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Title: Atomic Layer-by-Layer Deposition of Pt on Pd Nanocubes for Catalysts with Enhanced Activity and Durability toward Oxygen Reduction

Abstract

Here, an effective strategy for reducing the Pt content while retaining the activity of a Pt-based catalyst is to deposit the Pt atoms as ultrathin skins of only a few atomic layers thick on nanoscale substrates made of another metal. During deposition, however, the Pt atoms often take an island growth mode because of a strong bonding between Pt atoms. Here we report a versatile route to the conformal deposition of Pt as uniform, ultrathin shells on Pd nanocubes in a solution phase. The introduction of the Pt precursor at a relatively slow rate and high temperature allowed the deposited Pt atoms to spread across the entire surface of a Pd nanocube to generate a uniform shell. The thickness of the Pt shell could be controlled from one to six atomic layers by varying the amount of Pt precursor added into the system. Compared to a commercial Pt/C catalyst, the Pd@PtnL (n = 1–6) core–shell nanocubes showed enhancements in specific activity and durability toward the oxygen reduction reaction (ORR). Density functional theory (DFT) calculations on model (100) surfaces suggest that the enhancement in specific activity can be attributed to the weakening of OH binding through ligand and strain effects, which,more » in turn, increases the rate of OH hydrogenation. A volcano-type relationship between the ORR specific activity and the number of Pt atomic layers was derived, in good agreement with the experimental results. Both theoretical and experimental studies indicate that the ORR specific activity was maximized for the catalysts based on Pd@Pt2–3L nanocubes. Because of the reduction in Pt content used and the enhancement in specific activity, the Pd@Pt1L nanocubes showed a Pt mass activity with almost three-fold enhancement relative to the Pt/C catalyst.« less

Authors:
 [1];  [1];  [2];  [3];  [3];  [1];  [4];  [2];  [2];  [5];  [3];  [6]
  1. Georgia Institute of Technology and Emory Univ., Atlanta, GA (United States); Xiamen Univ., Fujian (China)
  2. Univ. of Texas at Dallas, Richardson, TX (United States)
  3. Univ. of Wisconsin-Madison, Madison, WI (United States)
  4. Georgia Inst. of Technology, Atlanta, GA (United States)
  5. Xiamen Univ., Fujian (China)
  6. Georgia Institute of Technology and Emory Univ., Atlanta, GA (United States)
Publication Date:
Research Org.:
Univ. of Wisconsin, Madison, WI (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Contributing Org.:
EMSL; CNM at ANL; and NERSC
OSTI Identifier:
1396241
Grant/Contract Number:  
FG02-05ER15731
Resource Type:
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 14; Journal Issue: 6; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; bimetallic catalyst; core−shell nanostructure; fuel cell; oxygen reduction reaction; Platinum-based catalyst

