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Title: High-performance fuel cell cathodes exclusively containing atomically dispersed iron active sites

Abstract

Platinum group metal-free (PGM-free) catalysts for the oxygen reduction reaction (ORR) with atomically dispersed FeN 4 sites have emerged as a potential replacement for low-PGM catalysts in acidic polymer electrolyte fuel cells (PEFCs).

Authors:
 [1];  [2];  [3];  [4]; ORCiD logo [4];  [5];  [2]; ORCiD logo [1]
  1. Univ. at Buffalo, NY (United States). Dept. of Chemical and Biological Engineering
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Materials Physics & Applications Division
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
  4. Technische Universität Darmstadt, Darmstadt (Germany) Dept. of Materials- and Earth Sciences, and Dept. of Chemistry
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1564158
Alternate Identifier(s):
OSTI ID: 1531027
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Energy & Environmental Science
Additional Journal Information:
Journal Volume: 12; Journal Issue: 8; Journal ID: ISSN 1754-5692
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Zhang, Hanguang, Chung, Hoon T., Cullen, David A., Wagner, Stephan, Kramm, Ulrike I., More, Karren L., Zelenay, Piotr, and Wu, Gang. High-performance fuel cell cathodes exclusively containing atomically dispersed iron active sites. United States: N. p., 2019. Web. doi:10.1039/c9ee00877b.
Zhang, Hanguang, Chung, Hoon T., Cullen, David A., Wagner, Stephan, Kramm, Ulrike I., More, Karren L., Zelenay, Piotr, & Wu, Gang. High-performance fuel cell cathodes exclusively containing atomically dispersed iron active sites. United States. doi:10.1039/c9ee00877b.
Zhang, Hanguang, Chung, Hoon T., Cullen, David A., Wagner, Stephan, Kramm, Ulrike I., More, Karren L., Zelenay, Piotr, and Wu, Gang. Mon . "High-performance fuel cell cathodes exclusively containing atomically dispersed iron active sites". United States. doi:10.1039/c9ee00877b. https://www.osti.gov/servlets/purl/1564158.
@article{osti_1564158,
title = {High-performance fuel cell cathodes exclusively containing atomically dispersed iron active sites},
author = {Zhang, Hanguang and Chung, Hoon T. and Cullen, David A. and Wagner, Stephan and Kramm, Ulrike I. and More, Karren L. and Zelenay, Piotr and Wu, Gang},
abstractNote = {Platinum group metal-free (PGM-free) catalysts for the oxygen reduction reaction (ORR) with atomically dispersed FeN 4 sites have emerged as a potential replacement for low-PGM catalysts in acidic polymer electrolyte fuel cells (PEFCs).},
doi = {10.1039/c9ee00877b},
journal = {Energy & Environmental Science},
issn = {1754-5692},
number = 8,
volume = 12,
place = {United States},
year = {2019},
month = {6}
}

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Cited by: 50 works
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Works referenced in this record:

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3D polymer hydrogel for high-performance atomic iron-rich catalysts for oxygen reduction in acidic media
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Molecular Oxygen Reduction in PEM Fuel Cells:  Evidence for the Simultaneous Presence of Two Active Sites in Fe-Based Catalysts
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Analyzing Structural Changes of Fe–N–C Cathode Catalysts in PEM Fuel Cell by Mößbauer Spectroscopy of Complete Membrane Electrode Assemblies
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Heat-treated cobalt–tripyridyl triazine (Co–TPTZ) electrocatalysts for oxygen reduction reaction in acidic medium
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Highly active atomically dispersed CoN 4 fuel cell cathode catalysts derived from surfactant-assisted MOFs: carbon-shell confinement strategy
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Single Cobalt Atoms with Precise N-Coordination as Superior Oxygen Reduction Reaction Catalysts
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    Works referencing / citing this record:

    Highly Efficient Non-Precious Metal Electrocatalysts Prepared from One-Pot Synthesized Zeolitic Imidazolate Frameworks
    journal, December 2013

