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Title: Water Oxidation Catalysis via Size-Selected Iridium Clusters

Abstract

Here, the detailed mechanism and efficacy of four electron electrochemical water oxidation depend critically upon the detailed atomic structure of each catalytic site, which are numerous and diverse in most metal oxides anodes. In order to limit the diversity of sites, arrays of discrete iridium clusters with identical metal atom number (Ir 2, Ir 4, or Ir 8) were deposited in submonolayer coverage on conductive oxide supports, and the electrochemical properties and activity of each was evaluated. Exceptional electroactivity for the oxygen evolving reaction (OER) was observed for all cluster samples in acidic electrolyte. Reproducible cluster-size-dependent trends in redox behavior were also resolved. First-principles computational models of the individual discrete-size clusters allow correlation of catalytic-site structure and multiplicity with redox behavior.

Authors:
 [1]; ORCiD logo [1];  [2];  [3];  [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [4]; ORCiD logo [1]
  1. Argonne National Lab. (ANL), Lemont, IL (United States)
  2. Argonne National Lab. (ANL), Lemont, IL (United States); Jilin Univ., Jilin (China)
  3. Northwestern Univ., Evanston, IL (United States)
  4. Argonne National Lab. (ANL), Lemont, IL (United States); The Univ. of Chicago, Chicago, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1440760
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 122; Journal Issue: 18; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Halder, Avik, Liu, Cong, Liu, Zhun, Emery, Jonathan D., Pellin, Michael J., Curtiss, Larry A., Zapol, Peter, Vajda, Stefan, and Martinson, Alex B. F. Water Oxidation Catalysis via Size-Selected Iridium Clusters. United States: N. p., 2018. Web. doi:10.1021/acs.jpcc.8b01318.
Halder, Avik, Liu, Cong, Liu, Zhun, Emery, Jonathan D., Pellin, Michael J., Curtiss, Larry A., Zapol, Peter, Vajda, Stefan, & Martinson, Alex B. F. Water Oxidation Catalysis via Size-Selected Iridium Clusters. United States. doi:10.1021/acs.jpcc.8b01318.
Halder, Avik, Liu, Cong, Liu, Zhun, Emery, Jonathan D., Pellin, Michael J., Curtiss, Larry A., Zapol, Peter, Vajda, Stefan, and Martinson, Alex B. F. Fri . "Water Oxidation Catalysis via Size-Selected Iridium Clusters". United States. doi:10.1021/acs.jpcc.8b01318.
@article{osti_1440760,
title = {Water Oxidation Catalysis via Size-Selected Iridium Clusters},
author = {Halder, Avik and Liu, Cong and Liu, Zhun and Emery, Jonathan D. and Pellin, Michael J. and Curtiss, Larry A. and Zapol, Peter and Vajda, Stefan and Martinson, Alex B. F.},
abstractNote = {Here, the detailed mechanism and efficacy of four electron electrochemical water oxidation depend critically upon the detailed atomic structure of each catalytic site, which are numerous and diverse in most metal oxides anodes. In order to limit the diversity of sites, arrays of discrete iridium clusters with identical metal atom number (Ir2, Ir4, or Ir8) were deposited in submonolayer coverage on conductive oxide supports, and the electrochemical properties and activity of each was evaluated. Exceptional electroactivity for the oxygen evolving reaction (OER) was observed for all cluster samples in acidic electrolyte. Reproducible cluster-size-dependent trends in redox behavior were also resolved. First-principles computational models of the individual discrete-size clusters allow correlation of catalytic-site structure and multiplicity with redox behavior.},
doi = {10.1021/acs.jpcc.8b01318},
journal = {Journal of Physical Chemistry. C},
number = 18,
volume = 122,
place = {United States},
year = {Fri Apr 27 00:00:00 EDT 2018},
month = {Fri Apr 27 00:00:00 EDT 2018}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on April 27, 2019
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