Citation Formats

Xie, Shuifen, Choi, Sang -Il, Lu, Ning, Roling, Luke T., Herron, Jeffrey A., Zhang, Lei, Park, Jinho, Wang, Jinguo, Kim, Moon J., Xie, Zhaoxiong, Mavrikakis, Manos, and Xia, Younan. Atomic Layer-by-Layer Deposition of Pt on Pd Nanocubes for Catalysts with Enhanced Activity and Durability toward Oxygen Reduction. United States: N. p., 2014. Web. doi:10.1021/nl501205j.
Xie, Shuifen, Choi, Sang -Il, Lu, Ning, Roling, Luke T., Herron, Jeffrey A., Zhang, Lei, Park, Jinho, Wang, Jinguo, Kim, Moon J., Xie, Zhaoxiong, Mavrikakis, Manos, & Xia, Younan. Atomic Layer-by-Layer Deposition of Pt on Pd Nanocubes for Catalysts with Enhanced Activity and Durability toward Oxygen Reduction. United States. https://doi.org/10.1021/nl501205j
Xie, Shuifen, Choi, Sang -Il, Lu, Ning, Roling, Luke T., Herron, Jeffrey A., Zhang, Lei, Park, Jinho, Wang, Jinguo, Kim, Moon J., Xie, Zhaoxiong, Mavrikakis, Manos, and Xia, Younan. Mon . "Atomic Layer-by-Layer Deposition of Pt on Pd Nanocubes for Catalysts with Enhanced Activity and Durability toward Oxygen Reduction". United States. https://doi.org/10.1021/nl501205j. https://www.osti.gov/servlets/purl/1396241.
@article{osti_1396241,
title = {Atomic Layer-by-Layer Deposition of Pt on Pd Nanocubes for Catalysts with Enhanced Activity and Durability toward Oxygen Reduction},
author = {Xie, Shuifen and Choi, Sang -Il and Lu, Ning and Roling, Luke T. and Herron, Jeffrey A. and Zhang, Lei and Park, Jinho and Wang, Jinguo and Kim, Moon J. and Xie, Zhaoxiong and Mavrikakis, Manos and Xia, Younan},
abstractNote = {Here, an effective strategy for reducing the Pt content while retaining the activity of a Pt-based catalyst is to deposit the Pt atoms as ultrathin skins of only a few atomic layers thick on nanoscale substrates made of another metal. During deposition, however, the Pt atoms often take an island growth mode because of a strong bonding between Pt atoms. Here we report a versatile route to the conformal deposition of Pt as uniform, ultrathin shells on Pd nanocubes in a solution phase. The introduction of the Pt precursor at a relatively slow rate and high temperature allowed the deposited Pt atoms to spread across the entire surface of a Pd nanocube to generate a uniform shell. The thickness of the Pt shell could be controlled from one to six atomic layers by varying the amount of Pt precursor added into the system. Compared to a commercial Pt/C catalyst, the Pd@PtnL (n = 1–6) core–shell nanocubes showed enhancements in specific activity and durability toward the oxygen reduction reaction (ORR). Density functional theory (DFT) calculations on model (100) surfaces suggest that the enhancement in specific activity can be attributed to the weakening of OH binding through ligand and strain effects, which, in turn, increases the rate of OH hydrogenation. A volcano-type relationship between the ORR specific activity and the number of Pt atomic layers was derived, in good agreement with the experimental results. Both theoretical and experimental studies indicate that the ORR specific activity was maximized for the catalysts based on Pd@Pt2–3L nanocubes. Because of the reduction in Pt content used and the enhancement in specific activity, the Pd@Pt1L nanocubes showed a Pt mass activity with almost three-fold enhancement relative to the Pt/C catalyst.},
doi = {10.1021/nl501205j},
journal = {Nano Letters},
number = 6,
volume = 14,
place = {United States},
year = {Mon May 05 00:00:00 EDT 2014},
month = {Mon May 05 00:00:00 EDT 2014}
}

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Shaping well-defined noble-metal-based nanostructures for fabricating high-performance electrocatalysts: advances and perspectives
journal, January 2019

  • Yin, Hai-Jing; Zhou, Jun-Hao; Zhang, Ya-Wen
  • Inorganic Chemistry Frontiers, Vol. 6, Issue 10
  • DOI: 10.1039/c9qi00689c

Acetylene in Organic Synthesis: Recent Progress and New Uses
journal, September 2018

  • Voronin, Vladimir V.; Ledovskaya, Maria S.; Bogachenkov, Alexander S.
  • Molecules, Vol. 23, Issue 10
  • DOI: 10.3390/molecules23102442

Sulfur-doping achieves efficient oxygen reduction in pyrolyzed zeolitic imidazolate frameworks
journal, January 2016

  • Zhang, Chao; An, Bing; Yang, Ling
  • Journal of Materials Chemistry A, Vol. 4, Issue 12
  • DOI: 10.1039/c6ta00768f

Well-faceted noble-metal nanocrystals with nonconvex polyhedral shapes
journal, January 2016

  • Chen, Qiaoli; Jia, Yanyan; Xie, Shuifen
  • Chemical Society Reviews, Vol. 45, Issue 11
  • DOI: 10.1039/c6cs00039h

Porous AgPd-Pd Composite Nanotubes as Highly Efficient Electrocatalysts for Lithium-Oxygen Batteries
journal, September 2015

  • Luo, Wen-Bin; Gao, Xuan-Wen; Chou, Shu-Lei
  • Advanced Materials, Vol. 27, Issue 43
  • DOI: 10.1002/adma.201502262

Pt-Based electrocatalysts with high atom utilization efficiency: from nanostructures to single atoms
journal, January 2019

  • Zhang, Lei; Doyle-Davis, Kieran; Sun, Xueliang
  • Energy & Environmental Science, Vol. 12, Issue 2
  • DOI: 10.1039/c8ee02939c

Shape-controlled synthesis of Au–Pd bimetallic nanocrystals for catalytic applications
journal, January 2016

