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

Zhang, Hanguang; Chung, Hoon T.; Cullen, David A.; Wagner, Stephan; Kramm, Ulrike I.; More, Karren L.; Zelenay, Piotr; Wu, Gang

doi:10.1039/c9ee00877b

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

Journal Article · 24 June 2019 · Energy & Environmental Science

DOI: https://doi.org/10.1039/c9ee00877b · OSTI ID:1564158

Zhang, Hanguang ^[1]; Chung, Hoon T. ^[2]; Cullen, David A. ^[3]; Wagner, Stephan ^[4];

^[4]; More, Karren L. ^[5]; Zelenay, Piotr ^[2];

^[1]

Univ. at Buffalo, NY (United States). Dept. of Chemical and Biological Engineering
Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Materials Physics & Applications Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
Technische Universität Darmstadt, Darmstadt (Germany) Dept. of Materials- and Earth Sciences, and Dept. of Chemistry
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences

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).

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Univ. at Buffalo, NY (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Fuel Cell Technologies Office

Grant/Contract Number:: AC05-00OR22725; EE0008076

OSTI ID:: 1564158

Alternate ID(s):: OSTI ID: 1531027; OSTI ID: 1897115

Journal Information:: Energy & Environmental Science, Vol. 12, Issue 8; ISSN 1754-5692

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 389 works

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References (53)

