Enhancement of oxygen reduction reaction activities by Pt nanoclusters decorated on ordered mesoporous porphyrinic carbons
Abstract
The high cost of Pt-based membrane electrode assemblies (MEAs) is a critical hurdle for the commercialization of polymer electrolyte fuel cells (PEFCs). Recently, non-precious metal-based catalysts (NPMCs) have demonstrated much enhanced activity but their oxygen reduction reaction (ORR) activity is still inferior to that of Pt-based catalysts resulting in a much thicker electrode in the MEA. For the reduction of mass transport and ohmic overpotential we adopted a new concept of catalyst that combines an ultra-low amount of Pt nanoclusters with metal–nitrogen (M–Nx) doped ordered mesoporous porphyrinic carbon (FeCo–OMPC(L)). The 5 wt% Pt/FeCo–OMPC(L) showed a 2-fold enhancement in activities compared to a higher loading of Pt. Our experimental results supported by first-principles calculations indicate that a trace amount of Pt nanoclusters on FeCo–OMPC(L) significantly enhances the ORR activity due to their electronic effect as well as geometric effect from the reduced active sites. Finally, in terms of fuel cell commercialization, this class of catalysts is a promising candidate due to the limited use of Pt in the MEA.
- Authors:
-
- SABIC Technology Center, Riyadh (Saudi Arabia)
- Pohang Accelerator Lab. (PAL) (Korea, Republic of)
- Korea Inst. of Energy Research (KIER), Daejeon (South Korea). Fuel Cell Lab.
- Ulsan National Inst. of Science and Technology (UNIST), Ulsan (South Korea). Dept. of Chemistry
- Ulsan National Inst. of Science and Technology (UNIST), Ulsan (South Korea). Dept. of Chemistry; Ulsan National Inst. of Science and Technology (UNIST), Ulsan (South Korea). School of Engineering
- Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Chemistry
- 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:
- 1302999
- Report Number(s):
- BNL-112405-2016-JA
Journal ID: ISSN 2050-7488; R&D Project: MA510MAEA; KC0302010
- Grant/Contract Number:
- SC00112704; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Materials Chemistry. A
- Additional Journal Information:
- Journal Volume: 4; Journal Issue: 16; Journal ID: ISSN 2050-7488
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE
Citation Formats
Sun-Mi Hwang, Choi, YongMan, Kim, Min Gyu, Sohn, Young-Jun, Cheon, Jae Yeong, Joo, Sang Hoon, Yim, Sung-Dae, Kuttiyiel, Kurian A., Sasaki, Kotaro, Adzic, Radoslav R., and Park, Gu-Gon. Enhancement of oxygen reduction reaction activities by Pt nanoclusters decorated on ordered mesoporous porphyrinic carbons. United States: N. p., 2016.
Web. doi:10.1039/c5ta09915c.
Sun-Mi Hwang, Choi, YongMan, Kim, Min Gyu, Sohn, Young-Jun, Cheon, Jae Yeong, Joo, Sang Hoon, Yim, Sung-Dae, Kuttiyiel, Kurian A., Sasaki, Kotaro, Adzic, Radoslav R., & Park, Gu-Gon. Enhancement of oxygen reduction reaction activities by Pt nanoclusters decorated on ordered mesoporous porphyrinic carbons. United States. https://doi.org/10.1039/c5ta09915c
Sun-Mi Hwang, Choi, YongMan, Kim, Min Gyu, Sohn, Young-Jun, Cheon, Jae Yeong, Joo, Sang Hoon, Yim, Sung-Dae, Kuttiyiel, Kurian A., Sasaki, Kotaro, Adzic, Radoslav R., and Park, Gu-Gon. Tue .
"Enhancement of oxygen reduction reaction activities by Pt nanoclusters decorated on ordered mesoporous porphyrinic carbons". United States. https://doi.org/10.1039/c5ta09915c. https://www.osti.gov/servlets/purl/1302999.
