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Title: Design of Ternary Nanoalloy Catalysts: Effect of Nanoscale Alloying and Structural Perfection on Electrocatalytic Enhancement

Abstract

The ability to tune the atomic-scale structural and chemical ordering in nanoalloy catalysts is essential for achieving the ultimate goal of high activity and stability of catalyst by design. This article shows this ability with a ternary nanoalloy of platinum with vanadium and cobalt for oxygen reduction reaction in fuel cells. The strategy is to enable nanoscale alloying and structural perfection through oxidative–reductive thermochemical treatments. The structural manipulation is shown to produce a significant enhancement in the electrocatalytic activity of the ternary nanoalloy catalysts for oxygen reduction reaction. Mass activities as high as 1 A/mg of Pt have been achieved by this strategy based on direct measurements of the kinetic currents from rotating disk electrode data. Using a synchrotron high-energy X-ray diffraction technique coupled with atomic pair function analysis and X-ray absorption fine structure spectroscopy as well as X-ray photoelectron spectroscopy, the atomic-scale structural and chemical ordering in nanoalloy catalysts prepared by the oxidative–reductive thermochemical treatments were examined. A phase transition has been observed, showing an fcc-type structure of the as-prepared and the lower-temperature-treated particles into an fct-type structure for the particles treated at the higher temperature. The results reveal a thermochemically driven evolution of the nanoalloys from a chemicallymore » disordered state into chemically ordered state with an enhanced degree of alloying. The increase in the chemical ordering and shrinking of interatomic distances as a result of thermochemical treatment at increased temperature is shown to increase the catalytic activity for oxygen reduction reaction, exhibiting an optimal activity at 600 °C. It is the alloying and structural perfection that allows the optimization of the catalytic performance in a controllable way, highlighting the significant role of atomic-scale structural and chemical ordering in the design of nanoalloy catalysts.« less

Authors:
 [1];  [1];  [1];  [2];  [3];  [1];  [3];  [1];  [1];  [1];  [4];  [1]
  1. State Univ. of New York (SUNY), Binghamton, NY (United States)
  2. Central Michigan Univ., Mount Pleasant, MI (United States)
  3. Pennsylvania State Univ., State College, PA (United States)
  4. UTC Power, South Windsor, CT (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Org.:
USDOE
OSTI Identifier:
1056697
Resource Type:
Journal Article
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 24; Journal Issue: 22; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
ENGLISH

Citation Formats

Wanjala, Bridgid N., Fang, Bin, Shan, Shiyao, Petkov, Valeri, Zhu, Pengyu, Loukrakpam, Rameshwori, Chen, Yongsheng, Luo, Jin, Yin, Jun, Yang, Lefu, Shao, Minhua, and Zhong, Chuan-Jian. Design of Ternary Nanoalloy Catalysts: Effect of Nanoscale Alloying and Structural Perfection on Electrocatalytic Enhancement. United States: N. p., 2012. Web. doi:10.1021/cm301613j.
Wanjala, Bridgid N., Fang, Bin, Shan, Shiyao, Petkov, Valeri, Zhu, Pengyu, Loukrakpam, Rameshwori, Chen, Yongsheng, Luo, Jin, Yin, Jun, Yang, Lefu, Shao, Minhua, & Zhong, Chuan-Jian. Design of Ternary Nanoalloy Catalysts: Effect of Nanoscale Alloying and Structural Perfection on Electrocatalytic Enhancement. United States. doi:10.1021/cm301613j.
Wanjala, Bridgid N., Fang, Bin, Shan, Shiyao, Petkov, Valeri, Zhu, Pengyu, Loukrakpam, Rameshwori, Chen, Yongsheng, Luo, Jin, Yin, Jun, Yang, Lefu, Shao, Minhua, and Zhong, Chuan-Jian. Mon . "Design of Ternary Nanoalloy Catalysts: Effect of Nanoscale Alloying and Structural Perfection on Electrocatalytic Enhancement". United States. doi:10.1021/cm301613j.
@article{osti_1056697,
title = {Design of Ternary Nanoalloy Catalysts: Effect of Nanoscale Alloying and Structural Perfection on Electrocatalytic Enhancement},
author = {Wanjala, Bridgid N. and Fang, Bin and Shan, Shiyao and Petkov, Valeri and Zhu, Pengyu and Loukrakpam, Rameshwori and Chen, Yongsheng and Luo, Jin and Yin, Jun and Yang, Lefu and Shao, Minhua and Zhong, Chuan-Jian},
abstractNote = {The ability to tune the atomic-scale structural and chemical ordering in nanoalloy catalysts is essential for achieving the ultimate goal of high activity and stability of catalyst by design. This article shows this ability with a ternary nanoalloy of platinum with vanadium and cobalt for oxygen reduction reaction in fuel cells. The strategy is to enable nanoscale alloying and structural perfection through oxidative–reductive thermochemical treatments. The structural manipulation is shown to produce a significant enhancement in the electrocatalytic activity of the ternary nanoalloy catalysts for oxygen reduction reaction. Mass activities as high as 1 A/mg of Pt have been achieved by this strategy based on direct measurements of the kinetic currents from rotating disk electrode data. Using a synchrotron high-energy X-ray diffraction technique coupled with atomic pair function analysis and X-ray absorption fine structure spectroscopy as well as X-ray photoelectron spectroscopy, the atomic-scale structural and chemical ordering in nanoalloy catalysts prepared by the oxidative–reductive thermochemical treatments were examined. A phase transition has been observed, showing an fcc-type structure of the as-prepared and the lower-temperature-treated particles into an fct-type structure for the particles treated at the higher temperature. The results reveal a thermochemically driven evolution of the nanoalloys from a chemically disordered state into chemically ordered state with an enhanced degree of alloying. The increase in the chemical ordering and shrinking of interatomic distances as a result of thermochemical treatment at increased temperature is shown to increase the catalytic activity for oxygen reduction reaction, exhibiting an optimal activity at 600 °C. It is the alloying and structural perfection that allows the optimization of the catalytic performance in a controllable way, highlighting the significant role of atomic-scale structural and chemical ordering in the design of nanoalloy catalysts.},
doi = {10.1021/cm301613j},
journal = {Chemistry of Materials},
issn = {0897-4756},
number = 22,
volume = 24,
place = {United States},
year = {2012},
month = {10}
}