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Title: Optimizing the ORR activity of Pd based nanocatalysts by tuning their strain and particle size

Abstract

Controlling of the particle size and surface strain is the key to tuning the surface chemistry and optimizing the catalytic performance of electrocatalysts. In this study, we show that by introducing both Fe and Co into Pd lattices, the surface strain of Pd nanocatalysts can be tuned to optimize their oxygen reduction activity in both fuel cells and Zn–air batteries. The Pd2FeCo/C alloy particles are uniquely coated with an ultrathin Fe2O3 shell which is in situ formed during a thermal annealing treatment. The thin shell acts as an effective barrier that prevents the coalescence and ripening of Pd2FeCo/C nanoparticles. Compared with Pd/C, Pd2FeCo/C exhibits higher catalytic activity and long-term stability for the ORR, signifying changes in catalytic behavior due to particle sizes and strain effects. Moreover, by spontaneous decoration of Pt on the surface of Pd2FeCo/C, the Pd2FeCo@Pt/C core@shell structure was formed and the Pt mass activity was about 37.6 and 112.5 times higher than that on Pt/C in a 0.1 M HClO4 and KOH solution at 0.9 V, respectively, suggesting an enhanced ORR performance after Pt decoration. More interestingly, Pd2FeCo@Pt/C also shows a power density of ~308 mW cm-2, which is much higher than that of Pt/C (175 mWmore » cm-2), and excellent durability in a home-made Zn–air battery.« less

Authors:
 [1];  [2];  [1];  [3];  [1];  [1];  [1]; ORCiD logo [2]; ORCiD logo [1]
  1. Huazhong Univ. of Science and Technology, Wuhan (China). Ministry of Education and Key Lab. of Material Chemistry for Energy Conversion and Storage, Hubei Key Lab. of Material Chemistry and Service Failure and School of Chemistry and Chemical Engineering
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  3. Tianjin Univ. (China). School of Materials Science and Engineering
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NSFC); Huazhong Univ. of Science and Technology, Wuhan (China)
OSTI Identifier:
1431451
Report Number(s):
BNL-203451-2018-JAAM
Journal ID: ISSN 2050-7488; JMCAET; TRN: US1802938
Grant/Contract Number:  
SC0012704; 21573083; NCET-13-0237
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 5; Journal Issue: 20; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 25 ENERGY STORAGE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; ORR activity

Citation Formats

Xiao, Weiping, Liutheviciene Cordeiro, Marco Aurelio, Gong, Mingxing, Han, Lili, Wang, Jie, Bian, Ce, Zhu, Jing, Xin, Huolin L., and Wang, Deli. Optimizing the ORR activity of Pd based nanocatalysts by tuning their strain and particle size. United States: N. p., 2017. Web. doi:10.1039/C7TA02479G.
Xiao, Weiping, Liutheviciene Cordeiro, Marco Aurelio, Gong, Mingxing, Han, Lili, Wang, Jie, Bian, Ce, Zhu, Jing, Xin, Huolin L., & Wang, Deli. Optimizing the ORR activity of Pd based nanocatalysts by tuning their strain and particle size. United States. https://doi.org/10.1039/C7TA02479G
Xiao, Weiping, Liutheviciene Cordeiro, Marco Aurelio, Gong, Mingxing, Han, Lili, Wang, Jie, Bian, Ce, Zhu, Jing, Xin, Huolin L., and Wang, Deli. Tue . "Optimizing the ORR activity of Pd based nanocatalysts by tuning their strain and particle size". United States. https://doi.org/10.1039/C7TA02479G. https://www.osti.gov/servlets/purl/1431451.
@article{osti_1431451,
title = {Optimizing the ORR activity of Pd based nanocatalysts by tuning their strain and particle size},
author = {Xiao, Weiping and Liutheviciene Cordeiro, Marco Aurelio and Gong, Mingxing and Han, Lili and Wang, Jie and Bian, Ce and Zhu, Jing and Xin, Huolin L. and Wang, Deli},
abstractNote = {Controlling of the particle size and surface strain is the key to tuning the surface chemistry and optimizing the catalytic performance of electrocatalysts. In this study, we show that by introducing both Fe and Co into Pd lattices, the surface strain of Pd nanocatalysts can be tuned to optimize their oxygen reduction activity in both fuel cells and Zn–air batteries. The Pd2FeCo/C alloy particles are uniquely coated with an ultrathin Fe2O3 shell which is in situ formed during a thermal annealing treatment. The thin shell acts as an effective barrier that prevents the coalescence and ripening of Pd2FeCo/C nanoparticles. Compared with Pd/C, Pd2FeCo/C exhibits higher catalytic activity and long-term stability for the ORR, signifying changes in catalytic behavior due to particle sizes and strain effects. Moreover, by spontaneous decoration of Pt on the surface of Pd2FeCo/C, the Pd2FeCo@Pt/C core@shell structure was formed and the Pt mass activity was about 37.6 and 112.5 times higher than that on Pt/C in a 0.1 M HClO4 and KOH solution at 0.9 V, respectively, suggesting an enhanced ORR performance after Pt decoration. More interestingly, Pd2FeCo@Pt/C also shows a power density of ~308 mW cm-2, which is much higher than that of Pt/C (175 mW cm-2), and excellent durability in a home-made Zn–air battery.},
doi = {10.1039/C7TA02479G},
journal = {Journal of Materials Chemistry. A},
number = 20,
volume = 5,
place = {United States},
year = {Tue Apr 18 00:00:00 EDT 2017},
month = {Tue Apr 18 00:00:00 EDT 2017}
}

