Optimizing Oxygen Reduction Catalyst Morphologies from First Principles
Name
optimizing-oxygen-reduction.pdf
Size
7.43 MB
Format
Adobe PDF
Checksum (MD5)
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Author(s)
Ahmad, Ehsan A.
Tileli, Vasiliki
Kramer, Denis
Mallia, Giuseppe
Stoerzinger, Kelsey A.
Shao-Horn, Yang
Kucernak, Anthony R.
Harrison, Nicholas M.
Date Issued
June 2015
Journal
The Journal of Physical Chemistry C
Publisher
American Chemical Society (ACS)
Citation
Ahmad, Ehsan A. et al. “Optimizing Oxygen Reduction Catalyst Morphologies from First Principles.” The Journal of Physical Chemistry C 119.29 (2015): 16804–16810.
Version
Author's final manuscript
Abstract
Catalytic activity of perovskites for oxygen reduction (ORR) was recently correlated with bulk d-electron occupancy of the transition metal. We expand on the resultant model, which successfully reproduces the high activity of LaMnO[subscript 3] relative to other perovskites, by addressing catalyst surface morphology as an important aspect of the optimal ORR catalyst. The nature of reaction sites on low index surfaces of orthorhombic (Pnma) LaMnO[subscript 3] is established from First Principles. The adsorption of O[subscript 2] is markedly influenced by local geometry and strong electron correlation. Only one of the six reactions sites that result from experimentally confirmed symmetry-breaking Jahn–Teller distortions is found to bind O[subscript 2] with an intermediate binding energy while facilitating the formation of superoxide, an important ORR intermediate in alkaline media. As demonstrated here for LaMnO[subscript 3], rational design of the catalyst morphology to promote specific active sites is a highly effective optimization strategy for advanced functional ORR catalysts.
MIT Department
Massachusetts Institute of Technology. Department of Mechanical Engineering
Terms of Use
Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use.
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DOI of Published Version
https://doi.org/10.1021/acs.jpcc.5b05460