@article{osti_1302999,
title = {Enhancement of oxygen reduction reaction activities by Pt nanoclusters decorated on ordered mesoporous porphyrinic carbons},
author = {Sun-Mi Hwang and Choi, YongMan and Kim, Min Gyu and Sohn, Young-Jun and Cheon, Jae Yeong and Joo, Sang Hoon and Yim, Sung-Dae and Kuttiyiel, Kurian A. and Sasaki, Kotaro and Adzic, Radoslav R. and Park, Gu-Gon},
abstractNote = {The high cost of Pt-based membrane electrode assemblies (MEAs) is a critical hurdle for the commercialization of polymer electrolyte fuel cells (PEFCs). Recently, non-precious metal-based catalysts (NPMCs) have demonstrated much enhanced activity but their oxygen reduction reaction (ORR) activity is still inferior to that of Pt-based catalysts resulting in a much thicker electrode in the MEA. For the reduction of mass transport and ohmic overpotential we adopted a new concept of catalyst that combines an ultra-low amount of Pt nanoclusters with metal–nitrogen (M–Nx) doped ordered mesoporous porphyrinic carbon (FeCo–OMPC(L)). The 5 wt% Pt/FeCo–OMPC(L) showed a 2-fold enhancement in activities compared to a higher loading of Pt. Our experimental results supported by first-principles calculations indicate that a trace amount of Pt nanoclusters on FeCo–OMPC(L) significantly enhances the ORR activity due to their electronic effect as well as geometric effect from the reduced active sites. Finally, in terms of fuel cell commercialization, this class of catalysts is a promising candidate due to the limited use of Pt in the MEA.},
doi = {10.1039/c5ta09915c},
journal = {Journal of Materials Chemistry. A},
number = 16,
volume = 4,
place = {United States},
year = {Tue Mar 08 00:00:00 EST 2016},
month = {Tue Mar 08 00:00:00 EST 2016}
}
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Works referenced in this record:
Electrocatalyst approaches and challenges for automotive fuel cells
journal, June 2012
- Debe, Mark K.
- Nature, Vol. 486, Issue 7401
Activity benchmarks and requirements for Pt, Pt-alloy, and non-Pt oxygen reduction catalysts for PEMFCs
journal, March 2005
- Gasteiger, Hubert A.; Kocha, Shyam S.; Sompalli, Bhaskar
- Applied Catalysis B: Environmental, Vol. 56, Issue 1-2, p. 9-35
Just a Dream—or Future Reality?
journal, April 2009
- Gasteiger, Hubert A.; Marković, Nenad M
- Science, Vol. 324, Issue 5923, p. 48-49
Low-platinum and platinum-free catalysts for the oxygen reduction reaction at fuel cell cathodes
journal, January 2011
- Morozan, Adina; Jousselme, Bruno; Palacin, Serge
- Energy & Environmental Science, Vol. 4, Issue 4
Low and non-platinum electrocatalysts for PEMFCs: Current status, challenges and prospects
journal, October 2012
- Brouzgou, A.; Song, S. Q.; Tsiakaras, P.