Carbonized Nanoscale Metal–Organic Frameworks as High Performance Electrocatalyst for Oxygen Reduction Reaction Zhao, Shenlong; Yin, Huajie; Du, Lei ACS Nano, Vol. 8, Issue 12 https://doi.org/10.1021/nn505582e	journal	November 2014
A density functional theory study of oxygen reduction reaction on Me–N4 (Me = Fe, Co, or Ni) clusters between graphitic pores Kattel, Shyam; Wang, Guofeng Journal of Materials Chemistry A, Vol. 1, Issue 36 https://doi.org/10.1039/c3ta12142a	journal	January 2013
Size-controlled large-diameter and few-walled carbon nanotube catalysts for oxygen reduction Wang, Xianliang; Li, Qing; Pan, Hengyu Nanoscale, Vol. 7, Issue 47 https://doi.org/10.1039/C5NR05864C	journal	January 2015
Structure of Fe–N _x –C Defects in Oxygen Reduction Reaction Catalysts from First-Principles Modeling Holby, Edward F.; Wu, Gang; Zelenay, Piotr The Journal of Physical Chemistry C, Vol. 118, Issue 26 https://doi.org/10.1021/jp503266h	journal	June 2014
Degradation of Fe/N/C catalysts upon high polarization in acid medium Goellner, Vincent; Baldizzone, Claudio; Schuppert, Anna Phys. Chem. Chem. Phys., Vol. 16, Issue 34 https://doi.org/10.1039/C4CP02882A	journal	January 2014
MOF derived catalysts for electrochemical oxygen reduction Wang, Xiaojuan; Zhou, Junwen; Fu, He J. Mater. Chem. A, Vol. 2, Issue 34 https://doi.org/10.1039/C4TA01506A	journal	January 2014
Metal-Organic-Framework-Based Materials as Platforms for Renewable Energy and Environmental Applications Zhang, Huabin; Nai, Jianwei; Yu, Le Joule, Vol. 1, Issue 1 https://doi.org/10.1016/j.joule.2017.08.008	journal	September 2017
Effect of iron-carbide formation on the number of active sites in Fe–N–C catalysts for the oxygen reduction reaction in acidic media Kramm, Ulrike I.; Herrmann-Geppert, Iris; Fiechter, Sebastian J. Mater. Chem. A, Vol. 2, Issue 8 https://doi.org/10.1039/C3TA13821F	journal	January 2014
Highly Crystalline Multimetallic Nanoframes with Three-Dimensional Electrocatalytic Surfaces Chen, C.; Kang, Y.; Huo, Z. Science, Vol. 343, Issue 6177 https://doi.org/10.1126/science.1249061	journal	February 2014
Carbon nanocomposite catalysts for oxygen reduction and evolution reactions: From nitrogen doping to transition-metal addition Wu, Gang; Santandreu, Ana; Kellogg, William Nano Energy, Vol. 29 https://doi.org/10.1016/j.nanoen.2015.12.032	journal	November 2016
Active and stable carbon nanotube/nanoparticle composite electrocatalyst for oxygen reduction Chung, Hoon T.; Won, Jong H.; Zelenay, Piotr Nature Communications, Vol. 4, Issue 1 https://doi.org/10.1038/ncomms2944	journal	May 2013
Raman microspectroscopy characterization of carbon blacks: Spectral analysis and structural information Pawlyta, Miroslawa; Rouzaud, Jean-Noël; Duber, Stanislaw Carbon, Vol. 84 https://doi.org/10.1016/j.carbon.2014.12.030	journal	April 2015
Structural Descriptors of Zeolitic–Imidazolate Frameworks Are Keys to the Activity of Fe–N–C Catalysts Armel, Vanessa; Hindocha, Sheena; Salles, Fabrice Journal of the American Chemical Society, Vol. 139, Issue 1 https://doi.org/10.1021/jacs.6b11248	journal	December 2016
Highly Efficient Non-Precious Metal Electrocatalysts Prepared from One-Pot Synthesized Zeolitic Imidazolate Frameworks Zhao, Dan; Shui, Jiang-Lan; Grabstanowicz, Lauren R. Advanced Materials, Vol. 26, Issue 7 https://doi.org/10.1002/adma.201304238	journal	December 2013
Fe loading of a carbon-supported Fe–N electrocatalyst and its effect on the oxygen reduction reaction Zhang, Lei; Lee, Kunchan; Bezerra, Cicero W. B. Electrochimica Acta, Vol. 54, Issue 26 https://doi.org/10.1016/j.electacta.2009.06.049	journal	November 2009
Structure of the catalytic sites in Fe/N/C-catalysts for O2-reduction in PEM fuel cells Kramm, Ulrike I.; Herranz, Juan; Larouche, Nicholas Physical Chemistry Chemical Physics, Vol. 14, Issue 33 https://doi.org/10.1039/c2cp41957b	journal	January 2012
High-Performance Electrocatalysts for Oxygen Reduction Derived from Polyaniline, Iron, and Cobalt Wu, G.; More, K. L.; Johnston, C. M. Science, Vol. 332, Issue 6028, p. 443-447 https://doi.org/10.1126/science.1200832	journal	April 2011
Atomically dispersed manganese catalysts for oxygen reduction in proton-exchange membrane fuel cells Li, Jiazhan; Chen, Mengjie; Cullen, David A. Nature Catalysis, Vol. 1, Issue 12 https://doi.org/10.1038/s41929-018-0164-8	journal	October 2018