    • Zhao, Dan; Shui, Jiang-Lan; Grabstanowicz, Lauren R.
    • Advanced Materials, Vol. 26, Issue 7
    • DOI: 10.1002/adma.201304238

    Nitrogen-Coordinated Single Cobalt Atom Catalysts for Oxygen Reduction in Proton Exchange Membrane Fuel Cells
    journal, January 2018

    • Wang, Xiao Xia; Cullen, David A.; Pan, Yung-Tin
    • Advanced Materials, Vol. 30, Issue 11
    • DOI: 10.1002/adma.201706758

    Iron‐Free Cathode Catalysts for Proton‐Exchange‐Membrane Fuel Cells: Cobalt Catalysts and the Peroxide Mitigation Approach
    journal, December 2018

    • Wang, Xiao Xia; Prabhakaran, Venkateshkumar; He, Yanghua
    • Advanced Materials, Vol. 31, Issue 31
    • DOI: 10.1002/adma.201805126

    Design Strategies toward Advanced MOF-Derived Electrocatalysts for Energy-Conversion Reactions
    journal, June 2017

    • Liu, Jinlong; Zhu, Dongdong; Guo, Chunxian
    • Advanced Energy Materials, Vol. 7, Issue 23
    • DOI: 10.1002/aenm.201700518

    Single Cobalt Atoms with Precise N-Coordination as Superior Oxygen Reduction Reaction Catalysts
    journal, August 2016

    • Yin, Peiqun; Yao, Tao; Wu, Yuen
    • Angewandte Chemie International Edition, Vol. 55, Issue 36
    • DOI: 10.1002/anie.201604802

    3D polymer hydrogel for high-performance atomic iron-rich catalysts for oxygen reduction in acidic media
    journal, December 2017


    Raman microspectroscopy characterization of carbon blacks: Spectral analysis and structural information
    journal, April 2015


    Fe loading of a carbon-supported Fe–N electrocatalyst and its effect on the oxygen reduction reaction
    journal, November 2009


    Heat-treated cobalt–tripyridyl triazine (Co–TPTZ) electrocatalysts for oxygen reduction reaction in acidic medium
    journal, June 2010


    Metal-Organic-Framework-Based Materials as Platforms for Renewable Energy and Environmental Applications
    journal, September 2017


    Development of high performance carbon composite catalyst for oxygen reduction reaction in PEM Proton Exchange Membrane fuel cells
    journal, August 2008

    • Nallathambi, Vijayadurga; Lee, Jong-Won; Kumaraguru, Swaminatha P.
    • Journal of Power Sources, Vol. 183, Issue 1, p. 34-42
    • DOI: 10.1016/j.jpowsour.2008.05.020

    Engineering nanostructures of PGM-free oxygen-reduction catalysts using metal-organic frameworks
    journal, January 2017


    Co/ZIF-8 Heterometallic Nanoparticles: Control of Nanocrystal Size and Properties by a Mixed-Metal Approach
    journal, September 2016

    • Zaręba, Jan K.; Nyk, Marcin; Samoć, Marek
    • Crystal Growth & Design, Vol. 16, Issue 11
    • DOI: 10.1021/acs.cgd.6b01090

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


    Role of Local Carbon Structure Surrounding FeN 4 Sites in Boosting the Catalytic Activity for Oxygen Reduction
    journal, May 2017

    • Liu, Kexi; Wu, Gang; Wang, Guofeng
    • The Journal of Physical Chemistry C, Vol. 121, Issue 21
    • DOI: 10.1021/acs.jpcc.7b00913

    Nanostructured Nonprecious Metal Catalysts for Oxygen Reduction Reaction
    journal, April 2013

    • Wu, Gang; Zelenay, Piotr
    • Accounts of Chemical Research, Vol. 46, Issue 8
    • DOI: 10.1021/ar400011z