- Applied Catalysis B: Environmental, Vol. 127
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
Trends in electrocatalysis on extended and nanoscale Pt-bimetallic alloy surfaces
journal, February 2007
- Stamenkovic, Vojislav R.; Mun, Bongjin Simon; Arenz, Matthias
- Nature Materials, Vol. 6, Issue 3, p. 241-247
A New Fuel Cell Cathode Catalyst
journal, March 1964
- Jasinski, Raymond
- Nature, Vol. 201, Issue 4925, p. 1212-1213
A class of non-precious metal composite catalysts for fuel cells
journal, September 2006
- Bashyam, Rajesh; Zelenay, Piotr
- Nature, Vol. 443, Issue 7107
A review on non-precious metal electrocatalysts for PEM fuel cells
journal, January 2011
- Chen, Zhongwei; Higgins, Drew; Yu, Aiping
- Energy & Environmental Science, Vol. 4, Issue 9
Recent advances in non-precious metal catalysis for oxygen-reduction reaction in polymer electrolyte fuelcells
journal, January 2011
- Jaouen, Frédéric; Proietti, Eric; Lefèvre, Michel
- Energy Environ. Sci., Vol. 4, Issue 1, p. 114-130
A review of the development of nitrogen-modified carbon-based catalysts for oxygen reduction at USC
journal, January 2011
- Liu, Gang; Li, Xuguang; Lee, Jong-Won
- Catalysis Science & Technology, Vol. 1, Issue 2
Recent progress on nitrogen/carbon structures designed for use in energy and sustainability applications
journal, January 2014
- Wood, Kevin N.; O'Hayre, Ryan; Pylypenko, Svitlana
- Energy Environ. Sci., Vol. 7, Issue 4
Review on Recent Progress in Nitrogen-Doped Graphene: Synthesis, Characterization, and Its Potential Applications
journal, April 2012
- Wang, Haibo; Maiyalagan, Thandavarayan; Wang, Xin
- ACS Catalysis, Vol. 2, Issue 5
A review of Fe–N/C and Co–N/C catalysts for the oxygen reduction reaction
journal, June 2008
- Bezerra, Cicero W.B.; Zhang, Lei; Lee, Kunchan
- Electrochimica Acta, Vol. 53, Issue 15, p. 4937-4951
Non precious metal catalysts for the PEM fuel cell cathode
journal, January 2012
- Othman, Rapidah; Dicks, Andrew L.; Zhu, Zhonghua
- International Journal of Hydrogen Energy, Vol. 37, Issue 1
Iron-Based Catalysts with Improved Oxygen Reduction Activity in Polymer Electrolyte Fuel Cells
journal, April 2009
- Lefèvre, Michel; Proietti, Eric; Jaouen, Frédéric
- Science, Vol. 324, Issue 5923, p. 71-74
Synthesis of nitrogen-doped onion-like carbon and its use in carbon-based CoFe binary non-precious-metal catalysts for oxygen-reduction
journal, October 2011
- Wu, Gang; Nelson, Mark; Ma, Shuguo
- Carbon, Vol. 49, Issue 12
High-Performance Electrocatalysts for Oxygen Reduction Derived from Polyaniline, Iron, and Cobalt
journal, April 2011
- Wu, G.; More, K. L.; Johnston, C. M.
- Science, Vol. 332, Issue 6028, p. 443-447
Synthesis–structure–performance correlation for polyaniline–Me–C non-precious metal cathode catalysts for oxygen reduction in fuel cells
journal, January 2011
- Wu, Gang; Johnston, Christina M.; Mack, Nathan H.
- Journal of Materials Chemistry, Vol. 21, Issue 30
Fe/N/C non-precious catalysts for PEM fuel cells: Influence of the structural parameters of pristine commercial carbon blacks on their activity for oxygen reduction
journal, February 2008
- Charreteur, Fanny; Jaouen, Frédéric; Ruggeri, Stéphane
- Electrochimica Acta, Vol. 53, Issue 6
Oxygen reduction by Fe-based catalysts in PEM fuel cell conditions: Activity and selectivity of the catalysts obtained with two Fe precursors and various carbon supports
journal, April 2006
- Médard, C.; Lefèvre, M.; Dodelet, J. P.
- Electrochimica Acta, Vol. 51, Issue 16, p. 3202-3213
Heat-Treated Fe/N/C Catalysts for O2 Electroreduction: Are Active Sites Hosted in Micropores?
journal, March 2006
- Jaouen, Frédéric; Lefèvre, Michel; Dodelet, Jean-Pol
- The Journal of Physical Chemistry B, Vol. 110, Issue 11, p. 5553-5558
Impact of Loading in RRDE Experiments on Fe–N–C Catalysts: Two- or Four-Electron Oxygen Reduction?
