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Title: Spontaneous incorporation of gold in palladium-based ternary nanoparticles makes durable electrocatalysts for oxygen reduction reaction

Abstract

Replacing platinum by a less precious metal such as palladium, is highly desirable for lowering the cost of fuel-cell electrocatalysts. However, the instability of palladium in the harsh environment of fuel-cell cathodes renders its commercial future bleak. Here in this paper, we show that by incorporating trace amounts of gold in palladium-based ternary (Pd6CoCu) nanocatalysts, the durability of the catalysts improves markedly. Using aberration-corrected analytical transmission electron microscopy in conjunction with synchrotron X-ray absorption spectroscopy, we show that gold not only galvanically replaces cobalt and copper on the surface, but also penetrates through the Pd–Co–Cu lattice and distributes uniformly within the particles. The uniform incorporation of Au provides a stability boost to the entire host particle, from the surface to the interior. The spontaneous replacement method we have developed is scalable and commercially viable. In conclusion, this work may provide new insight for the large-scale production of non-platinum electrocatalysts for fuel-cell applications.

Authors:
 [1];  [1];  [1];  [2]; ORCiD logo [3];  [4];  [4];  [4];  [5]; ORCiD logo [6];  [1]; ORCiD logo [4]; ORCiD logo [2];  [4]
+ Show Author Affiliations
  1. Huazhong Univ. of Science and Technology
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. JEOL USA, Inc., Peabody, MA (United States)
  4. Cornell Univ., Ithaca, NY (United States)
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  6. SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN); Energy Frontier Research Centers (EFRC) (United States). Energy Materials Center at Cornell (EMC2)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1280818
Alternate Identifier(s):
OSTI ID: 1336047
Report Number(s):
BNL-112299-2016-JA
Journal ID: ISSN 2041-1723; ncomms11941
Grant/Contract Number:  
AC02-76SF00515; SC0012704; SC0001086
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; 36 MATERIALS SCIENCE; Oxygen Reduction Reaction; Fuel Cell; Center for Functional Nanomaterials

Citation Formats

Wang, Deli, Liu, Sufen, Wang, Jie, Lin, Ruoqian, Kawasaki, Masahiro, Rus, Eric, Silberstein, Katharine E., Lowe, Michael A., Lin, Feng, Nordlund, Dennis, Liu, Hongfang, Muller, David A., Xin, Huolin L., and Abruña, Héctor D. Spontaneous incorporation of gold in palladium-based ternary nanoparticles makes durable electrocatalysts for oxygen reduction reaction. United States: N. p., 2016. Web. doi:10.1038/ncomms11941.
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Wang, Deli, Liu, Sufen, Wang, Jie, Lin, Ruoqian, Kawasaki, Masahiro, Rus, Eric, Silberstein, Katharine E., Lowe, Michael A., Lin, Feng, Nordlund, Dennis, Liu, Hongfang, Muller, David A., Xin, Huolin L., & Abruña, Héctor D. Spontaneous incorporation of gold in palladium-based ternary nanoparticles makes durable electrocatalysts for oxygen reduction reaction. United States. https://doi.org/10.1038/ncomms11941
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Wang, Deli, Liu, Sufen, Wang, Jie, Lin, Ruoqian, Kawasaki, Masahiro, Rus, Eric, Silberstein, Katharine E., Lowe, Michael A., Lin, Feng, Nordlund, Dennis, Liu, Hongfang, Muller, David A., Xin, Huolin L., and Abruña, Héctor D. Thu . "Spontaneous incorporation of gold in palladium-based ternary nanoparticles makes durable electrocatalysts for oxygen reduction reaction". United States. https://doi.org/10.1038/ncomms11941. https://www.osti.gov/servlets/purl/1280818.
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@article{osti_1280818,
title = {Spontaneous incorporation of gold in palladium-based ternary nanoparticles makes durable electrocatalysts for oxygen reduction reaction},
author = {Wang, Deli and Liu, Sufen and Wang, Jie and Lin, Ruoqian and Kawasaki, Masahiro and Rus, Eric and Silberstein, Katharine E. and Lowe, Michael A. and Lin, Feng and Nordlund, Dennis and Liu, Hongfang and Muller, David A. and Xin, Huolin L. and Abruña, Héctor D.},
abstractNote = {Replacing platinum by a less precious metal such as palladium, is highly desirable for lowering the cost of fuel-cell electrocatalysts. However, the instability of palladium in the harsh environment of fuel-cell cathodes renders its commercial future bleak. Here in this paper, we show that by incorporating trace amounts of gold in palladium-based ternary (Pd6CoCu) nanocatalysts, the durability of the catalysts improves markedly. Using aberration-corrected analytical transmission electron microscopy in conjunction with synchrotron X-ray absorption spectroscopy, we show that gold not only galvanically replaces cobalt and copper on the surface, but also penetrates through the Pd–Co–Cu lattice and distributes uniformly within the particles. The uniform incorporation of Au provides a stability boost to the entire host particle, from the surface to the interior. The spontaneous replacement method we have developed is scalable and commercially viable. In conclusion, this work may provide new insight for the large-scale production of non-platinum electrocatalysts for fuel-cell applications.},
doi = {10.1038/ncomms11941},
journal = {Nature Communications},
number = ,
volume = 7,
place = {United States},
year = {Thu Jun 23 00:00:00 EDT 2016},
month = {Thu Jun 23 00:00:00 EDT 2016}
}
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https://doi.org/10.1038/ncomms11941
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Rapid room-temperature synthesis of nanocrystalline spinels as oxygen reduction and evolution electrocatalysts
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Highly stable Pt monolayer on PdAu nanoparticle electrocatalysts for the oxygen reduction reaction
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Structurally ordered intermetallic platinum–cobalt core–shell nanoparticles with enhanced activity and stability as oxygen reduction electrocatalysts
journal, October 2012

  • Wang, Deli; Xin, Huolin L.; Hovden, Robert
  • Nature Materials, Vol. 12, Issue 1, p. 81-87
  • DOI: 10.1038/nmat3458

Compositional segregation in shaped Pt alloy nanoparticles and their structural behaviour during electrocatalysis
journal, June 2013

  • Cui, Chunhua; Gan, Lin; Heggen, Marc
  • Nature Materials, Vol. 12, Issue 8
  • DOI: 10.1038/nmat3668

An oxygen reduction electrocatalyst based on carbon nanotube–graphene complexes
journal, May 2012

  • Li, Yanguang; Zhou, Wu; Wang, Hailiang
  • Nature Nanotechnology, Vol. 7, Issue 6
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Manageable N-doped Graphene for High Performance Oxygen Reduction Reaction
journal, September 2013

  • Zhang, Yuewei; Ge, Jun; Wang, Lu
  • Scientific Reports, Vol. 3, Issue 1
  • DOI: 10.1038/srep02771

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

Nitrogen-Doped Carbon Nanotube Arrays with High Electrocatalytic Activity for Oxygen Reduction
journal, February 2009

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    Active Sites Derived from Heteroatom Doping in Carbon Materials for Oxygen Reduction Reaction
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