    Structural Descriptors of Zeolitic–Imidazolate Frameworks Are Keys to the Activity of Fe–N–C Catalysts
    journal, December 2016

    • Armel, Vanessa; Hindocha, Sheena; Salles, Fabrice
    • Journal of the American Chemical Society, Vol. 139, Issue 1
    • DOI: 10.1021/jacs.6b11248

    Single Atomic Iron Catalysts for Oxygen Reduction in Acidic Media: Particle Size Control and Thermal Activation
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    • Zhang, Hanguang; Hwang, Sooyeon; Wang, Maoyu
    • Journal of the American Chemical Society, Vol. 139, Issue 40
    • DOI: 10.1021/jacs.7b06514

    Molecular Oxygen Reduction in PEM Fuel Cells:  Evidence for the Simultaneous Presence of Two Active Sites in Fe-Based Catalysts
    journal, August 2002

    • Lefèvre, M.; Dodelet, J. P.; Bertrand, P.
    • The Journal of Physical Chemistry B, Vol. 106, Issue 34, p. 8705-8713
    • DOI: 10.1021/jp020267f

    Oxygen Reduction Catalysts for Polymer Electrolyte Fuel Cells from the Pyrolysis of Iron Acetate Adsorbed on Various Carbon Supports
    journal, February 2003

    • Jaouen, Frédéric; Marcotte, Sébastien; Dodelet, Jean-Pol
    • The Journal of Physical Chemistry B, Vol. 107, Issue 6, p. 1376-1386
    • DOI: 10.1021/jp021634q

    Structure of Fe–N x –C Defects in Oxygen Reduction Reaction Catalysts from First-Principles Modeling
    journal, June 2014

    • Holby, Edward F.; Wu, Gang; Zelenay, Piotr
    • The Journal of Physical Chemistry C, Vol. 118, Issue 26
    • DOI: 10.1021/jp503266h

    Reaction Pathway for Oxygen Reduction on FeN 4 Embedded Graphene
    journal, January 2014

    • Kattel, Shyam; Wang, Guofeng
    • The Journal of Physical Chemistry Letters, Vol. 5, Issue 3
    • DOI: 10.1021/jz402717r

    Analyzing Structural Changes of Fe–N–C Cathode Catalysts in PEM Fuel Cell by Mößbauer Spectroscopy of Complete Membrane Electrode Assemblies
    journal, October 2014

    • Kramm, Ulrike I.; Lefèvre, Michel; Bogdanoff, Peter
    • The Journal of Physical Chemistry Letters, Vol. 5, Issue 21
    • DOI: 10.1021/jz501955g

    Carbonized Nanoscale Metal–Organic Frameworks as High Performance Electrocatalyst for Oxygen Reduction Reaction
    journal, November 2014

    • Zhao, Shenlong; Yin, Huajie; Du, Lei
    • ACS Nano, Vol. 8, Issue 12
    • DOI: 10.1021/nn505582e

    Iron-based cathode catalyst with enhanced power density in polymer electrolyte membrane fuel cells
    journal, August 2011

    • Proietti, Eric; Jaouen, Frédéric; Lefèvre, Michel
    • Nature Communications, Vol. 2, Issue 1
    • DOI: 10.1038/ncomms1427

    Active and stable carbon nanotube/nanoparticle composite electrocatalyst for oxygen reduction
    journal, May 2013

    • Chung, Hoon T.; Won, Jong H.; Zelenay, Piotr
    • Nature Communications, Vol. 4, Issue 1
    • DOI: 10.1038/ncomms2944

    Quantifying the density and utilization of active sites in non-precious metal oxygen electroreduction catalysts
    journal, October 2015

    • Sahraie, Nastaran Ranjbar; Kramm, Ulrike I.; Steinberg, Julian
    • Nature Communications, Vol. 6, Issue 1
    • DOI: 10.1038/ncomms9618

    Identification of catalytic sites for oxygen reduction in iron- and nitrogen-doped graphene materials
    journal, August 2015

