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Title: Palladium–platinum core-shell icosahedra with substantially enhanced activity and durability towards oxygen reduction

Abstract

Conformal deposition of platinum as ultrathin shells on facet-controlled palladium nanocrystals offers a great opportunity to enhance the catalytic performance while reducing its loading. Here we report such a system based on palladium icosahedra. Owing to lateral confinement imposed by twin boundaries and thus vertical relaxation only, the platinum overlayers evolve into a corrugated structure under compressive strain. For the core-shell nanocrystals with an average of 2.7 platinum overlayers, their specific and platinum mass activities towards oxygen reduction are enhanced by eight- and sevenfold, respectively, relative to a commercial catalyst. Density functional theory calculations indicate that the enhancement can be attributed to the weakened binding of hydroxyl to the compressed platinum surface supported on palladium. After 10,000 testing cycles, the mass activity of the core-shell nanocrystals is still four times higher than the commercial catalyst. These results demonstrate an effective approach to the development of electrocatalysts with greatly enhanced activity and durability.

Authors:
 [1];  [2];  [3];  [2];  [4];  [1];  [4];  [5];  [6];  [3];  [3];  [2]
+ Show Author Affiliations
  1. Georgia Institute of Technology and Emory University, Atlanta, GA (United States); Xiamen Univ., Xiamen (China)
  2. Georgia Institute of Technology and Emory University, Atlanta, GA (United States)
  3. University of Wisconsin-Madison, Madison, WI (United States)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  5. Arizona State Univ., Tempe, AZ (United States)
  6. Xiamen Univ., Xiamen (China)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS); Univ. of Wisconsin, Madison, WI (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1259678
Alternate Identifier(s):
OSTI ID: 1337045; OSTI ID: 1395953
Grant/Contract Number:  
FG02-05ER15731; AC02-06CH11357; AC02-05CH11231; AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 6; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Wang, Xue, Choi, Sang-Il, Roling, Luke T., Luo, Ming, Ma, Cheng, Zhang, Lei, Chi, Miaofang, Liu, Jingyue, Xie, Zhaoxiong, Herron, Jeffrey A., Mavrikakis, Manos, and Xia, Younan. Palladium–platinum core-shell icosahedra with substantially enhanced activity and durability towards oxygen reduction. United States: N. p., 2015. Web. doi:10.1038/ncomms8594.
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Wang, Xue, Choi, Sang-Il, Roling, Luke T., Luo, Ming, Ma, Cheng, Zhang, Lei, Chi, Miaofang, Liu, Jingyue, Xie, Zhaoxiong, Herron, Jeffrey A., Mavrikakis, Manos, & Xia, Younan. Palladium–platinum core-shell icosahedra with substantially enhanced activity and durability towards oxygen reduction. United States. https://doi.org/10.1038/ncomms8594
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Wang, Xue, Choi, Sang-Il, Roling, Luke T., Luo, Ming, Ma, Cheng, Zhang, Lei, Chi, Miaofang, Liu, Jingyue, Xie, Zhaoxiong, Herron, Jeffrey A., Mavrikakis, Manos, and Xia, Younan. Thu . "Palladium–platinum core-shell icosahedra with substantially enhanced activity and durability towards oxygen reduction". United States. https://doi.org/10.1038/ncomms8594. https://www.osti.gov/servlets/purl/1259678.
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@article{osti_1259678,
title = {Palladium–platinum core-shell icosahedra with substantially enhanced activity and durability towards oxygen reduction},
author = {Wang, Xue and Choi, Sang-Il and Roling, Luke T. and Luo, Ming and Ma, Cheng and Zhang, Lei and Chi, Miaofang and Liu, Jingyue and Xie, Zhaoxiong and Herron, Jeffrey A. and Mavrikakis, Manos and Xia, Younan},
abstractNote = {Conformal deposition of platinum as ultrathin shells on facet-controlled palladium nanocrystals offers a great opportunity to enhance the catalytic performance while reducing its loading. Here we report such a system based on palladium icosahedra. Owing to lateral confinement imposed by twin boundaries and thus vertical relaxation only, the platinum overlayers evolve into a corrugated structure under compressive strain. For the core-shell nanocrystals with an average of 2.7 platinum overlayers, their specific and platinum mass activities towards oxygen reduction are enhanced by eight- and sevenfold, respectively, relative to a commercial catalyst. Density functional theory calculations indicate that the enhancement can be attributed to the weakened binding of hydroxyl to the compressed platinum surface supported on palladium. After 10,000 testing cycles, the mass activity of the core-shell nanocrystals is still four times higher than the commercial catalyst. These results demonstrate an effective approach to the development of electrocatalysts with greatly enhanced activity and durability.},
doi = {10.1038/ncomms8594},
journal = {Nature Communications},
number = ,
volume = 6,
place = {United States},
year = {Thu Jul 02 00:00:00 EDT 2015},
month = {Thu Jul 02 00:00:00 EDT 2015}
}
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https://doi.org/10.1038/ncomms8594
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    Core–Shell-Structured Low-Platinum Electrocatalysts for Fuel Cell Applications
    journal, July 2018

