Ab initio molecular dynamics of solvation effects on reactivity at electrified interfaces
Abstract
Significance Low-temperature fuel cells are efficient energy conversion devices that face a number of hurdles toward commercialization, including difficulties in storing hydrogen. Methanol represents a liquid-phase fuel alternative to hydrogen, yet the high cost of Pt-based catalysts limits fuel cells’ economic viability. Toward improved, lower-cost catalyst design, a fundamental understanding of the methanol electrooxidation reaction mechanism is necessary. Density functional theory calculations have become invaluable in elucidating these reaction mechanisms, although the complex reaction environment including solvation of a charged electrode has been a challenge to model. Using ab initio molecular dynamics, via the Blue Moon Ensemble, we have investigated methanol electrooxidation on a solvated and charged Pt(111) surface to understand the effect of solvation and charge on the reaction energetics.
- Authors:
-
- Department of Chemical and Biological Engineering, University of Wisconsin–Madison, Madison, WI 53706,
- Division of Precision Science &, Technology and Applied Physics, Osaka University, Osaka 565-0871, Japan
- Publication Date:
- Research Org.:
- Univ. of Wisconsin, Madison, WI (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); USDOE Office of Science (SC), Biological and Environmental Research (BER)
- Contributing Org.:
- EMSL, a National scientific user facility at Pacific Northwest National Laboratory (PNNL); the Center for Nanoscale Materials at Argonne National Laboratory (ANL); and the National Energy Research Scientific Computing Center (NERSC); Pacific Northwest National Laboratory (PNNL) (EMSL); Argonne National Laboratory (ANL) (CNM); Lawrence Berkeley National Laboratory (LBNL) (NERSC)
- OSTI Identifier:
- 1579289
- Alternate Identifier(s):
- OSTI ID: 1405318; OSTI ID: 1994811
- Grant/Contract Number:
- FG02-05ER15731; AC02-06CH11357; AC02-05CH11231
- Resource Type:
- Published Article
- Journal Name:
- Proceedings of the National Academy of Sciences of the United States of America
- Additional Journal Information:
- Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 113 Journal Issue: 34; Journal ID: ISSN 0027-8424
- Publisher:
- Proceedings of the National Academy of Sciences
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; AIMD; DFT; methanol; Pt(111); electrocatalysis; density functional theory
Citation Formats
Herron, Jeffrey A., Morikawa, Yoshitada, and Mavrikakis, Manos. Ab initio molecular dynamics of solvation effects on reactivity at electrified interfaces. United States: N. p., 2016.
Web. doi:10.1073/pnas.1604590113.
Herron, Jeffrey A., Morikawa, Yoshitada, & Mavrikakis, Manos. Ab initio molecular dynamics of solvation effects on reactivity at electrified interfaces. United States. https://doi.org/10.1073/pnas.1604590113
Herron, Jeffrey A., Morikawa, Yoshitada, and Mavrikakis, Manos. Mon .
"Ab initio molecular dynamics of solvation effects on reactivity at electrified interfaces". United States. https://doi.org/10.1073/pnas.1604590113.
@article{osti_1579289,
title = {Ab initio molecular dynamics of solvation effects on reactivity at electrified interfaces},
author = {Herron, Jeffrey A. and Morikawa, Yoshitada and Mavrikakis, Manos},
abstractNote = {Significance Low-temperature fuel cells are efficient energy conversion devices that face a number of hurdles toward commercialization, including difficulties in storing hydrogen. Methanol represents a liquid-phase fuel alternative to hydrogen, yet the high cost of Pt-based catalysts limits fuel cells’ economic viability. Toward improved, lower-cost catalyst design, a fundamental understanding of the methanol electrooxidation reaction mechanism is necessary. Density functional theory calculations have become invaluable in elucidating these reaction mechanisms, although the complex reaction environment including solvation of a charged electrode has been a challenge to model. Using ab initio molecular dynamics, via the Blue Moon Ensemble, we have investigated methanol electrooxidation on a solvated and charged Pt(111) surface to understand the effect of solvation and charge on the reaction energetics.},
doi = {10.1073/pnas.1604590113},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 34,
volume = 113,
place = {United States},
year = {Mon Aug 08 00:00:00 EDT 2016},
month = {Mon Aug 08 00:00:00 EDT 2016}
}
https://doi.org/10.1073/pnas.1604590113
Web of Science
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