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Title: Tetrahedral Palladium Nanocrystals: A New Support for Platinum Monolayer Electrocatalysts with High Activity and Stability in the Oxygen Reduction Reaction

Abstract

The recent availability of tetrahedral palladium (PdTH) nanocrystals with cleaned surfaces allowed us to evaluate their facet-specific electrochemical properties as a new support of platinum monolayer (PtML) catalysts. The Pd–PtML core-shell electrocatalyst was examined by combining structural analyses and Density Functional Theory (DFT) with electrochemical techniques. The surfaces of the PdTH core are composed of (111) facets wherein the Pd atoms are highly coordinated and have low surface energy. Our results revealed that in comparison with sphere Pd (PdSP)-supported PtML or pure Pt, the PdTH-supported PtML features more surface contraction and a downshift of d-band relative to the Fermi level. These geometric- and electronic-effects determine the higher activity of PtML/PdTH/C for the oxygen reduction reaction (ORR) compared to that of PtML/PdSP/C. This shape-property interdependence illuminated new approaches to basic- and applied- research on Pt-based ORR electrocatalysts of significant importance to the widespread use of fuel cells.

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [1]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1079318
Report Number(s):
BNL-99614-2013-JA
Journal ID: ISSN 0942-9352; R&D Project: 2014-BNL-MA510MAEA; KC-03-02-010
DOE Contract Number:  
AC02-98CH10886
Resource Type:
Journal Article
Journal Name:
Zeitschrift fuer Physikalische Chemie
Additional Journal Information:
Journal Volume: 226; Journal Issue: 9-10; Journal ID: ISSN 0942-9352
Publisher:
De Gruyter
Country of Publication:
United States
Language:
English
Subject:
30 DIRECT ENERGY CONVERSION; Tetrahedral Palladium; Platinum Monolayer; Oxygen Reduction Reaction; DFT

Citation Formats

Gong, Kuanping, Choi, YongMan, Vukmirovic, Miomir B., Liu, Ping, Ma, Chao, Su, Dong, and Adzic, Radoslav R. Tetrahedral Palladium Nanocrystals: A New Support for Platinum Monolayer Electrocatalysts with High Activity and Stability in the Oxygen Reduction Reaction. United States: N. p., 2012. Web. doi:10.1524/zpch.2012.0239.
Gong, Kuanping, Choi, YongMan, Vukmirovic, Miomir B., Liu, Ping, Ma, Chao, Su, Dong, & Adzic, Radoslav R. Tetrahedral Palladium Nanocrystals: A New Support for Platinum Monolayer Electrocatalysts with High Activity and Stability in the Oxygen Reduction Reaction. United States. https://doi.org/10.1524/zpch.2012.0239
Gong, Kuanping, Choi, YongMan, Vukmirovic, Miomir B., Liu, Ping, Ma, Chao, Su, Dong, and Adzic, Radoslav R. 2012. "Tetrahedral Palladium Nanocrystals: A New Support for Platinum Monolayer Electrocatalysts with High Activity and Stability in the Oxygen Reduction Reaction". United States. https://doi.org/10.1524/zpch.2012.0239.
@article{osti_1079318,
title = {Tetrahedral Palladium Nanocrystals: A New Support for Platinum Monolayer Electrocatalysts with High Activity and Stability in the Oxygen Reduction Reaction},
author = {Gong, Kuanping and Choi, YongMan and Vukmirovic, Miomir B. and Liu, Ping and Ma, Chao and Su, Dong and Adzic, Radoslav R.},
abstractNote = {The recent availability of tetrahedral palladium (PdTH) nanocrystals with cleaned surfaces allowed us to evaluate their facet-specific electrochemical properties as a new support of platinum monolayer (PtML) catalysts. The Pd–PtML core-shell electrocatalyst was examined by combining structural analyses and Density Functional Theory (DFT) with electrochemical techniques. The surfaces of the PdTH core are composed of (111) facets wherein the Pd atoms are highly coordinated and have low surface energy. Our results revealed that in comparison with sphere Pd (PdSP)-supported PtML or pure Pt, the PdTH-supported PtML features more surface contraction and a downshift of d-band relative to the Fermi level. These geometric- and electronic-effects determine the higher activity of PtML/PdTH/C for the oxygen reduction reaction (ORR) compared to that of PtML/PdSP/C. This shape-property interdependence illuminated new approaches to basic- and applied- research on Pt-based ORR electrocatalysts of significant importance to the widespread use of fuel cells.},
doi = {10.1524/zpch.2012.0239},
url = {https://www.osti.gov/biblio/1079318}, journal = {Zeitschrift fuer Physikalische Chemie},
issn = {0942-9352},
number = 9-10,
volume = 226,
place = {United States},
year = {Mon Oct 01 00:00:00 EDT 2012},
month = {Mon Oct 01 00:00:00 EDT 2012}
}