Optimizing Oxygen Reduction Catalyst Morphologies from First Principles
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 s...
| Main Authors: | , , , , , , , |
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| Other Authors: | |
| Format: | Article |
| Language: | en_US |
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American Chemical Society (ACS)
2017
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| Online Access: | http://hdl.handle.net/1721.1/109739 |
| _version_ | 1811088646831341568 |
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| author | Ahmad, Ehsan A. Tileli, Vasiliki Kramer, Denis Mallia, Giuseppe Stoerzinger, Kelsey A. Shao-Horn, Yang Kucernak, Anthony R. Harrison, Nicholas M. |
| author2 | Massachusetts Institute of Technology. Department of Mechanical Engineering |
| author_facet | Massachusetts Institute of Technology. Department of Mechanical Engineering Ahmad, Ehsan A. Tileli, Vasiliki Kramer, Denis Mallia, Giuseppe Stoerzinger, Kelsey A. Shao-Horn, Yang Kucernak, Anthony R. Harrison, Nicholas M. |
| author_sort | Ahmad, Ehsan A. |
| collection | MIT |
| description | 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. |
| first_indexed | 2024-09-23T14:05:18Z |
| format | Article |
| id | mit-1721.1/109739 |
| institution | Massachusetts Institute of Technology |
| language | en_US |
| last_indexed | 2024-09-23T14:05:18Z |
| publishDate | 2017 |
| publisher | American Chemical Society (ACS) |
| record_format | dspace |
| spelling | mit-1721.1/1097392022-09-28T18:20:41Z Optimizing Oxygen Reduction Catalyst Morphologies from First Principles Ahmad, Ehsan A. Tileli, Vasiliki Kramer, Denis Mallia, Giuseppe Stoerzinger, Kelsey A. Shao-Horn, Yang Kucernak, Anthony R. Harrison, Nicholas M. Massachusetts Institute of Technology. Department of Mechanical Engineering Shao-Horn, Yang Shao-Horn, Yang 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. 2017-06-08T14:54:44Z 2017-06-08T14:54:44Z 2015-06 2015-06 Article http://purl.org/eprint/type/JournalArticle 1932-7447 1932-7455 http://hdl.handle.net/1721.1/109739 Ahmad, Ehsan A. et al. “Optimizing Oxygen Reduction Catalyst Morphologies from First Principles.” The Journal of Physical Chemistry C 119.29 (2015): 16804–16810. en_US http://dx.doi.org/10.1021/acs.jpcc.5b05460 The Journal of Physical Chemistry C 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. application/pdf American Chemical Society (ACS) Prof. Shao-Horn via Angie Locknar |
| spellingShingle | Ahmad, Ehsan A. Tileli, Vasiliki Kramer, Denis Mallia, Giuseppe Stoerzinger, Kelsey A. Shao-Horn, Yang Kucernak, Anthony R. Harrison, Nicholas M. Optimizing Oxygen Reduction Catalyst Morphologies from First Principles |
| title | Optimizing Oxygen Reduction Catalyst Morphologies from First Principles |
| title_full | Optimizing Oxygen Reduction Catalyst Morphologies from First Principles |
| title_fullStr | Optimizing Oxygen Reduction Catalyst Morphologies from First Principles |
| title_full_unstemmed | Optimizing Oxygen Reduction Catalyst Morphologies from First Principles |
| title_short | Optimizing Oxygen Reduction Catalyst Morphologies from First Principles |
| title_sort | optimizing oxygen reduction catalyst morphologies from first principles |
| url | http://hdl.handle.net/1721.1/109739 |
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