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Title: Optimizing PtFe intermetallics for oxygen reduction reaction: from DFT screening to in situ XAFS characterization

Abstract

Rational designing of catalysts to promote the sluggish kinetics of the cathode oxygen reduction reaction in proton exchange membrane fuel cells is still challenging, yet of crucial importance to its commercial application. Here, on the basis of theoretical DFT calculations which suggest that order structured fct-phased PtFe (O-PtFe) with an atomic Pt shell exhibits superior electrocatalytic performance towards the ORR, the desired structure was prepared by using a scalable impregnation–reduction method. The as-prepared O-PtFe delivered enhanced activity (0.68 A mg-1Pt) and stability (73% activity retention after 10 000 potential cycles) compared with the corresponding disordered PtFe alloy (D-PtFe) and Pt. To confirm the excellent durability, in situ X-ray absorption fine structure spectroscopy was conducted to probe the local and electronic structure changes of O-PtFe during 10 000 cycle accelerated durability testing. In conclusion, we hope that this facile synthesis method and the in situ XAFS experiment could be readily adapted to other catalyst systems, facilitating the screening of highly efficient ORR catalysts for fuel cell application.

Authors:
 [1];  [1];  [2];  [3];  [1];  [1];  [1];  [2];  [1]; ORCiD logo [2];  [2];  [2];  [2]; ORCiD logo [2];  [2];  [4]; ORCiD logo [1]
  1. Huazhong University of Science and Technology, Wuhan (China)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Xinyang Normal Univ. (China)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States); Univ. of California, Irvine, CA (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1580265
Alternate Identifier(s):
OSTI ID: 1571310
Report Number(s):
BNL-212448-2019-JAAM
Journal ID: ISSN 2040-3364; NANOHL
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Nanoscale
Additional Journal Information:
Journal Volume: 11; Journal Issue: 42; Journal ID: ISSN 2040-3364
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Gong, Mingxing, Zhu, Jing, Liu, Mingjie, Liu, Peifang, Deng, Zhiping, Shen, Tao, Zhao, Tonghui, Lin, Ruoqian, Lu, Yun, Yang, Shize, Liang, Zhixiu, Bak, Seong Min, Stavitski, Eli, Wu, Qin, Adzic, Radoslav R., Xin, Huolin L., and Wang, Deli. Optimizing PtFe intermetallics for oxygen reduction reaction: from DFT screening to in situ XAFS characterization. United States: N. p., 2019. Web. https://doi.org/10.1039/C9NR04975D.
Gong, Mingxing, Zhu, Jing, Liu, Mingjie, Liu, Peifang, Deng, Zhiping, Shen, Tao, Zhao, Tonghui, Lin, Ruoqian, Lu, Yun, Yang, Shize, Liang, Zhixiu, Bak, Seong Min, Stavitski, Eli, Wu, Qin, Adzic, Radoslav R., Xin, Huolin L., & Wang, Deli. Optimizing PtFe intermetallics for oxygen reduction reaction: from DFT screening to in situ XAFS characterization. United States. https://doi.org/10.1039/C9NR04975D
Gong, Mingxing, Zhu, Jing, Liu, Mingjie, Liu, Peifang, Deng, Zhiping, Shen, Tao, Zhao, Tonghui, Lin, Ruoqian, Lu, Yun, Yang, Shize, Liang, Zhixiu, Bak, Seong Min, Stavitski, Eli, Wu, Qin, Adzic, Radoslav R., Xin, Huolin L., and Wang, Deli. Tue . "Optimizing PtFe intermetallics for oxygen reduction reaction: from DFT screening to in situ XAFS characterization". United States. https://doi.org/10.1039/C9NR04975D. https://www.osti.gov/servlets/purl/1580265.
@article{osti_1580265,
title = {Optimizing PtFe intermetallics for oxygen reduction reaction: from DFT screening to in situ XAFS characterization},
author = {Gong, Mingxing and Zhu, Jing and Liu, Mingjie and Liu, Peifang and Deng, Zhiping and Shen, Tao and Zhao, Tonghui and Lin, Ruoqian and Lu, Yun and Yang, Shize and Liang, Zhixiu and Bak, Seong Min and Stavitski, Eli and Wu, Qin and Adzic, Radoslav R. and Xin, Huolin L. and Wang, Deli},
abstractNote = {Rational designing of catalysts to promote the sluggish kinetics of the cathode oxygen reduction reaction in proton exchange membrane fuel cells is still challenging, yet of crucial importance to its commercial application. Here, on the basis of theoretical DFT calculations which suggest that order structured fct-phased PtFe (O-PtFe) with an atomic Pt shell exhibits superior electrocatalytic performance towards the ORR, the desired structure was prepared by using a scalable impregnation–reduction method. The as-prepared O-PtFe delivered enhanced activity (0.68 A mg-1Pt) and stability (73% activity retention after 10 000 potential cycles) compared with the corresponding disordered PtFe alloy (D-PtFe) and Pt. To confirm the excellent durability, in situ X-ray absorption fine structure spectroscopy was conducted to probe the local and electronic structure changes of O-PtFe during 10 000 cycle accelerated durability testing. In conclusion, we hope that this facile synthesis method and the in situ XAFS experiment could be readily adapted to other catalyst systems, facilitating the screening of highly efficient ORR catalysts for fuel cell application.},
doi = {10.1039/C9NR04975D},
journal = {Nanoscale},
number = 42,
volume = 11,
place = {United States},
year = {2019},
month = {9}
}