⁵⁷ Fe Mössbauer Spectroscopy Characterization of Electrocatalysts Kramm, Ulrike I.; Ni, Lingmei; Wagner, Stephan Advanced Materials, Vol. 31, Issue 31 https://doi.org/10.1002/adma.201805623	journal	December 2018
Advancements in rationally designed PGM-free fuel cell catalysts derived from metal–organic frameworks Barkholtz, Heather M.; Liu, Di-Jia Materials Horizons, Vol. 4, Issue 1 https://doi.org/10.1039/C6MH00344C	journal	January 2017
Oxygen Reduction Catalysts for Polymer Electrolyte Fuel Cells from the Pyrolysis of Iron Acetate Adsorbed on Various Carbon Supports Jaouen, Frédéric; Marcotte, Sébastien; Dodelet, Jean-Pol The Journal of Physical Chemistry B, Vol. 107, Issue 6, p. 1376-1386 https://doi.org/10.1021/jp021634q	journal	February 2003
3D polymer hydrogel for high-performance atomic iron-rich catalysts for oxygen reduction in acidic media Qiao, Zhi; Zhang, Hanguang; Karakalos, Stavros Applied Catalysis B: Environmental, Vol. 219 https://doi.org/10.1016/j.apcatb.2017.08.008	journal	December 2017
Molecular Oxygen Reduction in PEM Fuel Cells: Evidence for the Simultaneous Presence of Two Active Sites in Fe-Based Catalysts Lefèvre, M.; Dodelet, J. P.; Bertrand, P. The Journal of Physical Chemistry B, Vol. 106, Issue 34, p. 8705-8713 https://doi.org/10.1021/jp020267f	journal	August 2002
Recent Advances in Electrocatalysts for Oxygen Reduction Reaction Shao, Minhua; Chang, Qiaowan; Dodelet, Jean-Pol Chemical Reviews, Vol. 116, Issue 6 https://doi.org/10.1021/acs.chemrev.5b00462	journal	February 2016
Analyzing Structural Changes of Fe–N–C Cathode Catalysts in PEM Fuel Cell by Mößbauer Spectroscopy of Complete Membrane Electrode Assemblies Kramm, Ulrike I.; Lefèvre, Michel; Bogdanoff, Peter The Journal of Physical Chemistry Letters, Vol. 5, Issue 21 https://doi.org/10.1021/jz501955g	journal	October 2014
Identification of catalytic sites for oxygen reduction in iron- and nitrogen-doped graphene materials Zitolo, Andrea; Goellner, Vincent; Armel, Vanessa Nature Materials, Vol. 14, Issue 9 https://doi.org/10.1038/nmat4367	journal	August 2015
Co/ZIF-8 Heterometallic Nanoparticles: Control of Nanocrystal Size and Properties by a Mixed-Metal Approach Zaręba, Jan K.; Nyk, Marcin; Samoć, Marek Crystal Growth & Design, Vol. 16, Issue 11 https://doi.org/10.1021/acs.cgd.6b01090	journal	September 2016
Single Atomic Iron Catalysts for Oxygen Reduction in Acidic Media: Particle Size Control and Thermal Activation Zhang, Hanguang; Hwang, Sooyeon; Wang, Maoyu Journal of the American Chemical Society, Vol. 139, Issue 40 https://doi.org/10.1021/jacs.7b06514	journal	September 2017
Role of Local Carbon Structure Surrounding FeN ₄ Sites in Boosting the Catalytic Activity for Oxygen Reduction Liu, Kexi; Wu, Gang; Wang, Guofeng The Journal of Physical Chemistry C, Vol. 121, Issue 21 https://doi.org/10.1021/acs.jpcc.7b00913	journal	May 2017
Heat-treated cobalt–tripyridyl triazine (Co–TPTZ) electrocatalysts for oxygen reduction reaction in acidic medium Li, Shang; Zhang, Lei; Liu, Hansan Electrochimica Acta, Vol. 55, Issue 15 https://doi.org/10.1016/j.electacta.2010.01.090	journal	June 2010
Nitrogen-doped carbon nanotubes derived from Zn–Fe-ZIF nanospheres and their application as efficient oxygen reduction electrocatalysts with in situ generated iron species Su, Panpan; Xiao, Hui; Zhao, Jiao Chemical Science, Vol. 4, Issue 7 https://doi.org/10.1039/c3sc51052b	journal	January 2013
Bimetal–Organic Framework Self-Adjusted Synthesis of Support-Free Nonprecious Electrocatalysts for Efficient Oxygen Reduction You, Bo; Jiang, Nan; Sheng, Meili ACS Catalysis, Vol. 5, Issue 12 https://doi.org/10.1021/acscatal.5b02325	journal	October 2015
Highly active atomically dispersed CoN ₄ fuel cell cathode catalysts derived from surfactant-assisted MOFs: carbon-shell confinement strategy He, Yanghua; Hwang, Sooyeon; Cullen, David A. Energy & Environmental Science, Vol. 12, Issue 1 https://doi.org/10.1039/C8EE02694G	journal	January 2019
Reaction Pathway for Oxygen Reduction on FeN ₄ Embedded Graphene Kattel, Shyam; Wang, Guofeng The Journal of Physical Chemistry Letters, Vol. 5, Issue 3 https://doi.org/10.1021/jz402717r	journal	January 2014
Nanostructured Nonprecious Metal Catalysts for Oxygen Reduction Reaction Wu, Gang; Zelenay, Piotr Accounts of Chemical Research, Vol. 46, Issue 8 https://doi.org/10.1021/ar400011z	journal	April 2013
The role of carbon atoms of supported iron carbides in Fischer–Tropsch synthesis Ordomsky, V. V.; Legras, B.; Cheng, K. Catalysis Science & Technology, Vol. 5, Issue 3 https://doi.org/10.1039/C4CY01631A	journal	January 2015