    • Zitolo, Andrea; Goellner, Vincent; Armel, Vanessa
    • Nature Materials, Vol. 14, Issue 9
    • DOI: 10.1038/nmat4367

    Atomically dispersed manganese catalysts for oxygen reduction in proton-exchange membrane fuel cells
    journal, October 2018


    Titanium dioxide-supported non-precious metal oxygen reduction electrocatalyst
    journal, January 2010

    • Wu, Gang; Nelson, Mark A.; Mack, Nathan H.
    • Chemical Communications, Vol. 46, Issue 40, p. 7489-7491
    • DOI: 10.1039/c0cc03088k

    Structure of the catalytic sites in Fe/N/C-catalysts for O2-reduction in PEM fuel cells
    journal, January 2012

    • Kramm, Ulrike I.; Herranz, Juan; Larouche, Nicholas
    • Physical Chemistry Chemical Physics, Vol. 14, Issue 33
    • DOI: 10.1039/c2cp41957b

    A density functional theory study of oxygen reduction reaction on Me–N4 (Me = Fe, Co, or Ni) clusters between graphitic pores
    journal, January 2013

    • Kattel, Shyam; Wang, Guofeng
    • Journal of Materials Chemistry A, Vol. 1, Issue 36
    • DOI: 10.1039/c3ta12142a

    Effect of iron-carbide formation on the number of active sites in Fe–N–C catalysts for the oxygen reduction reaction in acidic media
    journal, January 2014

    • Kramm, Ulrike I.; Herrmann-Geppert, Iris; Fiechter, Sebastian
    • J. Mater. Chem. A, Vol. 2, Issue 8
    • DOI: 10.1039/c3ta13821f

    Degradation of Fe/N/C catalysts upon high polarization in acid medium
    journal, January 2014

    • Goellner, Vincent; Baldizzone, Claudio; Schuppert, Anna
    • Phys. Chem. Chem. Phys., Vol. 16, Issue 34
    • DOI: 10.1039/c4cp02882a

    The role of carbon atoms of supported iron carbides in Fischer–Tropsch synthesis
    journal, January 2015

    • Ordomsky, V. V.; Legras, B.; Cheng, K.
    • Catalysis Science & Technology, Vol. 5, Issue 3
    • DOI: 10.1039/c4cy01631a

    MOF derived catalysts for electrochemical oxygen reduction
    journal, January 2014

    • Wang, Xiaojuan; Zhou, Junwen; Fu, He
    • J. Mater. Chem. A, Vol. 2, Issue 34
    • DOI: 10.1039/c4ta01506a

    Well-defined carbon polyhedrons prepared from nano metal–organic frameworks for oxygen reduction
    journal, January 2014

    • Xia, Wei; Zhu, Jinghan; Guo, Wenhan
    • J. Mater. Chem. A, Vol. 2, Issue 30
    • DOI: 10.1039/c4ta01656d

    Size-controlled large-diameter and few-walled carbon nanotube catalysts for oxygen reduction
    journal, January 2015

    • Wang, Xianliang; Li, Qing; Pan, Hengyu
    • Nanoscale, Vol. 7, Issue 47
    • DOI: 10.1039/c5nr05864c

    Advancements in rationally designed PGM-free fuel cell catalysts derived from metal–organic frameworks
    journal, January 2017

    • Barkholtz, Heather M.; Liu, Di-Jia
    • Materials Horizons, Vol. 4, Issue 1
    • DOI: 10.1039/c6mh00344c

    An Fe–N–C hybrid electrocatalyst derived from a bimetal–organic framework for efficient oxygen reduction
    journal, January 2016

    • Liu, Teng; Zhao, Pingping; Hua, Xing
    • Journal of Materials Chemistry A, Vol. 4, Issue 29
    • DOI: 10.1039/c6ta03265f

    Highly active atomically dispersed CoN 4 fuel cell cathode catalysts derived from surfactant-assisted MOFs: carbon-shell confinement strategy
    journal, January 2019

