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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 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. 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]
  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 Lab., Menlo Park, CA (United States); Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1280818
Report Number(s):
BNL-112299-2016-JA
Journal ID: ISSN 2041-1723; ncomms11941
Grant/Contract Number:
AC02-76SF00515; SC0012704; SC0001086
Resource Type:
Journal Article: 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.
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. doi:10.1038/ncomms11941.
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. 2016. "Spontaneous incorporation of gold in palladium-based ternary nanoparticles makes durable electrocatalysts for oxygen reduction reaction". United States. doi:10.1038/ncomms11941. https://www.osti.gov/servlets/purl/1280818.
@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 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. 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 = 2016,
month = 6
}

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  • 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 (Pd 6CoCu) 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 uniformlymore » 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.« less
  • The impact of Nafion on the oxygen reduction reaction (ORR) activity is studied for Pt/C and Pt-alloy/C catalysts using thin-film rotating disk electrode (TF-RDE) methods in 0.1 M HClO4. Ultrathin uniform catalyst layers and standardized activity measurement protocols are employed to obtain accurate and reproducible ORR activity. Nafion lowers the ORR activity which plateaus with increasing loading on Pt catalysts. Pt particle size is found not to have significant influence on the extent of the SA decrease upon Nafion incorporation. Catalysts using high surface area carbon (HSC) support exhibit attenuated activity loss resulting from lower ionomer coverage on catalyst particlesmore » located within the deep pores. The impact of metallic composition on the activity loss due to Nafion incorporation is also discussed.« less
  • Considerable efforts to make palladium and palladium alloys active catalysts and a possible replacement for platinum have had a marginal success. Here, we report on a structurally ordered Au₁₀Pd₄₀Co₅₀ catalyst that exhibits comparable activity to conventional platinum catalysts in both acid and alkaline media. Electron microscopic techniques demonstrate that via addition of gold atoms PdCo nanoparticles undergo at elevated temperatures an atomic structural transition from core-shell to a rare intermetallic ordered structure with twin boundaries forming stable {111}, {110} and {100} facets. The superior stability of this catalyst compared to platinum after 10,000 potential cycles in alkaline media is attributedmore » to the atomic structural order of PdCo nanoparticles along with protective effect of clusters of gold atoms on the surface. This strategy of making ordered palladium intermetallic alloy nanoparticles can be used in diverse heterogeneous catalysis where particle size and structural stability matters.« less