Titanium dioxide-supported non-precious metal oxygen reduction electrocatalyst Wu, Gang; Nelson, Mark A.; Mack, Nathan H. Chemical Communications, Vol. 46, Issue 40, p. 7489-7491 https://doi.org/10.1039/c0cc03088k	journal	January 2010
Well-defined carbon polyhedrons prepared from nano metal–organic frameworks for oxygen reduction Xia, Wei; Zhu, Jinghan; Guo, Wenhan J. Mater. Chem. A, Vol. 2, Issue 30 https://doi.org/10.1039/C4TA01656D	journal	January 2014
An Fe–N–C hybrid electrocatalyst derived from a bimetal–organic framework for efficient oxygen reduction Liu, Teng; Zhao, Pingping; Hua, Xing Journal of Materials Chemistry A, Vol. 4, Issue 29 https://doi.org/10.1039/C6TA03265F	journal	January 2016
Quantifying the density and utilization of active sites in non-precious metal oxygen electroreduction catalysts Sahraie, Nastaran Ranjbar; Kramm, Ulrike I.; Steinberg, Julian Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms9618	journal	October 2015
Iron-based cathode catalyst with enhanced power density in polymer electrolyte membrane fuel cells Proietti, Eric; Jaouen, Frédéric; Lefèvre, Michel Nature Communications, Vol. 2, Issue 1 https://doi.org/10.1038/ncomms1427	journal	August 2011
Nitrogen-Coordinated Single Cobalt Atom Catalysts for Oxygen Reduction in Proton Exchange Membrane Fuel Cells Wang, Xiao Xia; Cullen, David A.; Pan, Yung-Tin Advanced Materials, Vol. 30, Issue 11 https://doi.org/10.1002/adma.201706758	journal	January 2018
Design Strategies toward Advanced MOF-Derived Electrocatalysts for Energy-Conversion Reactions Liu, Jinlong; Zhu, Dongdong; Guo, Chunxian Advanced Energy Materials, Vol. 7, Issue 23 https://doi.org/10.1002/aenm.201700518	journal	June 2017
Direct atomic-level insight into the active sites of a high-performance PGM-free ORR catalyst Chung, Hoon T.; Cullen, David A.; Higgins, Drew Science, Vol. 357, Issue 6350 https://doi.org/10.1126/science.aan2255	journal	August 2017
Single Cobalt Atoms with Precise N-Coordination as Superior Oxygen Reduction Reaction Catalysts Yin, Peiqun; Yao, Tao; Wu, Yuen Angewandte Chemie International Edition, Vol. 55, Issue 36 https://doi.org/10.1002/anie.201604802	journal	August 2016
Development of high performance carbon composite catalyst for oxygen reduction reaction in PEM Proton Exchange Membrane fuel cells Nallathambi, Vijayadurga; Lee, Jong-Won; Kumaraguru, Swaminatha P. Journal of Power Sources, Vol. 183, Issue 1, p. 34-42 https://doi.org/10.1016/j.jpowsour.2008.05.020	journal	August 2008
Engineering nanostructures of PGM-free oxygen-reduction catalysts using metal-organic frameworks Zhang, Hanguang; Osgood, Hannah; Xie, Xiaohong Nano Energy, Vol. 31 https://doi.org/10.1016/j.nanoen.2016.11.033	journal	January 2017
Directly converting Fe-doped metal–organic frameworks into highly active and stable Fe-N-C catalysts for oxygen reduction in acid Wang, Xiaojuan; Zhang, Hanguang; Lin, Honghong Nano Energy, Vol. 25 https://doi.org/10.1016/j.nanoen.2016.04.042	journal	July 2016
Influence of the Electron-Density of FeN[sub 4]-Centers Towards the Catalytic Activity of Pyrolyzed FeTMPPCl-Based ORR-Electrocatalysts Kramm, U. I.; Abs-Wurmbach, I.; Herrmann-Geppert, I. Journal of The Electrochemical Society, Vol. 158, Issue 1 https://doi.org/10.1149/1.3499621	journal	January 2011
Well-Dispersed ZIF-Derived Co,N-Co-doped Carbon Nanoframes through Mesoporous-Silica-Protected Calcination as Efficient Oxygen Reduction Electrocatalysts Shang, Lu; Yu, Huijun; Huang, Xing Advanced Materials, Vol. 28, Issue 8 https://doi.org/10.1002/adma.201505045	journal	December 2015
Iron‐Free Cathode Catalysts for Proton‐Exchange‐Membrane Fuel Cells: Cobalt Catalysts and the Peroxide Mitigation Approach Wang, Xiao Xia; Prabhakaran, Venkateshkumar; He, Yanghua Advanced Materials, Vol. 31, Issue 31 https://doi.org/10.1002/adma.201805126	journal	December 2018
Single Cobalt Atoms with Precise N-Coordination as Superior Oxygen Reduction Reaction Catalysts Yin, Peiqun; Yao, Tao; Wu, Yuen Angewandte Chemie, Vol. 128, Issue 36 https://doi.org/10.1002/ange.201604802	journal	August 2016
Structure of the catalytic sites in Fe/N/C-catalysts for O-2-reduction in PEM fuel cells Kramm, Ulrike I.; Herranz, Juan; Larouche, Nicholas Technische Universität Berlin https://doi.org/10.14279/depositonce-5307	text	January 2012

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