    Synthesis of low- and high-index faceted metal (Pt, Pd, Ru, Ir, Rh) nanoparticles for improved activity and stability in electrocatalysis
    journal, January 2019

    • Poerwoprajitno, Agus R.; Gloag, Lucy; Cheong, Soshan
    • Nanoscale, Vol. 11, Issue 41
    • DOI: 10.1039/c9nr05802h

    The Marriage of the FeN 4 Moiety and MXene Boosts Oxygen Reduction Catalysis: Fe 3d Electron Delocalization Matters
    journal, September 2018

    Surface/Interfacial Catalysis of (Metal)/Oxide System: Structure and Performance Control
    journal, March 2018

    Surface Atomic Regulation of Core–Shell Noble Metal Catalysts
    journal, January 2019

    • Ge, Jingjie; Li, Zhijun; Hong, Xun
    • Chemistry – A European Journal, Vol. 25, Issue 20
    • DOI: 10.1002/chem.201805332

    Rh-Based Nanocatalysts for Heterogeneous Reactions
    journal, April 2018

    Low Pt-content ternary PdCuPt nanodendrites: an efficient electrocatalyst for oxygen reduction reaction
    journal, January 2017

    • Fu, Shaofang; Zhu, Chengzhou; Song, Junhua
    • Nanoscale, Vol. 9, Issue 3
    • DOI: 10.1039/c6nr06646a

    Achieving excellent activity and stability for oxygen reduction electrocatalysis by hollow mesoporous iron–nitrogen-doped graphitic carbon spheres
    journal, January 2017

    • Zhou, Tingsheng; Zhou, Yao; Ma, Ruguang
    • Journal of Materials Chemistry A, Vol. 5, Issue 24
    • DOI: 10.1039/c7ta01896g

    Nanoscale kinetics of asymmetrical corrosion in core-shell nanoparticles
    journal, March 2018

    Unusual 4H-phase twinned noble metal nanokites
    journal, June 2019

    Carbon-supported metal nanodendrites as efficient, stable catalysts for the oxygen reduction reaction
    journal, January 2018

    • Venarusso, Luna B.; Boone, Chirley V.; Bettini, Jefferson
    • Journal of Materials Chemistry A, Vol. 6, Issue 4
    • DOI: 10.1039/c7ta08964c

    Wavy PtCu alloy nanowire networks with abundant surface defects enhanced oxygen reduction reaction
    journal, September 2019

    Seed-Mediated Growth of Colloidal Metal Nanocrystals
    journal, December 2016

    • Xia, Younan; Gilroy, Kyle D.; Peng, Hsin-Chieh
    • Angewandte Chemie International Edition, Vol. 56, Issue 1
    • DOI: 10.1002/anie.201604731

    The Advanced Designs of High-Performance Platinum-Based Electrocatalysts: Recent Progresses and Challenges
    journal, June 2018

    Stabilization of Nanoparticles Produced by Hydrogenation of Palladium–N-Heterocyclic Carbene Complexes on the Surface of Graphene and Implications in Catalysis
    journal, November 2018

    • Mollar-Cuni, Andrés; Ventura-Espinosa, David; Martín, Santiago
    • ACS Omega, Vol. 3, Issue 11
    • DOI: 10.1021/acsomega.8b02193

    Decoupling strain and ligand effects in ternary nanoparticles for improved ORR electrocatalysis
    journal, January 2016

    • Jennings, Paul C.; Lysgaard, Steen; Hansen, Heine A.
    • Physical Chemistry Chemical Physics, Vol. 18, Issue 35
    • DOI: 10.1039/c6cp04194a

    Rational design and synthesis of noble-metal nanoframes for catalytic and photonic applications
    journal, September 2016