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Works referenced in this record:

Recent Advances in Electrocatalysts for Oxygen Reduction Reaction
journal, February 2016


Enhanced Electrocatalytic Performance of Processed, Ultrathin, Supported Pd–Pt Core–Shell Nanowire Catalysts for the Oxygen Reduction Reaction
journal, June 2011

  • Koenigsmann, Christopher; Santulli, Alexander C.; Gong, Kuanping
  • Journal of the American Chemical Society, Vol. 133, Issue 25
  • DOI: 10.1021/ja111130t

Recent advancements in Pt and Pt-free catalysts for oxygen reduction reaction
journal, January 2015

  • Nie, Yao; Li, Li; Wei, Zidong
  • Chemical Society Reviews, Vol. 44, Issue 8
  • DOI: 10.1039/C4CS00484A

Highly stable Pt monolayer on PdAu nanoparticle electrocatalysts for the oxygen reduction reaction
journal, January 2012

  • Sasaki, Kotaro; Naohara, Hideo; Choi, YongMan
  • Nature Communications, Vol. 3, Issue 1
  • DOI: 10.1038/ncomms2124

Tuning Nanoparticle Catalysis for the Oxygen Reduction Reaction
journal, June 2013

  • Guo, Shaojun; Zhang, Sen; Sun, Shouheng
  • Angewandte Chemie International Edition, Vol. 52, Issue 33
  • DOI: 10.1002/anie.201207186

Platinum-Based Oxygen Reduction Electrocatalysts
journal, April 2013

  • Wu, Jianbo; Yang, Hong
  • Accounts of Chemical Research, Vol. 46, Issue 8
  • DOI: 10.1021/ar300359w

Pd-Pt Bimetallic Nanodendrites with High Activity for Oxygen Reduction
journal, May 2009


Highly Crystalline Multimetallic Nanoframes with Three-Dimensional Electrocatalytic Surfaces
journal, February 2014


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


Electrochemical Stability of Nanometer-Scale Pt Particles in Acidic Environments
journal, January 2010

  • Tang, Lei; Han, Byungchan; Persson, Kristin
  • Journal of the American Chemical Society, Vol. 132, Issue 2
  • DOI: 10.1021/ja9071496

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

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

Intermetallics as Novel Supports for Pt Monolayer O 2 Reduction Electrocatalysts: Potential for Significantly Improving Properties
journal, January 2010

  • Ghosh, Tanushree; Vukmirovic, Miomir B.; DiSalvo, Francis J.
  • Journal of the American Chemical Society, Vol. 132, Issue 3
  • DOI: 10.1021/ja905850c

Tuning Multimetallic Ordered Intermetallic Nanocrystals for Efficient Energy Electrocatalysis
journal, December 2016

  • Luo, Mingchuan; Sun, Yingjun; Wang, Lei
  • Advanced Energy Materials, Vol. 7, Issue 11
  • DOI: 10.1002/aenm.201602073

Strain-controlled electrocatalysis on multimetallic nanomaterials
journal, September 2017


Pt Skin on AuCu Intermetallic Substrate: A Strategy to Maximize Pt Utilization for Fuel Cells
journal, June 2014

