Towards identifying the active sites on RuO2(110) in catalyzing oxygen evolution

被引：356

作者：

Rao, Reshma R. ^{[1
]}

Kolb, Manuel J. ^{[2
,12
,13
]}

Halck, Niels Bendtsen ^{[3
]}

Pedersen, Anders Filsoe ^{[4
]}

Mehta, Apurva ^{[5
]}

You, Hoydoo ^{[6
]}

Stoerzinger, Kelsey A. ^{[7
,14
]}

Feng, Zhenxing ^{[8
]}

Hansen, Heine A. ^{[3
]}

Zhou, Hua ^{[9
]}

Giordano, Livia ^{[1
,10
]}

Rossmeisl, Jan ^{[11
]}

Vegge, Tejs ^{[3
]}

Chorkendorff, Ib ^{[4
]}

Stephens, Ifan E. L. ^{[4
,15
]}

Shao-Horn, Yang ^{[1
,2
,7
]}

机构：

[1] MIT, Dept Mech Engn, Cambridge, MA 02139 USA

[2] MIT, Elect Res Lab, Cambridge, MA 02139 USA

[3] Tech Univ Denmark, Dept Energy Convers & Storage, DK-2800 Lyngby, Denmark

[4] Tech Univ Denmark, Dept Phys, Sect Surface Phys & Catalysis, DK-2800 Lyngby, Denmark

[5] SLAC Natl Accelerator Lab, Menlo Pk, CA 94025 USA

[6] Argonne Natl Lab, Div Mat Sci, Argonne, IL USA

[7] MIT, Dept Mat Sci & Engn, Cambridge, MA 02139 USA

[8] Oregon State Univ, Sch Chem Biol & Environm Engn, Corvallis, OR 97331 USA

[9] Argonne Natl Lab, Xray Sci Div, 9700 S Cass Ave, Argonne, IL 60439 USA

[10] Univ Milano Bicocca, Dipartimento Sci Mat, Milan, Italy

[11] Univ Copenhagen, Dept Chem, Univ Pk 5, DK-2100 Copenhagen, Denmark

[12] Stockholm Univ, AlbaNova, FYSIKUM, S-10691 Stockholm, Sweden

[13] Stanford Univ, SUNCAT Ctr Interface Sci & Catalysis, Dept Chem Engn, 443 Via Ortega, Stanford, CA 94305 USA

[14] Pacific Northwest Natl Lab, Phys & Computat Sci Directorate, Richland, WA 99354 USA

[15] Imperial Coll London, Royal Sch Mines, South Kensington Campus, London SW 2AZ, England

来源：

ENERGY & ENVIRONMENTAL SCIENCE | 2017年 / 10卷 / 12期

基金：

美国国家科学基金会;

关键词：

INITIO MOLECULAR-DYNAMICS; X-RAY-REFLECTIVITY; RUTHENIUM DIOXIDE; SINGLE-CRYSTAL; SURFACE-CHEMISTRY; WATER; OXIDE; RUO2; OXIDATION; ELECTROCATALYSIS;

D O I：

10.1039/c7ee02307c

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

While the surface atomic structure of RuO2 has been well studied in ultra high vacuum, much less is known about the interaction between water and RuO2 in aqueous solution. In this work, in situ surface X-ray scattering measurements combined with density functional theory (DFT) were used to determine the surface structural changes on single-crystal RuO2(110) as a function of potential in acidic electrolyte. The redox peaks at 0.7, 1.1 and 1.4 V vs. reversible hydrogen electrode (RHE) could be attributed to surface transitions associated with the successive deprotonation of -H2O on the coordinatively unsaturated Ru sites (CUS) and hydrogen adsorbed to the bridging oxygen sites. At potentials relevant to the oxygen evolution reaction (OER), an -OO species on the Ru CUS sites was detected, which was stabilized by a neighboring -OH group on the Ru CUS or bridge site. Combining potential-dependent surface structures with their energetics from DFT led to a new OER pathway, where the deprotonation of the -OH group used to stabilize -OO was found to be rate-limiting.

引用

页码：2626 / 2637

页数：12

共 76 条

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