The reaction mechanism with free energy barriers at constant potentials for the oxygen evolution reaction at the IrO2 (110) surface
Abstract
Complex charge transfer processes, high overpotential, and corrosion make it difficult to efficiently oxidize H2O to O2 (Oxygen Evolution Reaction, OER) in photoelectrochemical cells (PEC). So far no OER mechanism has been fully explained atomistically with both thermodynamic and kinetics. IrO2 is the only known OER catalyst with both high catalytic activity and stability in acidic conditions. This is important because PEC experiments often operate at extreme pH conditions. Here, we performed first principles calculations integrated with implicit solvation at constant potentials to examine the detailed atomistic reaction mechanism of OER at the IrO2 (110) surface. We also determined the surface phase diagram, explored the possible reaction pathways including kinetic barriers, and computed reaction rates based on the micro-kinetic models. This allowed us to resolve several long-standing puzzles about the atomistic OER mechanism.
- Authors:
-
[2]
- California Inst. of Technology (CalTech), Pasadena, CA (United States); Univ. of California, Santa Cruz, CA (United States)
- California Inst. of Technology (CalTech), Pasadena, CA (United States)
- Publication Date:
- Research Org.:
- California Institute of Technology (CalTech), Pasadena, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1346958
- Alternate Identifier(s):
- OSTI ID: 1347420
- Grant/Contract Number:
- SC0004993; AC02-05CH11231; SC004993
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 139; Journal Issue: 1; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE
Citation Formats
Ping, Yuan, Nielsen, Robert J., and Goddard, William A. The reaction mechanism with free energy barriers at constant potentials for the oxygen evolution reaction at the IrO2 (110) surface. United States: N. p., 2016.
Web. doi:10.1021/jacs.6b07557.
Ping, Yuan, Nielsen, Robert J., & Goddard, William A. The reaction mechanism with free energy barriers at constant potentials for the oxygen evolution reaction at the IrO2 (110) surface. United States. https://doi.org/10.1021/jacs.6b07557
Ping, Yuan, Nielsen, Robert J., and Goddard, William A. Fri .
"The reaction mechanism with free energy barriers at constant potentials for the oxygen evolution reaction at the IrO2 (110) surface". United States. https://doi.org/10.1021/jacs.6b07557. https://www.osti.gov/servlets/purl/1346958.
@article{osti_1346958,
title = {The reaction mechanism with free energy barriers at constant potentials for the oxygen evolution reaction at the IrO2 (110) surface},
author = {Ping, Yuan and Nielsen, Robert J. and Goddard, William A.},
abstractNote = {Complex charge transfer processes, high overpotential, and corrosion make it difficult to efficiently oxidize H2O to O2 (Oxygen Evolution Reaction, OER) in photoelectrochemical cells (PEC). So far no OER mechanism has been fully explained atomistically with both thermodynamic and kinetics. IrO2 is the only known OER catalyst with both high catalytic activity and stability in acidic conditions. This is important because PEC experiments often operate at extreme pH conditions. Here, we performed first principles calculations integrated with implicit solvation at constant potentials to examine the detailed atomistic reaction mechanism of OER at the IrO2 (110) surface. We also determined the surface phase diagram, explored the possible reaction pathways including kinetic barriers, and computed reaction rates based on the micro-kinetic models. This allowed us to resolve several long-standing puzzles about the atomistic OER mechanism.},
doi = {10.1021/jacs.6b07557},
journal = {Journal of the American Chemical Society},
number = 1,
volume = 139,
place = {United States},
year = {Fri Dec 09 00:00:00 EST 2016},
month = {Fri Dec 09 00:00:00 EST 2016}
}
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