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Title: Optimized Pt-Based Catalysts for Oxygen Reduction Reaction in Alkaline Solution: A First Principle Study

Abstract

The combined density functional theory (DFT) and kinetic Monte Carlo (KMC) is employed to understand the capability of Pt alloys via Pt-X-Pt sandwich motif in tuning the oxygen reduction reaction activity and stability of Pt catalysts in alkaline solution. For X = Fe, Co, Ni, Cu, the structure of Pt-X-Pt alloy is likely to stay under reaction condition for lowering the surface energy. Both Co and Ni are identified as promoters, being able to facilitate the removal of hydroxyl from the surface and the ORR; while all four systems show the enhancement in the stability of surface Pt compared to pure Pt. We find that for X = Ti, Mn, Ce, the alloyed X metal is too active, which tends to anti-segregates to the Pt surface and forms oxides due to the strong X-O interaction. Wherein, the decoration of Ce oxide shows a promoting effect for the ORR on Pt, which induces strain on the neighboring Pt-Pt bonds and helps in release of hydroxyl species; yet it destabilizes the interacted Pt atom and can lead to the deactivation of the catalyst.

Authors:
 [1]; ORCiD logo [2]
  1. State Univ. of New York (SUNY), Stony Brook, NY (United States). Chemistry Dept.
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Dept.
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1471752
Alternate Identifier(s):
OSTI ID: 1473659
Report Number(s):
BNL-209071-2018-JAAM
Journal ID: ISSN 0013-4651
Grant/Contract Number:  
SC0012704
Resource Type:
Journal Article: Published Article
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
Journal Volume: 165; Journal Issue: 15; Journal ID: ISSN 0013-4651
Publisher:
The Electrochemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; Alkaline; ORR; Pt alloy

Citation Formats

Liu, Shizhong, and Liu, Ping. Optimized Pt-Based Catalysts for Oxygen Reduction Reaction in Alkaline Solution: A First Principle Study. United States: N. p., 2018. Web. doi:10.1149/2.0171815jes.
Liu, Shizhong, & Liu, Ping. Optimized Pt-Based Catalysts for Oxygen Reduction Reaction in Alkaline Solution: A First Principle Study. United States. doi:10.1149/2.0171815jes.
Liu, Shizhong, and Liu, Ping. Thu . "Optimized Pt-Based Catalysts for Oxygen Reduction Reaction in Alkaline Solution: A First Principle Study". United States. doi:10.1149/2.0171815jes.
@article{osti_1471752,
title = {Optimized Pt-Based Catalysts for Oxygen Reduction Reaction in Alkaline Solution: A First Principle Study},
author = {Liu, Shizhong and Liu, Ping},
abstractNote = {The combined density functional theory (DFT) and kinetic Monte Carlo (KMC) is employed to understand the capability of Pt alloys via Pt-X-Pt sandwich motif in tuning the oxygen reduction reaction activity and stability of Pt catalysts in alkaline solution. For X = Fe, Co, Ni, Cu, the structure of Pt-X-Pt alloy is likely to stay under reaction condition for lowering the surface energy. Both Co and Ni are identified as promoters, being able to facilitate the removal of hydroxyl from the surface and the ORR; while all four systems show the enhancement in the stability of surface Pt compared to pure Pt. We find that for X = Ti, Mn, Ce, the alloyed X metal is too active, which tends to anti-segregates to the Pt surface and forms oxides due to the strong X-O interaction. Wherein, the decoration of Ce oxide shows a promoting effect for the ORR on Pt, which induces strain on the neighboring Pt-Pt bonds and helps in release of hydroxyl species; yet it destabilizes the interacted Pt atom and can lead to the deactivation of the catalyst.},
doi = {10.1149/2.0171815jes},
journal = {Journal of the Electrochemical Society},
number = 15,
volume = 165,
place = {United States},
year = {Thu Sep 20 00:00:00 EDT 2018},
month = {Thu Sep 20 00:00:00 EDT 2018}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1149/2.0171815jes

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Works referenced in this record:

Core-Protected Platinum Monolayer Shell High-Stability Electrocatalysts for Fuel-Cell Cathodes
journal, October 2010

  • Sasaki, Kotaro; Naohara, Hideo; Cai, Yun
  • Angewandte Chemie International Edition, Vol. 49, Issue 46, p. 8602-8607
  • DOI: 10.1002/anie.201004287

Prospects for Alkaline Anion-Exchange Membranes in Low Temperature Fuel�Cells
journal, October 2004


Projector augmented-wave method
journal, December 1994


Near-surface alloys for hydrogen fuel cell applications
journal, January 2006


From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999


Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study
journal, January 1998

  • Dudarev, S. L.; Botton, G. A.; Savrasov, S. Y.
  • Physical Review B, Vol. 57, Issue 3, p. 1505-1509
  • DOI: 10.1103/PhysRevB.57.1505

Ab initiomolecular dynamics for liquid metals
journal, January 1993


Improved Oxygen Reduction Activity on Pt3Ni(111) via Increased Surface Site Availability
journal, January 2007

  • Stamenkovic, V. R.; Fowler, B.; Mun, B. S.
  • Science, Vol. 315, Issue 5811, p. 493-497
  • DOI: 10.1126/science.1135941

Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996


Special points for Brillouin-zone integrations
journal, June 1976

  • Monkhorst, Hendrik J.; Pack, James D.
  • Physical Review B, Vol. 13, Issue 12, p. 5188-5192
  • DOI: 10.1103/PhysRevB.13.5188

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996


Ab initio molecular-dynamics simulation of the liquid-metal�amorphous-semiconductor transition in germanium
journal, May 1994


Pd-Pt Bimetallic Nanodendrites with High Activity for Oxygen Reduction
journal, May 2009


Theoretical surface science and catalysis—calculations and concepts
book, January 2000


Alloys of platinum and early transition metals as oxygen reduction electrocatalysts
journal, September 2009

  • Greeley, J.; Stephens, I. E. L.; Bondarenko, A. S.
  • Nature Chemistry, Vol. 1, Issue 7, p. 552-556
  • DOI: 10.1038/nchem.367

Alkaline polymer electrolyte fuel cells completely free from noble metal catalysts
journal, December 2008

  • Lu, S.; Pan, J.; Huang, A.
  • Proceedings of the National Academy of Sciences, Vol. 105, Issue 52, p. 20611-20614
  • DOI: 10.1073/pnas.0810041106