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Works referenced in this record:

Structurally ordered intermetallic platinum–cobalt core–shell nanoparticles with enhanced activity and stability as oxygen reduction electrocatalysts
journal, October 2012

  • Wang, Deli; Xin, Huolin L.; Hovden, Robert
  • Nature Materials, Vol. 12, Issue 1, p. 81-87
  • DOI: 10.1038/nmat3458

Pd−Fe Nanoparticles as Electrocatalysts for Oxygen Reduction
journal, March 2006

  • Shao, Min-Hua; Sasaki, Kotaro; Adzic, Radoslav R.
  • Journal of the American Chemical Society, Vol. 128, Issue 11
  • DOI: 10.1021/ja060167d

First-Principles Considerations in the Design of Pd-Alloy Catalysts for Oxygen Reduction
journal, April 2007

  • Suo, Yange; Zhuang, Lin; Lu, Juntao
  • Angewandte Chemie International Edition, Vol. 46, Issue 16
  • DOI: 10.1002/anie.200604332

Bimetallic Nanocrystals: Syntheses, Properties, and Applications
journal, July 2016


Origin of Enhanced Activity in Palladium Alloy Electrocatalysts for Oxygen Reduction Reaction
journal, June 2007

  • Shao, Minhua; Liu, Ping; Zhang, Junliang
  • The Journal of Physical Chemistry B, Vol. 111, Issue 24
  • DOI: 10.1021/jp0689971

Structurally Ordered FePt Nanoparticles and Their Enhanced Catalysis for Oxygen Reduction Reaction
journal, April 2010

  • Kim, Jaemin; Lee, Youngmin; Sun, Shouheng
  • Journal of the American Chemical Society, Vol. 132, Issue 14
  • DOI: 10.1021/ja1009629

Confined-Space Alloying of Nanoparticles for the Synthesis of Efficient PtNi Fuel-Cell Catalysts
journal, October 2014

  • Baldizzone, Claudio; Mezzavilla, Stefano; Carvalho, Hudson W. P.
  • Angewandte Chemie International Edition, Vol. 53, Issue 51
  • DOI: 10.1002/anie.201406812

Cu–Pt Nanocage with 3-D Electrocatalytic Surface as an Efficient Oxygen Reduction Electrocatalyst for a Primary Zn–Air Battery
journal, January 2015

  • Dhavale, Vishal M.; Kurungot, Sreekumar
  • ACS Catalysis, Vol. 5, Issue 3
  • DOI: 10.1021/cs501571e

From Core/Shell Structured FePt/Fe 3 O 4 /MgO to Ferromagnetic FePt Nanoparticles
journal, December 2008

