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Title: Interface engineering for a rational design of poison-free bimetallic CO oxidation catalysts

Abstract

We use density functional theory calculations of Pt@Cu core@shell nanoparticles (NPs) to design bifunctional poison-free CO oxidation catalysts. By calculating the adsorption chemistry under CO oxidation conditions, we find that the Pt@Cu NPs will be active for CO oxidation with resistance to CO-poisoning. The CO oxidation pathway at the Pt–Cu interface is determined on the Pt NP covered with a full- and partial-shell of Cu. The exposed portion of the Pt core preferentially binds CO and the Cu shell binds O2, supplying oxygen for the reaction. The Pt–Cu interface provides CO-oxidation sites that are not poisoned by either CO or O2. Additional computational screening shows that this separation of reactant binding sites is possible for several other core@shell NPs. Our results indicate that the metal–metal interface within a single NP can be optimized for design of bifunctional catalytic systems with improved performance.

Authors:
 [1]; ORCiD logo [2];  [3];  [3];  [3];  [1];  [2]; ORCiD logo [3]
  1. Korea Advanced Inst. Science and Technology (KAIST), Daejeon (Korea, Republic of). Dept. of Materials Science and Engineering
  2. Univ. of Texas, Austin, TX (United States). Dept. of Chemistry
  3. Changnam National Univ, Daejeon (Korea). Dept. fo Materials Science and Engineering
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory-National Energy Research Scientific Computing Center
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1492966
DOE Contract Number:  
SC0012704; FG02-09ER16090
Resource Type:
Journal Article
Journal Name:
Nanoscale
Additional Journal Information:
Journal Volume: 9; Journal Issue: 16; Journal ID: ISSN 2040-3364
Country of Publication:
United States
Language:
English

Citation Formats

Shin, Kihyun, Zhang, Liang, An, Hyesung, Ha, Hyunwoo, Yoo, Mi, Lee, Hyuck Mo, Henkelman, Graeme, and Kim, Hyun You. Interface engineering for a rational design of poison-free bimetallic CO oxidation catalysts. United States: N. p., 2017. Web. doi:10.1039/c7nr01382e.
Shin, Kihyun, Zhang, Liang, An, Hyesung, Ha, Hyunwoo, Yoo, Mi, Lee, Hyuck Mo, Henkelman, Graeme, & Kim, Hyun You. Interface engineering for a rational design of poison-free bimetallic CO oxidation catalysts. United States. doi:10.1039/c7nr01382e.
Shin, Kihyun, Zhang, Liang, An, Hyesung, Ha, Hyunwoo, Yoo, Mi, Lee, Hyuck Mo, Henkelman, Graeme, and Kim, Hyun You. Sun . "Interface engineering for a rational design of poison-free bimetallic CO oxidation catalysts". United States. doi:10.1039/c7nr01382e.
@article{osti_1492966,
title = {Interface engineering for a rational design of poison-free bimetallic CO oxidation catalysts},
author = {Shin, Kihyun and Zhang, Liang and An, Hyesung and Ha, Hyunwoo and Yoo, Mi and Lee, Hyuck Mo and Henkelman, Graeme and Kim, Hyun You},
abstractNote = {We use density functional theory calculations of Pt@Cu core@shell nanoparticles (NPs) to design bifunctional poison-free CO oxidation catalysts. By calculating the adsorption chemistry under CO oxidation conditions, we find that the Pt@Cu NPs will be active for CO oxidation with resistance to CO-poisoning. The CO oxidation pathway at the Pt–Cu interface is determined on the Pt NP covered with a full- and partial-shell of Cu. The exposed portion of the Pt core preferentially binds CO and the Cu shell binds O2, supplying oxygen for the reaction. The Pt–Cu interface provides CO-oxidation sites that are not poisoned by either CO or O2. Additional computational screening shows that this separation of reactant binding sites is possible for several other core@shell NPs. Our results indicate that the metal–metal interface within a single NP can be optimized for design of bifunctional catalytic systems with improved performance.},
doi = {10.1039/c7nr01382e},
journal = {Nanoscale},
issn = {2040-3364},
number = 16,
volume = 9,
place = {United States},
year = {2017},
month = {1}
}

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