Influence of Surface Adsorption on the Oxygen Evolution Reaction on IrO2(110)

被引:277
作者
Kuo, Ding-Yuan [1 ]
Kawasaki, Jason K. [2 ,3 ,5 ]
Nelson, Jocienne N. [2 ]
Kloppenburg, Jan [4 ]
Hautier, Geoffroy [4 ]
Shen, Kyle M. [2 ,3 ]
Schlom, Darrell G. [1 ,3 ]
Suntivich, Jin [1 ,3 ]
机构
[1] Cornell Univ, Dept Mat Sci & Engn, Ithaca, NY 14853 USA
[2] Cornell Univ, Atom & Solid State Phys Lab, Dept Phys, Ithaca, NY 14853 USA
[3] Kavli Inst Cornell Nanoscale Sci, Ithaca, NY 14853 USA
[4] Catholic Univ Louvain, ICMN, B-1348 Louvain La Neuve, Belgium
[5] Univ Wisconsin, Dept Mat Sci & Engn, 1509 Univ Ave, Madison, WI 53706 USA
基金
美国国家科学基金会;
关键词
IRIDIUM OXIDE-FILMS; DENSITY-FUNCTIONAL THEORY; TOTAL-ENERGY CALCULATIONS; X-RAY-ABSORPTION; WAVE BASIS-SET; ELECTROCHEMICAL OXIDATION; HYDROGEN ADSORPTION; REDUCTION ACTIVITY; SINGLE-CRYSTALS; WATER;
D O I
10.1021/jacs.6b11932
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
A catalyst functions by stabilizing reaction intermediates, usually through surface adsorption. In the oxygen evolution reaction (OER), surface oxygen adsorption plays an indispensable role in the electrocatalysis. The relationship between the adsorption energetics and OER kinetics, however, has not yet been experimentally measured. Herein we report an experimental relationship between the adsorption of surface oxygen and the kinetics of the OER on IrO2(110) epitaxially grown on a TiO2(110) single crystal. The high quality of the IrO2 film grown using molecular-beam epitaxy affords the ability to extract the surface oxygen adsorption and its impact on the OER. By examining a series of electrolytes, we find that the adsorption energy changes linearly with pH, which we attribute to the electrified interfacial water. We support this hypothesis by showing that an electrolyte salt modification can lead to an adsorption energy shift. The dependence of the adsorption energy on pH has implications for the OER kinetics, but it is not the only factor; the dependence of the OER electrocatalysis on pH stipulates two OER mechanisms, one operating in acidic solution and another operating in alkaline solution. Our work points to the subtle adsorption kinetics relationship in the OER and highlights the importance of the interfacial electrified interaction in electrocatalyst design.
引用
收藏
页码:3473 / 3479
页数:7
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