  • Kim, Jaemin; Rong, Chuanbing; Lee, Youngmin
  • Chemistry of Materials, Vol. 20, Issue 23
  • DOI: 10.1021/cm8024878

New Approach to Fully Ordered fct-FePt Nanoparticles for Much Enhanced Electrocatalysis in Acid
journal, March 2015


Synthesis and Magnetic Properties of Silica-Coated FePt Nanocrystals
journal, June 2006

  • Lee, Doh C.; Mikulec, Frederic V.; Pelaez, José M.
  • The Journal of Physical Chemistry B, Vol. 110, Issue 23, p. 11160-11166
  • DOI: 10.1021/jp060974z

High-performance transition metal-doped Pt3Ni octahedra for oxygen reduction reaction
journal, June 2015


Ultra-low overpotential and high rate capability in Li–O2 batteries through surface atom arrangement of PdCu nanocatalysts
journal, January 2014

  • Choi, Ran; Jung, Jaepyeong; Kim, Gyubong
  • Energy & Environmental Science, Vol. 7, Issue 4
  • DOI: 10.1039/c3ee43437k

Improved adsorption energetics within density-functional theory using revised Perdew-Burke-Ernzerhof functionals
journal, March 1999


Palladium Monolayer and Palladium Alloy Electrocatalysts for Oxygen Reduction
journal, December 2006


A Synthetic Route to Size-Controlled fcc and fct FePt Nanoparticles
journal, July 2005

  • Howard, Luciano E. M.; Nguyen, H. Loc; Giblin, Sean R.
  • Journal of the American Chemical Society, Vol. 127, Issue 29
  • DOI: 10.1021/ja051669e

Nanocatalyst Superior to Pt for Oxygen Reduction Reactions: The Case of Core/Shell Ag(Au)/CuPd Nanoparticles
journal, October 2014

  • Guo, Shaojun; Zhang, Xu; Zhu, Wenlei
  • Journal of the American Chemical Society, Vol. 136, Issue 42
  • DOI: 10.1021/ja508256g

Highly Durable and Active PtFe Nanocatalyst for Electrochemical Oxygen Reduction Reaction
journal, December 2015

  • Chung, Dong Young; Jun, Samuel Woojoo; Yoon, Gabin
  • Journal of the American Chemical Society, Vol. 137, Issue 49
  • DOI: 10.1021/jacs.5b09653

Size-Dependent Disorder–Order Transformation in the Synthesis of Monodisperse Intermetallic PdCu Nanocatalysts
journal, May 2016


Extremely Stable Platinum Nanoparticles Encapsulated in a Zirconia Nanocage by Area-Selective Atomic Layer Deposition for the Oxygen Reduction Reaction
journal, November 2014

  • Cheng, Niancai; Banis, Mohammad Norouzi; Liu, Jian
  • Advanced Materials, Vol. 27, Issue 2
  • DOI: 10.1002/adma.201404314

Five-Fold Twinned Pd 2 NiAg Nanocrystals with Increased Surface Ni Site Availability to Improve Oxygen Reduction Activity
journal, February 2015

  • Liu, Suli; Zhang, Qinghua; Li, Yafei
  • Journal of the American Chemical Society, Vol. 137, Issue 8
  • DOI: 10.1021/ja5129154

Enhancing the catalytic and electrocatalytic properties of Pt-based catalysts by forming bimetallic nanocrystals with Pd
journal, January 2012

  • Zhang, Hui; Jin, Mingshang; Xia, Younan
  • Chemical Society Reviews, Vol. 41, Issue 24
  • DOI: 10.1039/c2cs35173k

Advanced zinc-air batteries based on high-performance hybrid electrocatalysts
journal, May 2013

  • Li, Yanguang; Gong, Ming; Liang, Yongye
  • Nature Communications, Vol. 4, Issue 1
  • DOI: 10.1038/ncomms2812

Synthesis of PdNi catalysts for the oxidation of ethanol in alkaline direct ethanol fuel cells
journal, February 2010


Toward Highly Stable Electrocatalysts via Nanoparticle Pore Confinement
journal, December 2012