    • Wang, Xue; Ruditskiy, Aleksey; Xia, Younan
    • National Science Review, Vol. 3, Issue 4
    • DOI: 10.1093/nsr/nww062

    Rapid Activation of Platinum with Black Phosphorus for Efficient Hydrogen Evolution
    journal, December 2019

    • Wang, Xin; Bai, Licheng; Lu, Jiang
    • Angewandte Chemie International Edition, Vol. 58, Issue 52
    • DOI: 10.1002/anie.201911696

    Advanced Catalysts Derived from Composition‐Segregated Platinum–Nickel Nanostructures: New Opportunities and Challenges
    journal, February 2019

    • Zhang, Nan; Shao, Qi; Xiao, Xiangheng
    • Advanced Functional Materials, Vol. 29, Issue 13
    • DOI: 10.1002/adfm.201808161

    Chitosan-Covered Pd@Pt Core–Shell Nanocubes for Direct Electron Transfer in Electrochemical Enzymatic Glucose Biosensor
    journal, May 2017

    Engineering stable electrocatalysts by synergistic stabilization between carbide cores and Pt shells
    journal, December 2019

    Hollow Metal Nanocrystals with Ultrathin, Porous Walls and Well-Controlled Surface Structures
    journal, July 2018

    Nanostructured Materials for Heterogeneous Electrocatalytic CO 2 Reduction and their Related Reaction Mechanisms
    journal, July 2017

    • Zhang, Lei; Zhao, Zhi-Jian; Gong, Jinlong
    • Angewandte Chemie International Edition, Vol. 56, Issue 38
    • DOI: 10.1002/anie.201612214

    Design of Noble Metal Electrocatalysts on an Atomic Level
    journal, October 2018

    Structure Sensitivity of Formic Acid Electrooxidation on Transition Metal Surfaces: A First-Principles Study
    journal, January 2018

    • Elnabawy, Ahmed O.; Herron, Jeffrey A.; Scaranto, Jessica
    • Journal of The Electrochemical Society, Vol. 165, Issue 15
    • DOI: 10.1149/2.0161815jes

    Robust synthesis of ultrathin Au–Ag nanowires as a high-surface-area, synergistic substrate for constructing efficient Pt-based catalysts
    journal, January 2018

    • Zhang, Shumeng; Zhang, Lei; Liu, Zhaojun
    • Journal of Materials Chemistry A, Vol. 6, Issue 44
    • DOI: 10.1039/c8ta05663c

    Shape‐Controlled Synthesis of Colloidal Metal Nanocrystals by Replicating the Surface Atomic Structure on the Seed
    journal, April 2018

    Facile Aqueous-Phase Synthesis of Bimetallic (AgPt, AgPd, and CuPt) and Trimetallic (AgCuPt) Nanoparticles
    journal, January 2020

    • Tang, Zengmin; Jung, Euiyoung; Jang, Yejin
    • Materials, Vol. 13, Issue 2
    • DOI: 10.3390/ma13020254

    Surface evolution of a Pt–Pd–Au electrocatalyst for stable oxygen reduction
    journal, July 2017

    Toward affordable and sustainable use of precious metals in catalysis and nanomedicine
    journal, November 2018

    Core-Shell Structuring of Pure Metallic Aerogels towards Highly Efficient Platinum Utilization for the Oxygen Reduction Reaction
    journal, February 2018

    • Cai, Bin; Hübner, René; Sasaki, Kotaro
    • Angewandte Chemie International Edition, Vol. 57, Issue 11
    • DOI: 10.1002/anie.201710997

    Boosting Photocatalytic Water Splitting: Interfacial Charge Polarization in Atomically Controlled Core-Shell Cocatalysts
    journal, October 2015

    • Bai, Song; Yang, Li; Wang, Chunlei
    • Angewandte Chemie International Edition, Vol. 54, Issue 49
    • DOI: 10.1002/anie.201508024

    Enhancing Electrocatalytic Water Splitting by Strain Engineering
    journal, February 2019

    Constructing an Atomic Layer Pt Electrocatalyst with a Concave Curved Surface for the Oxygen Reduction Reaction
    journal, July 2017

    Enhanced oxygen reduction activity of Pt shells on PdCu truncated octahedra with different compositions
    journal, January 2018

    • Wu, Xingqiao; Xu, Qingfeng; Yan, Yucong
    • RSC Advances, Vol. 8, Issue 61
    • DOI: 10.1039/c8ra07415a