  • Zhang, Lei; Xie, Zhaoxiong; Gong, Jinlong
  • Chemical Society Reviews, Vol. 45, Issue 14
  • DOI: 10.1039/c5cs00958h

Continuous Flow Routes toward Designer Metal Nanocatalysts
journal, September 2019

  • Santana, Joshua S.; Skrabalak, Sara E.
  • Advanced Energy Materials, Vol. 10, Issue 11
  • DOI: 10.1002/aenm.201902051

Concave Pd-Pt Core-Shell Nanocrystals with Ultrathin Pt Shell Feature and Enhanced Catalytic Performance
journal, December 2015


Alloy Nanocatalysts for the Electrochemical Oxygen Reduction (ORR) and the Direct Electrochemical Carbon Dioxide Reduction Reaction (CO 2 RR)
journal, December 2018

  • Kim, Cheonghee; Dionigi, Fabio; Beermann, Vera
  • Advanced Materials, Vol. 31, Issue 31
  • DOI: 10.1002/adma.201805617

Precursor-mediated size tuning of monodisperse PtRh nanocubes as efficient electrocatalysts for ethylene glycol oxidation
journal, January 2019

  • Gao, Fei; Zhang, Yangping; Song, Pingping
  • Journal of Materials Chemistry A, Vol. 7, Issue 13
  • DOI: 10.1039/c9ta01071h

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

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


A general seed-mediated approach to the synthesis of AgM (M = Au, Pt, and Pd) core–shell nanoplates and their SERS properties
journal, January 2017

  • Kumar-Krishnan, Siva; Estevez-González, M.; Pérez, Ramiro
  • RSC Advances, Vol. 7, Issue 44
  • DOI: 10.1039/c7ra04301e

Surfactant-Stripped Micelles of Near Infrared Dye and Paclitaxel for Photoacoustic Imaging Guided Photothermal-Chemotherapy
journal, October 2018


Intermetallic Nanocrystals: Syntheses and Catalytic Applications
journal, February 2017

  • Yan, Yucong; Du, Jingshan S.; Gilroy, Kyle D.
  • Advanced Materials, Vol. 29, Issue 14
  • DOI: 10.1002/adma.201605997

A highly durable carbon-nanofiber-supported Pt–C core–shell cathode catalyst for ultra-low Pt loading proton exchange membrane fuel cells: facile carbon encapsulation
journal, January 2019

  • Karuppannan, Mohanraju; Kim, Youngkwang; Gok, Sujin
  • Energy & Environmental Science, Vol. 12, Issue 9
  • DOI: 10.1039/c9ee01000a

Core–shell-structured nanoporous PtCu with high Cu content and enhanced catalytic performance
journal, January 2015

  • Qiu, H. -J.; Xu, H. T.; Li, X.
  • Journal of Materials Chemistry A, Vol. 3, Issue 15
  • DOI: 10.1039/c5ta00020c

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


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


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


Palladium–platinum core-shell icosahedra with substantially enhanced activity and durability towards oxygen reduction
journal, July 2015

  • Wang, Xue; Choi, Sang-Il; Roling, Luke T.
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms8594

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


Shape-Controlled Synthesis of Pt Nanopeanuts
journal, August 2016

  • Zhang, Xuemei; Xia, Zengzilu; Huang, Yingzhou
  • Scientific Reports, Vol. 6, Issue 1
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Reduction rate as a quantitative knob for achieving deterministic synthesis of colloidal metal nanocrystals
journal, January 2017

  • Yang, Tung-Han; Gilroy, Kyle D.; Xia, Younan
  • Chemical Science, Vol. 8, Issue 10
  • DOI: 10.1039/c7sc02833d

Facile aqueous-phase synthesis of Ag–Cu–Pt–Pd quadrometallic nanoparticles
journal, December 2019


Acetylene in Organic Synthesis: Recent Progress and New Uses
journal, September 2018

  • Voronin, Vladimir V.; Ledovskaya, Maria S.; Bogachenkov, Alexander S.
  • Molecules, Vol. 23, Issue 10
  • DOI: 10.3390/molecules23102442

Nanostructure Optimization of Platinum-Based Nanomaterials for Catalytic Applications
journal, November 2018

  • Duan, Sibin; Du, Zhe; Fan, Hongsheng
  • Nanomaterials, Vol. 8, Issue 11
  • DOI: 10.3390/nano8110949