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Title: Metal and Metal Oxide Interactions and Their Catalytic Consequences for Oxygen Reduction Reaction

Abstract

Many industrial catalysts are composed of metal particles supported on metal oxides (MMO). It is known that the catalytic activity of MMO materials is governed by metal and metal oxide interactions (MMOI), but how to optimize MMO systems via manipulation of MMOI remains unclear, due primarily to the ambiguous nature of MMOI. Herein, we develop a Pt/NbOx/C system with tunable structural and electronic properties via a modified arc plasma deposition method. We unravel the nature of MMOI by characterizing this system under reactive conditions utilizing combined electrochemical, microscopy, and in situ spectroscopy. We show that Pt interacts with the Nb in unsaturated NbOx owing to the oxygen deficiency in the MMO interface, whereas Pt interacts with the O in nearly saturated NbOx, and further interacts with Nb when the oxygen atoms penetrate into the Pt cluster at elevated potentials. While the Pt–Nb interactions do not benefit the inherent activity of Pt toward oxygen reduction reaction (ORR), the Pt–O interactions improve the ORR activity by shortening the Pt–Pt bond distance. Pt donates electrons to NbOx in both Pt–Nb and Pt–O cases. The resultant electron efficiency stabilizes low-coordinated Pt sites, hereby stabilizing small Pt particles. This determines the two characteristic features ofmore » MMO systems: dispersion of small metal particles and high catalytic durability. These findings contribute to our understandings of MMO catalytic systems.« less

Authors:
ORCiD logo; ; ORCiD logo; ;  [1];  [2];  [2];  [2]; ORCiD logo
  1. ULVAC Technologies, Inc., 401 Griffin Brook Drive, Methuen, Massachusetts 01844, United States
  2. Shanghai Electrochemical Energy Devices Research Center, Department of Chemical Engineering, Shanghai Jiao Tong University, Shanghai 200240, People’s Republic of 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:
1409565
Report Number(s):
BNL-114617-2017-JA¿¿¿
Journal ID: ISSN 0002-7863
DOE Contract Number:  
SC0012704
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of the American Chemical Society; Journal Volume: 139; Journal Issue: 23
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Jia, Qingying, Ghoshal, Shraboni, Li, Jingkun, Liang, Wentao, Meng, Guangnan, Che, Haiying, Zhang, Shiming, Ma, Zi-Feng, and Mukerjee, Sanjeev. Metal and Metal Oxide Interactions and Their Catalytic Consequences for Oxygen Reduction Reaction. United States: N. p., 2017. Web. doi:10.1021/jacs.7b02378.
Jia, Qingying, Ghoshal, Shraboni, Li, Jingkun, Liang, Wentao, Meng, Guangnan, Che, Haiying, Zhang, Shiming, Ma, Zi-Feng, & Mukerjee, Sanjeev. Metal and Metal Oxide Interactions and Their Catalytic Consequences for Oxygen Reduction Reaction. United States. doi:10.1021/jacs.7b02378.
Jia, Qingying, Ghoshal, Shraboni, Li, Jingkun, Liang, Wentao, Meng, Guangnan, Che, Haiying, Zhang, Shiming, Ma, Zi-Feng, and Mukerjee, Sanjeev. Thu . "Metal and Metal Oxide Interactions and Their Catalytic Consequences for Oxygen Reduction Reaction". United States. doi:10.1021/jacs.7b02378.
@article{osti_1409565,
title = {Metal and Metal Oxide Interactions and Their Catalytic Consequences for Oxygen Reduction Reaction},
author = {Jia, Qingying and Ghoshal, Shraboni and Li, Jingkun and Liang, Wentao and Meng, Guangnan and Che, Haiying and Zhang, Shiming and Ma, Zi-Feng and Mukerjee, Sanjeev},
abstractNote = {Many industrial catalysts are composed of metal particles supported on metal oxides (MMO). It is known that the catalytic activity of MMO materials is governed by metal and metal oxide interactions (MMOI), but how to optimize MMO systems via manipulation of MMOI remains unclear, due primarily to the ambiguous nature of MMOI. Herein, we develop a Pt/NbOx/C system with tunable structural and electronic properties via a modified arc plasma deposition method. We unravel the nature of MMOI by characterizing this system under reactive conditions utilizing combined electrochemical, microscopy, and in situ spectroscopy. We show that Pt interacts with the Nb in unsaturated NbOx owing to the oxygen deficiency in the MMO interface, whereas Pt interacts with the O in nearly saturated NbOx, and further interacts with Nb when the oxygen atoms penetrate into the Pt cluster at elevated potentials. While the Pt–Nb interactions do not benefit the inherent activity of Pt toward oxygen reduction reaction (ORR), the Pt–O interactions improve the ORR activity by shortening the Pt–Pt bond distance. Pt donates electrons to NbOx in both Pt–Nb and Pt–O cases. The resultant electron efficiency stabilizes low-coordinated Pt sites, hereby stabilizing small Pt particles. This determines the two characteristic features of MMO systems: dispersion of small metal particles and high catalytic durability. These findings contribute to our understandings of MMO catalytic systems.},
doi = {10.1021/jacs.7b02378},
journal = {Journal of the American Chemical Society},
number = 23,
volume = 139,
place = {United States},
year = {Thu Jun 01 00:00:00 EDT 2017},
month = {Thu Jun 01 00:00:00 EDT 2017}
}