    One‐Pot Synthesis of Pd@Pt n L Core‐Shell Icosahedral Nanocrystals in High Throughput through a Quantitative Analysis of the Reduction Kinetics
    journal, March 2019

    • Lee, Chi‐Ta; Wang, Helan; Zhao, Ming
    • Chemistry – A European Journal, Vol. 25, Issue 20
    • DOI: 10.1002/chem.201900229

    Lithium Electrochemical Tuning for Electrocatalysis
    journal, September 2018

    Facile Aqueous-Phase Synthesis of Bimetallic (AgPt, AgPd, and CuPt) and Trimetallic (AgCuPt) Nanoparticles
    journal, January 2020

    • Tang, Zengmin; Jung, Euiyoung; Jang, Yejin
    • Materials, Vol. 13, Issue 2
    • DOI: 10.3390/ma13020254

    Highly Active and Stable Pt-Pd Alloy Catalysts Synthesized by Room-Temperature Electron Reduction for Oxygen Reduction Reaction
    journal, January 2017

    Fabrication of Pd/P nanoparticle networks with high activity for methanol oxidation
    journal, January 2016

    • Zhang, Ke; Wang, Caiqin; Bin, Duan
    • Catalysis Science & Technology, Vol. 6, Issue 16
    • DOI: 10.1039/c6cy00789a

    Recent Developments in Electrocatalysts and Hybrid Electrocatalyst Support Systems for Polymer Electrolyte Fuel Cells
    book, January 2017

    • Sharma, Surbhi
    • Electrocatalysts for Low Temperature Fuel Cells: Fundamentals and Recent Trends
    • DOI: 10.1002/9783527803873.ch7

    Kern-Schale-Strukturierung rein metallischer Aerogele für eine hocheffiziente Nutzung von Platin für die Sauerstoffreduktion
    journal, February 2018

    Highly stable Pt 3 Ni nanowires tailored with trace Au for the oxygen reduction reaction
    journal, January 2019

    • Wu, Zhifu; Su, Ya-Qiong; Hensen, Emiel J. M.
    • Journal of Materials Chemistry A, Vol. 7, Issue 46
    • DOI: 10.1039/c9ta08682j

    Hollow nanoparticles as emerging electrocatalysts for renewable energy conversion reactions
    journal, January 2018

    • Park, Jongsik; Kwon, Taehyun; Kim, Jun
    • Chemical Society Reviews, Vol. 47, Issue 22
    • DOI: 10.1039/c8cs00336j

    Preparation of hollow PtCu nanoparticles as high-performance electrocatalysts for oxygen reduction reaction in the absence of a surfactant
    journal, January 2016

    • Cao, Longsheng; Zhang, Geng; Lu, Wangting
    • RSC Advances, Vol. 6, Issue 46
    • DOI: 10.1039/c6ra04619c

    Functional Applications of Metallic Glasses in Electrocatalysis
    journal, April 2019

    Engineering one-dimensional and hierarchical PtFe alloy assemblies towards durable methanol electrooxidation
    journal, January 2019

    • Wang, Lijuan; Tian, Xin Long; Xu, Yangyang
    • Journal of Materials Chemistry A, Vol. 7, Issue 21
    • DOI: 10.1039/c9ta02508a

    Morphology led high dispersion of Pt icosahedral nanocrystals on carbon nanotubes for enhanced electro-catalytic activity and stability
    journal, January 2018

    • Du, Guifen; Zhang, Jiawei; Chen, Qiaoli
    • Chemical Communications, Vol. 54, Issue 77
    • DOI: 10.1039/c8cc05213a

    Superior Bifunctional Liquid Fuel Oxidation and Oxygen Reduction Electrocatalysis Enabled by PtNiPd Core-Shell Nanowires
    journal, December 2016

    Boosting Photocatalytic Water Splitting: Interfacial Charge Polarization in Atomically Controlled Core–Shell Cocatalysts
    journal, October 2015

    Biaxially strained PtPb/Pt core/shell nanoplate boosts oxygen reduction catalysis
    journal, December 2016

    Tuning the electrocatalytic activity of Pt by structurally ordered PdFe/C for the hydrogen oxidation reaction in alkaline media
    journal, January 2018

    • Xiao, Weiping; Lei, Wen; Wang, Jie
    • Journal of Materials Chemistry A, Vol. 6, Issue 24
    • DOI: 10.1039/c8ta03250e
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