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Title: Hydrogen Adsorption on Ordered and Disordered Pt-Ni Alloys

Abstract

The bulk properties and chemical reactivity of disordered Pt-Ni alloys in the A1 (fcc) structure are investigated herein using different methods: Virtual Crystal Approximation (VCA), Korringa–Kohn–Rostoker Coherent Potential Approximation (KKR-CPA), and large explicit supercells generated using Super-Cell Random Approximates (SCRAPs). While VCA predicts lattice constants that closely follow Vegard’s law, the large supercells and KKR-CPA predict lattice constants that are consistently larger than Vegard’s law. KKR-CPA results closely agree with those from the large supercells for the disordered alloys, producing similar projected density of states and magnetic moment across the composition range. For instance, while VCA predicts the disordered alloys to be non-magnetic at a Pt concentration (xPt) ≥ 0.5, KKR-CPA and SCRAPs predict the disordered alloys to remain ferromagnetic to higher Pt concentrations. As xPt decreases, the adsorption of H becomes more exothermic on bulk-terminated (111) surfaces but less exothermic on Pt monolayer-terminated (111) surfaces due largely to strain effects. (111) surfaces cut from the large supercells predict average H adsorption energies on the disordered alloys similar to those on the ordered phases of the same compositions, while VCA predicts H adsorption to be more exothermic.

Authors:
 [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [1]
  1. Louisiana State Univ., Baton Rouge, LA (United States)
  2. Iowa State Univ., Ames, IA (United States); Ames Lab., Ames, IA (United States)
  3. Louisiana State Univ., Baton Rouge, LA (United States); Ames Lab., Ames, IA (United States)
Publication Date:
Research Org.:
Ames Laboratory (AMES), Ames, IA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Iowa State Univ., Ames, IA (United States); Louisiana State Univ., Baton Rouge, LA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
OSTI Identifier:
1645121
Alternate Identifier(s):
OSTI ID: 1656762
Report Number(s):
IS-J-10,277
Journal ID: ISSN 1022-5528
Grant/Contract Number:  
SC0018408; AC02-07CH11358; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Topics in Catalysis
Additional Journal Information:
Journal Volume: 63; Journal Issue: 7-8; Journal ID: ISSN 1022-5528
Publisher:
Springer
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Zhang, Shengjie, Johnson, Duane D., Shelton, William A., and Xu, Ye. Hydrogen Adsorption on Ordered and Disordered Pt-Ni Alloys. United States: N. p., 2020. Web. doi:10.1007/s11244-020-01338-4.
Zhang, Shengjie, Johnson, Duane D., Shelton, William A., & Xu, Ye. Hydrogen Adsorption on Ordered and Disordered Pt-Ni Alloys. United States. https://doi.org/10.1007/s11244-020-01338-4
Zhang, Shengjie, Johnson, Duane D., Shelton, William A., and Xu, Ye. Mon . "Hydrogen Adsorption on Ordered and Disordered Pt-Ni Alloys". United States. https://doi.org/10.1007/s11244-020-01338-4. https://www.osti.gov/servlets/purl/1645121.
@article{osti_1645121,
title = {Hydrogen Adsorption on Ordered and Disordered Pt-Ni Alloys},
author = {Zhang, Shengjie and Johnson, Duane D. and Shelton, William A. and Xu, Ye},
abstractNote = {The bulk properties and chemical reactivity of disordered Pt-Ni alloys in the A1 (fcc) structure are investigated herein using different methods: Virtual Crystal Approximation (VCA), Korringa–Kohn–Rostoker Coherent Potential Approximation (KKR-CPA), and large explicit supercells generated using Super-Cell Random Approximates (SCRAPs). While VCA predicts lattice constants that closely follow Vegard’s law, the large supercells and KKR-CPA predict lattice constants that are consistently larger than Vegard’s law. KKR-CPA results closely agree with those from the large supercells for the disordered alloys, producing similar projected density of states and magnetic moment across the composition range. For instance, while VCA predicts the disordered alloys to be non-magnetic at a Pt concentration (xPt) ≥ 0.5, KKR-CPA and SCRAPs predict the disordered alloys to remain ferromagnetic to higher Pt concentrations. As xPt decreases, the adsorption of H becomes more exothermic on bulk-terminated (111) surfaces but less exothermic on Pt monolayer-terminated (111) surfaces due largely to strain effects. (111) surfaces cut from the large supercells predict average H adsorption energies on the disordered alloys similar to those on the ordered phases of the same compositions, while VCA predicts H adsorption to be more exothermic.},
doi = {10.1007/s11244-020-01338-4},
journal = {Topics in Catalysis},
number = 7-8,
volume = 63,
place = {United States},
year = {Mon Jul 27 00:00:00 EDT 2020},
month = {Mon Jul 27 00:00:00 EDT 2020}
}

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