  • Galeano, Carolina; Meier, Josef C.; Peinecke, Volker
  • Journal of the American Chemical Society, Vol. 134, Issue 50
  • DOI: 10.1021/ja308570c

An oxygen reduction electrocatalyst based on carbon nanotube–graphene complexes
journal, May 2012

  • Li, Yanguang; Zhou, Wu; Wang, Hailiang
  • Nature Nanotechnology, Vol. 7, Issue 6
  • DOI: 10.1038/nnano.2012.72

Improved Oxygen Reduction Activity on Pt3Ni(111) via Increased Surface Site Availability
journal, January 2007

  • Stamenkovic, V. R.; Fowler, B.; Mun, B. S.
  • Science, Vol. 315, Issue 5811, p. 493-497
  • DOI: 10.1126/science.1135941

First-Principles Considerations in the Design of Pd-Alloy Catalysts for Oxygen Reduction
journal, April 2007


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Unique Half Embedded/Exposed PdFeCu/C Interfacial Nanoalloy as High‐Performance Electrocatalyst for Oxygen Reduction Reaction
journal, June 2019

  • Jyoti Borah, Biraj; Saikia, Himadri; Goswami, Chiranjita
  • ChemCatChem, Vol. 11, Issue 15
  • DOI: 10.1002/cctc.201900469

Highly‐Branched Palladium Nanodandelions: Simple, Fast, and Green Fabrication with Superior Oxygen Reduction Property
journal, March 2019

  • Fan, Chuang; Huang, Zihan; Wang, Chao
  • Chemistry – A European Journal, Vol. 25, Issue 19
  • DOI: 10.1002/chem.201805521

Yolk-Shell Fe/Fe 4 N@Pd/C Magnetic Nanocomposite as an Efficient Recyclable ORR Electrocatalyst and SERS Substrate
journal, January 2019


Electrodeposition-fabricated PtCu-alloy cathode catalysts for high-temperature proton exchange membrane fuel cells
journal, May 2018

  • Park, Hyanjoo; Kim, Kyung Min; Kim, Hoyoung
  • Korean Journal of Chemical Engineering, Vol. 35, Issue 7
  • DOI: 10.1007/s11814-018-0059-z

Highly active zigzag-like Pt-Zn alloy nanowires with high-index facets for alcohol electrooxidation
journal, April 2019


Surface composition-tunable octahedral PtCu nanoalloys advance the electrocatalytic performance on methanol and ethanol oxidation
journal, July 2019


Dendritic defect-rich palladium–copper–cobalt nanoalloys as robust multifunctional non-platinum electrocatalysts for fuel cells
journal, September 2018


PDA-assisted formation of ordered intermetallic CoPt 3 catalysts with enhanced oxygen reduction activity and stability
journal, January 2018

  • Zhao, Yige; Wang, Chen; Liu, Jingjun
  • Nanoscale, Vol. 10, Issue 19
  • DOI: 10.1039/c8nr02207k

Electrocatalytic activity of electrochemically dealloyed PdCu 3 intermetallic compound towards oxygen reduction reaction in acidic media
journal, January 2018

  • Gunji, Takao; Noh, Seung Hyo; Ando, Fuma
  • Journal of Materials Chemistry A, Vol. 6, Issue 30
  • DOI: 10.1039/c8ta03233e

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

Interfacial proton enrichment enhances proton-coupled electrocatalytic reactions
journal, January 2018

  • Zhao, Yue; Ding, Yu; Qiao, Bin
  • Journal of Materials Chemistry A, Vol. 6, Issue 36
  • DOI: 10.1039/c8ta06856a

Recent advancements in Pt-nanostructure-based electrocatalysts for the oxygen reduction reaction
journal, January 2019

  • Mahata, Arup; Nair, Akhil S.; Pathak, Biswarup
  • Catalysis Science & Technology, Vol. 9, Issue 18
  • DOI: 10.1039/c9cy00895k

DFT Study on Intermetallic Pd–Cu Alloy with Cover Layer Pd as Efficient Catalyst for Oxygen Reduction Reaction
journal, December 2017