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Title: Tailoring manganese oxide with atomic precision to increase surface site availability for oxygen reduction catalysis

Abstract

Controlling the structure of catalysts at the atomic level provides an opportunity to establish detailed understanding of the catalytic form-to-function and realize new, non-equilibrium catalytic structures. Here, advanced thin-film deposition is used to control the atomic structure of La 2/3Sr 1/3MnO 3, a well-known catalyst for the oxygen reduction reaction. The surface and sub-surface is customized, whereas the overall composition and d-electron configuration of the oxide is kept constant. Although the addition of SrMnO 3 benefits the oxygen reduction reaction via electronic structure and conductivity improvements, SrMnO 3 can react with ambient air to reduce the surface site availability. Placing SrMnO 3 in the sub-surface underneath a LaMnO 3 overlayer allows the catalyst to maintain the surface site availability while benefiting from improved electronic effects. The results show the promise of advanced thin-film deposition for realizing atomically precise catalysts, in which the surface and sub-surface structure and stoichiometry are tailored for functionality, over controlling only bulk compositions.

Authors:
 [1];  [1];  [2];  [3];  [4]; ORCiD logo [5];  [6];  [6]
  1. Cornell Univ., Ithaca, NY (United States). Dept. of Materials Science and Engineering
  2. Stanford Univ., CA (United States). Dept. of Applied Physics
  3. Drexel Univ., Philadelphia, PA (United States). Dept. of Materials Science and Engineering
  4. Drexel Univ., Philadelphia, PA (United States). Dept. of Materials Science and Engineerin
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  6. Cornell Univ., Ithaca, NY (United States). Dept. of Materials Science and Engineering; Cornell Univ., Ithaca, NY (United States). Kavli Inst. at Cornell for Nanoscale Science
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1494099
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Eom, C. John, Kuo, Ding-Yuan, Adamo, Carolina, Moon, Eun Ju, May, Steve J., Crumlin, Ethan J., Schlom, Darrell G., and Suntivich, Jin. Tailoring manganese oxide with atomic precision to increase surface site availability for oxygen reduction catalysis. United States: N. p., 2018. Web. doi:10.1038/s41467-018-06503-8.
Eom, C. John, Kuo, Ding-Yuan, Adamo, Carolina, Moon, Eun Ju, May, Steve J., Crumlin, Ethan J., Schlom, Darrell G., & Suntivich, Jin. Tailoring manganese oxide with atomic precision to increase surface site availability for oxygen reduction catalysis. United States. doi:10.1038/s41467-018-06503-8.
Eom, C. John, Kuo, Ding-Yuan, Adamo, Carolina, Moon, Eun Ju, May, Steve J., Crumlin, Ethan J., Schlom, Darrell G., and Suntivich, Jin. Tue . "Tailoring manganese oxide with atomic precision to increase surface site availability for oxygen reduction catalysis". United States. doi:10.1038/s41467-018-06503-8. https://www.osti.gov/servlets/purl/1494099.
@article{osti_1494099,
title = {Tailoring manganese oxide with atomic precision to increase surface site availability for oxygen reduction catalysis},
author = {Eom, C. John and Kuo, Ding-Yuan and Adamo, Carolina and Moon, Eun Ju and May, Steve J. and Crumlin, Ethan J. and Schlom, Darrell G. and Suntivich, Jin},
abstractNote = {Controlling the structure of catalysts at the atomic level provides an opportunity to establish detailed understanding of the catalytic form-to-function and realize new, non-equilibrium catalytic structures. Here, advanced thin-film deposition is used to control the atomic structure of La2/3Sr1/3MnO3, a well-known catalyst for the oxygen reduction reaction. The surface and sub-surface is customized, whereas the overall composition and d-electron configuration of the oxide is kept constant. Although the addition of SrMnO3 benefits the oxygen reduction reaction via electronic structure and conductivity improvements, SrMnO3 can react with ambient air to reduce the surface site availability. Placing SrMnO3 in the sub-surface underneath a LaMnO3 overlayer allows the catalyst to maintain the surface site availability while benefiting from improved electronic effects. The results show the promise of advanced thin-film deposition for realizing atomically precise catalysts, in which the surface and sub-surface structure and stoichiometry are tailored for functionality, over controlling only bulk compositions.},
doi = {10.1038/s41467-018-06503-8},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {2018},
month = {10}
}

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Works referenced in this record:

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