Hydrogen Evolution on Supported Incomplete Cubane-type [Mo3S4]4+ Electrocatalysts

被引：203

作者：

Jaramillo, Thomas F. ^{[3
]}

Bonde, Jacob ^{[1
]}

Zhang, Jingdong ^{[2
]}

Ooi, Bee-Lean ^{[2
]}

Andersson, Klas ^{[1
]}

Ulstrup, Jens ^{[2
]}

Chorkendorff, Ib ^{[1
]}

机构：

[1] Tech Univ Denmark, CINF, Dept Phys, DK-2800 Lyngby, Denmark

[2] Tech Univ Denmark, Dept Chem, DK-2800 Lyngby, Denmark

[3] Stanford Univ, Dept Chem Engn, Stanford, CA 94305 USA

来源：

JOURNAL OF PHYSICAL CHEMISTRY C | 2008年 / 112卷 / 45期

基金：

新加坡国家研究基金会;

关键词：

D O I：

10.1021/jp802695e

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Electrocatalytic properties of biomimetic supported incomplete cubane-type [Mo3S4](4+) clusters are investigated. The activity toward the hydrogen evolution reaction (HER) is evaluated on both a high surface area gas diffusion electrode in a membrane electrode assembly and on highly orientated pyrolytic graphite (HOPG) supports. Sub-monolayers of the clusters were imaged by means of scanning tunnelling microscopy (STM) prior to electrochemical characterization. This enabled the quantification of the activity on a per cluster basis for the HER and the comparison of the activity with other HER catalysts. We find that the HER activity of the [Mo3S4](4+) is comparable with that of the edge sites of MoS2. The supported [Mo3S4](4+) molecules were also characterized by X-ray photoelectron spectroscopy (XPS), and the observed deterioration in electrocatalytic activity with time was assigned to slow [Mo3S4](4+) cathodic desorption from the catalyst support.

引用

页码：17492 / 17498

页数：7

共 39 条

[1] Scaling properties of adsorption energies for hydrogen-containing molecules on transition-metal surfaces
Abild-Pedersen, F.
Greeley, J.
Studt, F.
Rossmeisl, J.
Munter, T. R.
Moses, P. G.
Skulason, E.
Bligaard, T.
Norskov, J. K.
[J]. PHYSICAL REVIEW LETTERS, 2007, 99 (01)
[2] Recent developments in dynamic electrochemical studies of adsorbed enzymes and their active sites
Armstrong, FA
[J]. CURRENT OPINION IN CHEMICAL BIOLOGY, 2005, 9 (02) : 110 - 117
[3] The Bronsted-Evans-Polanyi relation and the volcano curve in heterogeneous catalysis
Bligaard, T
Norskov, JK
Dahl, S
Matthiesen, J
Christensen, CH
Sehested, J
[J]. JOURNAL OF CATALYSIS, 2004, 224 (01) : 206 - 217
[4] Hydrogen evolution on nano-particulate transition metal sulfides
Bonde, Jacob
Moses, Poul G.
Jaramillo, Thomas F.
Norskov, Jens K.
Chorkendorff, Ib
[J]. FARADAY DISCUSSIONS, 2008, 140 : 219 - 231
[5] Long-range interfacial electron transfer of metalloproteins based on molecular wiring assemblies
Chi, QJ
Zhang, JD
Jensen, PS
Christensen, HEM
Ulstrup, J
[J]. FARADAY DISCUSSIONS, 2006, 131 : 181 - 195
[6] Long-range protein electron transfer observed at the single-molecule level:: In situ mapping of redox-gated tunneling resonance
Chi, QJ
Farver, O
Ulstrup, J
[J]. PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2005, 102 (45) : 16203 - 16208
[7] Electrochemical reduction of NO by hemin adsorbed at pyrolitic graphite
de Groot, MT
Merkx, M
Wonders, AH
Koper, MTM
[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2005, 127 (20) : 7579 - 7586
[8] Alternative energy technologies
Dresselhaus, MS
Thomas, IL
[J]. NATURE, 2001, 414 (6861) : 332 - 337
[9] Computational high-throughput screening of electrocatalytic materials for hydrogen evolution
Greeley, Jeff
Jaramillo, Thomas F.
Bonde, Jacob
Chorkendorff, I. B.
Norskov, Jens K.
[J]. NATURE MATERIALS, 2006, 5 (11) : 909 - 913
[10] Hydrogen evolution over bimetallic systems: Understanding the trends
Greeley, Jeff
Norskov, Jens K.
Kibler, Ludwig A.
El-Aziz, Ahmed M.
Kolb, Dieter M.
[J]. CHEMPHYSCHEM, 2006, 7 (05) : 1032 - 1035

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