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Finding Correlations of the Oxygen Reduction Reaction Activity of Transition Metal Catalysts with Parameters Obtained from Quantum Mechanics

Yu, Ted H. and Hofmann, Timo and Sha, Yao and Merinov, Boris V. and Myers, Deborah J. and Heske, Clemens and Goddard, William A., III (2013) Finding Correlations of the Oxygen Reduction Reaction Activity of Transition Metal Catalysts with Parameters Obtained from Quantum Mechanics. Journal of Physical Chemistry C, 117 (50). pp. 26598-26607. ISSN 1932-7447. doi:10.1021/jp4071554. https://resolver.caltech.edu/CaltechAUTHORS:20140124-111244709

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Abstract

To facilitate a less empirical approach to developing improved catalysts, it is important to correlate catalytic performance to surrogate properties that can be measured or predicted accurately and quickly, allowing experimental synthesis and testing of catalysts to focus on the most promising cases. Particularly hopeful is correlating catalysis performance to the electronic density of states (DOS). Indeed, there has been success in using just the center of the d-electron density, which in some cases correlates linearly with oxygen atom chemisorption energy, leading to a volcano plot for catalytic performance versus “d-band center”. To test such concepts we calculated the barriers and binding energies for the various reactions and intermediates involved in the oxygen reduction reaction (ORR) for all 12 transition metals in groups 8–11 (Fe–Cu columns). Our results show that the oxygen binding energy can serve as a useful parameter in describing the catalytic activity for pure metals, but it does not necessarily correlate with the d-band center. In addition, we find that the d-band center depends substantially on the calculation method or the experimental setup, making it a much less reliable indicator for ORR activity than the oxygen binding energy. We further examine several surfaces of the same pure metals to evaluate how the d-band center and oxygen binding energy depend on the surface.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1021/jp4071554DOIArticle
http://pubs.acs.org/doi/abs/10.1021/jp4071554PublisherArticle
ORCID:
AuthorORCID
Yu, Ted H.0000-0003-3202-0981
Merinov, Boris V.0000-0002-2783-4262
Goddard, William A., III0000-0003-0097-5716
Additional Information:© 2013 American Chemical Society. Received: July 18, 2013; revised: November 21, 2013; published: November 25, 2013. We gratefully acknowledge funding by the U.S. Department of Energy, Prime Contract No. DE-AC02-06CH11357 (ANL) and ANL Subcontract Nos. 7F-01041 (UNLV) and 7F-01321 (Caltech), and National Science Foundation (Grant CBET-1067848, Caltech). The facilities of the Materials and Process Simulation Center used in this study were established with grants from DURIP-ONR, DURIP-ARO, and NSF-CSEM.
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE-AC02-06CH11357
Argonne National Laboratory7F-01041
Argonne National Laboratory7F-01321
NSFCBET-1067848
Office of Naval Research (ONR)UNSPECIFIED
Army Research Office (ARO)UNSPECIFIED
Issue or Number:50
DOI:10.1021/jp4071554
Record Number:CaltechAUTHORS:20140124-111244709
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20140124-111244709
Official Citation:Finding Correlations of the Oxygen Reduction Reaction Activity of Transition Metal Catalysts with Parameters Obtained from Quantum Mechanics Ted H. Yu, Timo Hofmann, Yao Sha, Boris V. Merinov, Deborah J. Myers, Clemens Heske, and William A. Goddard, III The Journal of Physical Chemistry C 2013 117 (50), 26598-26607
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:43511
Collection:CaltechAUTHORS
Deposited By: Jason Perez
Deposited On:24 Jan 2014 21:47
Last Modified:10 Nov 2021 16:38

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