  • Wang, Gongwei; Huang, Bing; Xiao, Li
  • Journal of the American Chemical Society, Vol. 136, Issue 27
  • DOI: 10.1021/ja503315s

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

Recent Advances of Structurally Ordered Intermetallic Nanoparticles for Electrocatalysis
journal, March 2018


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

Synthesis of Structurally Ordered Pt 3 Ti and Pt 3 V Nanoparticles as Methanol Oxidation Catalysts
journal, July 2014

  • Cui, Zhiming; Chen, Hao; Zhao, Mengtian
  • Journal of the American Chemical Society, Vol. 136, Issue 29
  • DOI: 10.1021/ja504573a

Core/Shell Face-Centered Tetragonal FePd/Pd Nanoparticles as an Efficient Non-Pt Catalyst for the Oxygen Reduction Reaction
journal, October 2015


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


Fe Stabilization by Intermetallic L1 0 -FePt and Pt Catalysis Enhancement in L1 0 -FePt/Pt Nanoparticles for Efficient Oxygen Reduction Reaction in Fuel Cells
journal, February 2018

  • Li, Junrui; Xi, Zheng; Pan, Yung-Tin
  • Journal of the American Chemical Society, Vol. 140, Issue 8
  • DOI: 10.1021/jacs.7b12829

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996


Projector augmented-wave method
journal, December 1994


From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999


The adiabatic connection method: a non-empirical hybrid
journal, January 1997


Estimations of electric field effects on the oxygen reduction reaction based on the density functional theory
journal, January 2007

  • Karlberg, G. S.; Rossmeisl, J.; Nørskov, J. K.
  • Physical Chemistry Chemical Physics, Vol. 9, Issue 37
  • DOI: 10.1039/b705938h

Origin of the Overpotential for Oxygen Reduction at a Fuel-Cell Cathode
journal, November 2004

  • Nørskov, J. K.; Rossmeisl, J.; Logadottir, A.
  • The Journal of Physical Chemistry B, Vol. 108, Issue 46
  • DOI: 10.1021/jp047349j

Morphology and Activity Tuning of Cu 3 Pt/C Ordered Intermetallic Nanoparticles by Selective Electrochemical Dealloying
journal, January 2015

  • Wang, Deli; Yu, Yingchao; Zhu, Jing
  • Nano Letters, Vol. 15, Issue 2
  • DOI: 10.1021/nl504597j

Structurally ordered Pt–Zn/C series nanoparticles as efficient anode catalysts for formic acid electrooxidation
journal, January 2015

  • Zhu, Jing; Zheng, Xin; Wang, Jie
  • Journal of Materials Chemistry A, Vol. 3, Issue 44
  • DOI: 10.1039/C5TA05699C

Hard-Magnet L10-CoPt Nanoparticles Advance Fuel Cell Catalysis
journal, January 2019


Electrocatalytic reduction of dioxygen at platinum particles dispersed in a polyaniline film
journal, December 2000


Towards active and stable oxygen reduction cathodes: a density functional theory survey on Pt2M skin alloys
journal, January 2011

  • Wei, Guang-Feng; Liu, Zhi-Pan
  • Energy & Environmental Science, Vol. 4, Issue 4
  • DOI: 10.1039/c0ee00762e

Surfactant Removal for Colloidal Nanoparticles from Solution Synthesis: The Effect on Catalytic Performance
journal, June 2012

  • Li, Dongguo; Wang, Chao; Tripkovic, Dusan
  • ACS Catalysis, Vol. 2, Issue 7
  • DOI: 10.1021/cs300219j

Local Structure, Electronic Behavior, and Electrocatalytic Reactivity of CO-Reduced Platinum–Iron Oxide Nanoparticles
journal, November 2013

  • Duchesne, Paul N.; Chen, Guangxu; Zheng, Nanfeng
  • The Journal of Physical Chemistry C, Vol. 117, Issue 49
  • DOI: 10.1021/jp4093496

Reversibility of Pt-Skin and Pt-Skeleton Nanostructures in Acidic Media
journal, January 2014

  • Durst, Julien; Lopez-Haro, Miguel; Dubau, Laetitia
  • The Journal of Physical Chemistry Letters, Vol. 5, Issue 3
  • DOI: 10.1021/jz4025707