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Title: Oxygen reduction kinetics on Pt monolayer shell highly affected by the structure of bimetallic AuNi cores

Abstract

Here, we describe pronounced effects of structural changes of the AuNi cores on the oxygen reduction reaction (ORR) activity of a Pt monolayer shell. The study of alloyed AuNi nanoparticles compared with AuNi core–shell structured nanoparticles revealed configurations having different electronic and electrochemical properties. Controlled alloying of Au with Ni was essential to tune the electronic properties of Au interacting with the Pt monolayer shell to achieve suitable adsorption of O 2 on Pt for expediting the ORR. The alloyed AuNi nanoparticles made the Pt shell more catalytically active for the ORR than the core–shell structured AuNi nanoparticles. The Pt monolayer supported on the alloyed AuNi nanoparticles showed the Pt mass and specific activities as high as 1.52 A mg –1 and 1.18 mA cm –2, respectively, with almost no loss over 5 000 cycles of stability test. This high ORR activity is ascribed to the role of nonspecific steric configuration of Ni atoms changing the electronic properties of the alloy that affect the oxygen and water interaction with the Pt shell and facilitate increased ORR kinetics.

Authors:
 [1];  [2];  [2];  [2];  [2];  [2];  [3];  [3];  [3];  [2];  [2];  [2]
  1. Harbin Institute of Technology, Harbin (China); Brookhaven National Lab. (BNL), Upton, NY (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Harbin Institute of Technology, Harbin (China)
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:
1329922
Report Number(s):
BNL-112748-2016-JA
Journal ID: ISSN 0897-4756; R&D Project: MA510MAEA; KC0302010
Grant/Contract Number:
SC00112704
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 28; Journal Issue: 15; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Chen, Guangyu, Kuttiyiel, Kurian A., Su, Dong, Li, Meng, Wang, Chiu -Hui, Buceta, David, Du, Chunyu, Gao, Yunzhi, Yin, Geping, Sasaki, Kotaro, Vukmirovic, Miomir B., and Adzic, Radoslav R. Oxygen reduction kinetics on Pt monolayer shell highly affected by the structure of bimetallic AuNi cores. United States: N. p., 2016. Web. doi:10.1021/acs.chemmater.6b00500.
Chen, Guangyu, Kuttiyiel, Kurian A., Su, Dong, Li, Meng, Wang, Chiu -Hui, Buceta, David, Du, Chunyu, Gao, Yunzhi, Yin, Geping, Sasaki, Kotaro, Vukmirovic, Miomir B., & Adzic, Radoslav R. Oxygen reduction kinetics on Pt monolayer shell highly affected by the structure of bimetallic AuNi cores. United States. doi:10.1021/acs.chemmater.6b00500.
Chen, Guangyu, Kuttiyiel, Kurian A., Su, Dong, Li, Meng, Wang, Chiu -Hui, Buceta, David, Du, Chunyu, Gao, Yunzhi, Yin, Geping, Sasaki, Kotaro, Vukmirovic, Miomir B., and Adzic, Radoslav R. Tue . "Oxygen reduction kinetics on Pt monolayer shell highly affected by the structure of bimetallic AuNi cores". United States. doi:10.1021/acs.chemmater.6b00500. https://www.osti.gov/servlets/purl/1329922.
@article{osti_1329922,
title = {Oxygen reduction kinetics on Pt monolayer shell highly affected by the structure of bimetallic AuNi cores},
author = {Chen, Guangyu and Kuttiyiel, Kurian A. and Su, Dong and Li, Meng and Wang, Chiu -Hui and Buceta, David and Du, Chunyu and Gao, Yunzhi and Yin, Geping and Sasaki, Kotaro and Vukmirovic, Miomir B. and Adzic, Radoslav R.},
abstractNote = {Here, we describe pronounced effects of structural changes of the AuNi cores on the oxygen reduction reaction (ORR) activity of a Pt monolayer shell. The study of alloyed AuNi nanoparticles compared with AuNi core–shell structured nanoparticles revealed configurations having different electronic and electrochemical properties. Controlled alloying of Au with Ni was essential to tune the electronic properties of Au interacting with the Pt monolayer shell to achieve suitable adsorption of O2 on Pt for expediting the ORR. The alloyed AuNi nanoparticles made the Pt shell more catalytically active for the ORR than the core–shell structured AuNi nanoparticles. The Pt monolayer supported on the alloyed AuNi nanoparticles showed the Pt mass and specific activities as high as 1.52 A mg–1 and 1.18 mA cm–2, respectively, with almost no loss over 5 000 cycles of stability test. This high ORR activity is ascribed to the role of nonspecific steric configuration of Ni atoms changing the electronic properties of the alloy that affect the oxygen and water interaction with the Pt shell and facilitate increased ORR kinetics.},
doi = {10.1021/acs.chemmater.6b00500},
journal = {Chemistry of Materials},
number = 15,
volume = 28,
place = {United States},
year = {Tue Jul 12 00:00:00 EDT 2016},
month = {Tue Jul 12 00:00:00 EDT 2016}
}

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