    • He, Yanghua; Hwang, Sooyeon; Cullen, David A.
    • Energy & Environmental Science, Vol. 12, Issue 1
    • DOI: 10.1039/c8ee02694g

    High-Performance Electrocatalysts for Oxygen Reduction Derived from Polyaniline, Iron, and Cobalt
    journal, April 2011


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


    Direct atomic-level insight into the active sites of a high-performance PGM-free ORR catalyst
    journal, August 2017


    Influence of the Electron-Density of FeN[sub 4]-Centers Towards the Catalytic Activity of Pyrolyzed FeTMPPCl-Based ORR-Electrocatalysts
    journal, January 2011

    • Kramm, U. I.; Abs-Wurmbach, I.; Herrmann-Geppert, I.
    • Journal of The Electrochemical Society, Vol. 158, Issue 1
    • DOI: 10.1149/1.3499621

    Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion
    journal, November 2019

    • Zhu, Yuanzhi; Sokolowski, Joshua; Song, Xiancheng
    • Advanced Energy Materials, Vol. 10, Issue 11
    • DOI: 10.1002/aenm.201902844

    Thermally Driven Structure and Performance Evolution of Atomically Dispersed FeN 4 Sites for Oxygen Reduction
    journal, November 2019

    • Li, Jiazhan; Zhang, Hanguang; Samarakoon, Widitha
    • Angewandte Chemie, Vol. 131, Issue 52
    • DOI: 10.1002/ange.201909312

    On the Influence of Oxygen on the Degradation of Fe‐N‐C Catalysts
    journal, January 2020

    • Kumar, Kavita; Dubau, Laetitia; Mermoux, Michel
    • Angewandte Chemie, Vol. 132, Issue 8
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    Thermally Driven Structure and Performance Evolution of Atomically Dispersed FeN 4 Sites for Oxygen Reduction
    journal, November 2019

    • Li, Jiazhan; Zhang, Hanguang; Samarakoon, Widitha
    • Angewandte Chemie International Edition, Vol. 58, Issue 52
    • DOI: 10.1002/anie.201909312

    On the Influence of Oxygen on the Degradation of Fe‐N‐C Catalysts
    journal, February 2020

    • Kumar, Kavita; Dubau, Laetitia; Mermoux, Michel
    • Angewandte Chemie International Edition, Vol. 59, Issue 8
    • DOI: 10.1002/anie.201912451

    Atomically Dispersed Single Ni Site Catalysts for Nitrogen Reduction toward Electrochemical Ammonia Synthesis Using N 2 and H 2 O
    journal, February 2020


    Recent progress in pyrolyzed carbon materials as electrocatalysts for the oxygen reduction reaction
    journal, January 2020

    • Ouyang, Chen; Wang, Xun
    • Inorganic Chemistry Frontiers, Vol. 7, Issue 1
    • DOI: 10.1039/c9qi00962k

    Controllable synthesis of CoN 3 catalysts derived from Co/Zn-ZIF-67 for electrocatalytic oxygen reduction in acidic electrolytes
    journal, January 2019

    • Lai, Shoujuan; Xu, Li; Liu, Hongli
    • Journal of Materials Chemistry A, Vol. 7, Issue 38
    • DOI: 10.1039/c9ta08134h

    Atomic-level active sites of efficient imidazolate framework-derived nickel catalysts for CO 2 reduction
    journal, January 2019

    • Pan, Fuping; Zhang, Hanguang; Liu, Zhenyu
    • Journal of Materials Chemistry A, Vol. 7, Issue 46
    • DOI: 10.1039/c9ta08862h

    Nanoporous bimetallic Zn/Fe–N–C for efficient oxygen reduction in acidic and alkaline media
    journal, January 2020

    • Xue, Jinling; Li, Yinshi; Hu, Jue
    • Journal of Materials Chemistry A, Vol. 8, Issue 15
    • DOI: 10.1039/c9ta13471a