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Title: Nanoscale Engineering of Efficient Oxygen Reduction Electrocatalysts by Tailoring the Local Chemical Environment of Pt Surface Sites

Abstract

The oxygen reduction reaction is the limiting half-reaction in hydrogen fuel cells. While Pt is the most active single component electrocatalyst for the reaction, it is hampered by high cost and low reaction rates. Most research to overcome these limitations has focused on Pt/3d alloys, which offer higher rates and lower cost. Here, we have synthesized, characterized, and tested alloy materials belonging to a multilayer family of electrocatalysts. The multilayer alloy materials contain an AuCu alloy core of precise composition, surrounded by Au layers and covered by a catalytically active Pt surface layer. Their performance relative to that of the commercial Pt standards reaches up to 4 times improved area-specific activity. Characterization studies support the hypothesis that the activity improvement originates from a combination of Au–Pt ligand effects and local strain effects manipulated through the AuCu alloy core. The approach we present to control the strain and ligand effects in the synthesis of Pt-based alloys for the ORR is very general and could lead to promising alloy materials.

Authors:
ORCiD logo [1];  [1];  [1]; ORCiD logo [2];  [1]
+ Show Author Affiliations
  1. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Chemical Engineering
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1414683
Grant/Contract Number:  
AC05-00OR22725; FG-02-05ER15686
Resource Type:
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 7; Journal Issue: 1; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; core-shell nanoparticles; electrocatalysis; fuel cells; oxygen reduction; platinum alloy catalysts

Citation Formats

Cleve, Tim Van, Moniri, Saman, Belok, Gabrielle, More, Karren L., and Linic, Suljo. Nanoscale Engineering of Efficient Oxygen Reduction Electrocatalysts by Tailoring the Local Chemical Environment of Pt Surface Sites. United States: N. p., 2016. Web. doi:10.1021/acscatal.6b01565.
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Cleve, Tim Van, Moniri, Saman, Belok, Gabrielle, More, Karren L., & Linic, Suljo. Nanoscale Engineering of Efficient Oxygen Reduction Electrocatalysts by Tailoring the Local Chemical Environment of Pt Surface Sites. United States. https://doi.org/10.1021/acscatal.6b01565
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Cleve, Tim Van, Moniri, Saman, Belok, Gabrielle, More, Karren L., and Linic, Suljo. Wed . "Nanoscale Engineering of Efficient Oxygen Reduction Electrocatalysts by Tailoring the Local Chemical Environment of Pt Surface Sites". United States. https://doi.org/10.1021/acscatal.6b01565. https://www.osti.gov/servlets/purl/1414683.
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@article{osti_1414683,
title = {Nanoscale Engineering of Efficient Oxygen Reduction Electrocatalysts by Tailoring the Local Chemical Environment of Pt Surface Sites},
author = {Cleve, Tim Van and Moniri, Saman and Belok, Gabrielle and More, Karren L. and Linic, Suljo},
abstractNote = {The oxygen reduction reaction is the limiting half-reaction in hydrogen fuel cells. While Pt is the most active single component electrocatalyst for the reaction, it is hampered by high cost and low reaction rates. Most research to overcome these limitations has focused on Pt/3d alloys, which offer higher rates and lower cost. Here, we have synthesized, characterized, and tested alloy materials belonging to a multilayer family of electrocatalysts. The multilayer alloy materials contain an AuCu alloy core of precise composition, surrounded by Au layers and covered by a catalytically active Pt surface layer. Their performance relative to that of the commercial Pt standards reaches up to 4 times improved area-specific activity. Characterization studies support the hypothesis that the activity improvement originates from a combination of Au–Pt ligand effects and local strain effects manipulated through the AuCu alloy core. The approach we present to control the strain and ligand effects in the synthesis of Pt-based alloys for the ORR is very general and could lead to promising alloy materials.},
doi = {10.1021/acscatal.6b01565},
journal = {ACS Catalysis},
number = 1,
volume = 7,
place = {United States},
year = {Wed Nov 16 00:00:00 EST 2016},
month = {Wed Nov 16 00:00:00 EST 2016}
}
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https://doi.org/10.1021/acscatal.6b01565
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    • Journal of Materials Chemistry A, Vol. 6, Issue 23
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