Identification of Highly Active Fe Sites in (Ni,Fe)OOH for Electrocatalytic Water Splitting

被引：2188

作者：

Friebel, Daniel ^{[1
,3
]}

Louie, Mary W. ^{[1
,2
]}

Bajdich, Michal ^{[3
]}

Sanwald, Kai E. ^{[3
,4
]}

Cai, Yun ^{[1
,2
]}

Wise, Anna M. ^{[5
]}

Cheng, Mu-Jeng ^{[1
,2
]}

Sokaras, Dimosthenis ^{[5
]}

Weng, Tsu-Chien ^{[5
]}

Alonso-Mori, Roberto ^{[6
]}

Davis, Ryan C. ^{[5
]}

Bargar, John R. ^{[5
]}

Norskov, Jens K. ^{[3
]}

Nilsson, Anders ^{[1
,3
,5
]}

Bell, Alexis T. ^{[1
,2
]}

机构：

[1] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Joint Ctr Artificial Photosynth, Berkeley, CA 94720 USA

[2] Univ Calif Berkeley, Dept Chem & Biomol Engn, Berkeley, CA 94720 USA

[3] SLAC Natl Accelerator Lab, SUNCAT Ctr Interface Sci & Catalysis, Menlo Pk, CA 94025 USA

[4] Tech Univ Munich, Dept Chem, D-85749 Garching, Germany

[5] SLAC Natl Accelerator Lab, Stanford Synchrotron Radiat Lightsource, Menlo Pk, CA 94025 USA

[6] SLAC Natl Accelerator Lab, Linac Coherent Lightsource, Menlo Pk, CA 94025 USA

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2015年 / 137卷 / 03期

关键词：

ABSORPTION FINE-STRUCTURE; OXYGEN EVOLUTION REACTION; NICKEL-HYDROXIDE; ELECTRONIC-STRUCTURE; ELECTROCHEMICAL-BEHAVIOR; OXIDE ELECTROCATALYSTS; NEUTRON-DIFFRACTION; IRON; OXIDATION; SPECTROSCOPY;

D O I：

10.1021/ja511559d

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Highly active catalysts for the oxygen evolution reaction (OER) are required for the development of photoelectrochemical devices that generate hydrogen efficiently from water using solar energy. Here, we identify the origin of a 500-fold OER activity enhancement that can be achieved with mixed (Ni,Fe)oxyhydroxides (Ni1-xFexOOH) over their pure Ni and Fe parent compounds, resulting in one of the most active currently known OER catalysts in alkaline electrolyte. Operando X-ray absorption spectroscopy (XAS) using high energy resolution fluorescence detection (HERFD) reveals that Fe3+ in Ni1-xFexOOH occupies octahedral sites with unusually short Fe-O bond distances, induced by edge-sharing with surrounding [NiO6] octahedra. Using computational methods, we establish that this structural motif results in near optimal adsorption energies of OER intermediates and low overpotentials at Fe sites. By contrast, Ni sites in Ni1-xFexOOH are not active sites for the oxidation of water.

引用

页码：1305 / 1313

页数：9

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