAL SCIENCE
ISSN1754-5692
Volume9Issue:3Pages:1012-1023
Abstract

A beneficial "microenvironment effect" on the efficiency of confined electrocatalysts is predicted by theory. However, examples of its experimental confirmation are scarce for catalysts based on polyoxometalates for the hydrogen evolution reaction (HER). For this purpose, the cyclic 48-tungsto-8-phosphate [H7P8W48O184](33) (P8W48) was fixed in a 3D configuration on reduced graphene oxide sheets (rGO) to boost its HER activity. The HRTEM imaging and the solid state P-31 NMR spectrum of P8W48/rGO reveal a strong interaction between individual P8W48 and transparent rGO sheets. The calculation of the interaction between P8W48 and graphene (G) sheets is difficult to perform within a reasonable period of time because of the large size and very high overall negative charge of P8W48. However, as P8W48 is symmetrical, a quarter of its structure [H2P2W12O48](12-) (P2W12) was extracted as a DFT calculation model. As P8W48 in P8W48/rGO is neutral, due to surrounding counter cations, the calculation model P2W12 is neutral with protons considering the affordable computational time. The adsorption energy for P2W12 on G (-1.55 eV) and the charge transfer between P2W12 and G (0.66 vertical bar e vertical bar) indicate that a strong interaction between P2W12 and G sheets exists. Kinetic studies show that the P8W48/rGO hybrids display excellent HER activity in acid, further confirmed by reproducible generation of hydrogen with quantitative faradaic yield and a high turnover frequency (11 s(-1) at 295 mV overpotential) for a noble metal-free electrocatalyst. Importantly, the overpotentials required for the HER compare well with those of the commercial Pt/C (20 wt% Pt), which indicates that P8W48/rGO is a promising cheap HER electrocatalyst. We demonstrate here the most convincing experimental evidence of the "microenvironment effect" on HER electrocatalysis by a polyoxometalate.

KeywordMetal-organic Frameworks Crown Heteropolyanion Nanosheets Catalyst Oxide Water Mos2 Electrocatalysis Nanocomposite Behavior
SubtypeArticle
Subject AreaChemistry, Multidisciplinary ; Energy & Fuels ; Engineering, Chemical ; Environmental Sciences ; Chemistry ; Energy & Fuels ; Engineering ; Environmental Sciences & Ecology
WOS HeadingsScience & Technology ; Physical Sciences ; Technology ; Life Sciences & Biomedicine
DOI10.1039/c5ee03503a
URL查看原文
Indexed BySCI
Language英语
WOS KeywordMetal-organic Frameworks ; Crown Heteropolyanion ; Nanosheets ; Catalyst ; Oxide ; Water ; Mos2 ; Electrocatalysis ; Nanocomposite ; Behavior
WOS Research AreaChemistry ; Energy & Fuels ; Engineering ; Environmental Sciences & Ecology
WOS SubjectChemistry, Multidisciplinary ; Energy & Fuels ; Engineering, Chemical ; Environmental Sciences
Funding OrganizationNational Natural Science Foundation of China(21371173 ; China Postdoctoral Foundation(2014M550846) ; Chinese Academy of Sciences President's International Fellowship Initiative(2015VMA041) ; Jacobs University ; German Science Foundation(DFG KO-2288/20-1) ; German Academic Exchange Service (DAAD) ; Florida State University ; U.S. NSF Major Research Instrumentation (MRI) program(NSF 1126587) ; 51402298 ; 91545125)
WOS IDWOS:000372243600031
Citation statistics
Cited Times:68[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.ipe.ac.cn/handle/122111/20676
Collection研究所(批量导入)
Corresponding AuthorZhang, Guangjin
Affiliation1.Chinese Acad Sci, Inst Proc Engn, Key Lab Green Proc & Engn, Beijing 100190, Peoples R China
2.Jacobs Univ Bremen, Dept Life Sci & Chem, POB 750 561, D-28725 Bremen, Germany
3.Florida State Univ, Dept Chem & Biochem, Tallahassee, FL 32306 USA
4.Chinese Acad Sci, Inst Chem, Key Lab Photochem, BNLMS, Beijing 100190, Peoples R China
5.Natl Ctr Nanosci & Technol, Key Lab Nanosyst & Hierarch Fabricat, Beijing 100190, Peoples R China
6.NE Normal Univ, Fac Chem, Changchun 130024, Peoples R China
7.Univ Paris 11, CNRS, UMR 8000, Chim Phys Lab, F-91405 Orsay, France
Recommended Citation
GB/T 7714
Liu, Rongji,Zhang, Guangjin,Cao, Hongbin,et al. Enhanced proton and electron reservoir abilities of polyoxometalate grafted on graphene for high-performance hydrogen evolution[J]. ENERGY & ENVIRONMENTAL SCIENCE,2016,9(3):1012-1023.
APA Liu, Rongji.,Zhang, Guangjin.,Cao, Hongbin.,Zhang, Suojiang.,Xie, Yongbing.,...&Keita, Bineta.(2016).Enhanced proton and electron reservoir abilities of polyoxometalate grafted on graphene for high-performance hydrogen evolution.ENERGY & ENVIRONMENTAL SCIENCE,9(3),1012-1023.
MLA Liu, Rongji,et al."Enhanced proton and electron reservoir abilities of polyoxometalate grafted on graphene for high-performance hydrogen evolution".ENERGY & ENVIRONMENTAL SCIENCE 9.3(2016):1012-1023.
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