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Title: Core-Shell Structuring of Pure Metallic Aerogels towards Highly Efficient Platinum Utilization for the Oxygen Reduction Reaction

The development of core–shell structures remains a fundamental challenge for pure metallic aerogels. Here we report the synthesis of Pd xAu-Pt core–shell aerogels composed of an ultrathin Pt shell and a composition-tunable Pd xAu alloy core. The universality of this strategy ensures the extension of core compositions to Pd transition-metal alloys. The core–shell aerogels exhibited largely improved Pt utilization efficiencies for the oxygen reduction reaction and their activities show a volcano-type relationship as a function of the lattice parameter of the core substrate. The maximum mass and specific activities are 5.25 A mg Pt -1 and 2.53 mA cm -2, which are 18.7 and 4.1 times higher than those of Pt/C, respectively, demonstrating the superiority of the core–shell metallic aerogels. The proposed core-based activity descriptor provides a new possible strategy for the design of future core–shell electrocatalysts.
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [3] ;  [4] ;  [3] ;  [5] ;  [3] ; ORCiD logo [4]
  1. Technische Univ. Dresden (Germany); Brookhaven National Lab. (BNL), Upton, NY (United States)
  2. Helmholtz-Zentrum Dresden-Rossendorf, (Germany)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States)
  4. Technische Univ. Dresden (Germany)
  5. Leibniz Inst. for Solid State and Materials Research (IFW), Dresden (Germany)
Publication Date:
Report Number(s):
BNL-200018-2018-JAAM
Journal ID: ISSN 1433-7851
Grant/Contract Number:
SC0012704
Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition); Journal Volume: 57; Journal Issue: 11; Journal ID: ISSN 1433-7851
Publisher:
Wiley
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1425037
Alternate Identifier(s):
OSTI ID: 1419897

Cai, Bin, Hübner, René, Sasaki, Kotaro, Zhang, Yuanzhe, Su, Dong, Ziegler, Christoph, Vukmirovic, Miomir B., Rellinghaus, Bernd, Adzic, Radoslav R., and Eychmüller, Alexander. Core-Shell Structuring of Pure Metallic Aerogels towards Highly Efficient Platinum Utilization for the Oxygen Reduction Reaction. United States: N. p., Web. doi:10.1002/anie.201710997.
Cai, Bin, Hübner, René, Sasaki, Kotaro, Zhang, Yuanzhe, Su, Dong, Ziegler, Christoph, Vukmirovic, Miomir B., Rellinghaus, Bernd, Adzic, Radoslav R., & Eychmüller, Alexander. Core-Shell Structuring of Pure Metallic Aerogels towards Highly Efficient Platinum Utilization for the Oxygen Reduction Reaction. United States. doi:10.1002/anie.201710997.
Cai, Bin, Hübner, René, Sasaki, Kotaro, Zhang, Yuanzhe, Su, Dong, Ziegler, Christoph, Vukmirovic, Miomir B., Rellinghaus, Bernd, Adzic, Radoslav R., and Eychmüller, Alexander. 2018. "Core-Shell Structuring of Pure Metallic Aerogels towards Highly Efficient Platinum Utilization for the Oxygen Reduction Reaction". United States. doi:10.1002/anie.201710997.
@article{osti_1425037,
title = {Core-Shell Structuring of Pure Metallic Aerogels towards Highly Efficient Platinum Utilization for the Oxygen Reduction Reaction},
author = {Cai, Bin and Hübner, René and Sasaki, Kotaro and Zhang, Yuanzhe and Su, Dong and Ziegler, Christoph and Vukmirovic, Miomir B. and Rellinghaus, Bernd and Adzic, Radoslav R. and Eychmüller, Alexander},
abstractNote = {The development of core–shell structures remains a fundamental challenge for pure metallic aerogels. Here we report the synthesis of PdxAu-Pt core–shell aerogels composed of an ultrathin Pt shell and a composition-tunable PdxAu alloy core. The universality of this strategy ensures the extension of core compositions to Pd transition-metal alloys. The core–shell aerogels exhibited largely improved Pt utilization efficiencies for the oxygen reduction reaction and their activities show a volcano-type relationship as a function of the lattice parameter of the core substrate. The maximum mass and specific activities are 5.25 A mgPt-1 and 2.53 mA cm-2, which are 18.7 and 4.1 times higher than those of Pt/C, respectively, demonstrating the superiority of the core–shell metallic aerogels. The proposed core-based activity descriptor provides a new possible strategy for the design of future core–shell electrocatalysts.},
doi = {10.1002/anie.201710997},
journal = {Angewandte Chemie (International Edition)},
number = 11,
volume = 57,
place = {United States},
year = {2018},
month = {2}
}