journal, January 2008
- Bonakdarpour, Arman; Lefevre, Michel; Yang, Ruizhi
- Electrochemical and Solid-State Letters, Vol. 11, Issue 6, p. B105-B108
Cross-Laboratory Experimental Study of Non-Noble-Metal Electrocatalysts for the Oxygen Reduction Reaction
journal, July 2009
- Jaouen, Frédéric; Herranz, Juan; Lefèvre, Michel
- ACS Applied Materials & Interfaces, Vol. 1, Issue 8, p. 1623-1639
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
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
Activity and stability in proton exchange membrane fuel cells of iron-based cathode catalysts synthesized with addition of carbon fibers
journal, January 2014
- Larouche, Nicholas; Chenitz, Régis; Lefèvre, Michel
- Electrochimica Acta, Vol. 115
Activity, Performance, and Durability for the Reduction of Oxygen in PEM Fuel Cells, of Fe/N/C Electrocatalysts Obtained from the Pyrolysis of Metal-Organic-Framework and Iron Porphyrin Precursors
journal, March 2015
- Yang, Lijun; Larouche, Nicholas; Chenitz, Régis
- Electrochimica Acta, Vol. 159
Self-Supporting Oxygen Reduction Electrocatalysts Made from a Nitrogen-Rich Network Polymer
journal, November 2012
- Zhao, Yong; Watanabe, Kazuya; Hashimoto, Kazuhito
- Journal of the American Chemical Society, Vol. 134, Issue 48
Direct Spectroscopic Observation of the Structural Origin of Peroxide Generation from Co-Based Pyrolyzed Porphyrins for ORR Applications
journal, May 2008
- Ziegelbauer, Joseph M.; Olson, Tim S.; Pylypenko, Svitlana
- The Journal of Physical Chemistry C, Vol. 112, Issue 24
Unveiling N-Protonation and Anion-Binding Effects on Fe/N/C Catalysts for O 2 Reduction in Proton-Exchange-Membrane Fuel Cells
journal, July 2011
- Herranz, Juan; Jaouen, Frédéric; Lefèvre, Michel
- The Journal of Physical Chemistry C, Vol. 115, Issue 32
Fundamental Mechanistic Understanding of Electrocatalysis of Oxygen Reduction on Pt and Non-Pt Surfaces: Acid versus Alkaline Media
journal, March 2012
- Ramaswamy, Nagappan; Mukerjee, Sanjeev
- Advances in Physical Chemistry, Vol. 2012
Activity and stability of non-precious metal catalysts for oxygen reduction in acid and alkaline electrolytes
journal, October 2010
- Li, Xuguang; Liu, Gang; Popov, Branko N.
- Journal of Power Sources, Vol. 195, Issue 19
Non-precious metal catalysts synthesized from precursors of carbon, nitrogen, and transition metal for oxygen reduction in alkaline fuel cells
journal, February 2011
- Li, Xuguang; Popov, Branko N.; Kawahara, Takeo
- Journal of Power Sources, Vol. 196, Issue 4
Elucidating Oxygen Reduction Active Sites in Pyrolyzed Metal–Nitrogen Coordinated Non-Precious-Metal Electrocatalyst Systems
journal, April 2014
- Tylus, Urszula; Jia, Qingying; Strickland, Kara
- The Journal of Physical Chemistry C, Vol. 118, Issue 17
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
Development of non-precious metal oxygen-reduction catalysts for PEM fuel cells based on N-doped ordered porous carbon
journal, November 2009
- Liu, Gang; Li, Xuguang; Ganesan, Prabhu
- Applied Catalysis B: Environmental, Vol. 93, Issue 1-2, p. 156-165
The role of trace Fe in Fe–N-doped amorphous carbon with excellent electrocatalytic performance for oxygen reduction reaction
journal, February 2015
- Chen, Jingyan; Cui, Xiaoqiang; Zheng, Weitao
- Catalysis Communications, Vol. 60
Ordered mesoporous porphyrinic carbons with very high electrocatalytic activity for the oxygen reduction reaction
journal, September 2013
- Cheon, Jae Yeong; Kim, Taeyoung; Choi, YongMan
- Scientific Reports, Vol. 3, Issue 1
Oxygen reduction activities compared in rotating-disk electrode and proton exchange membrane fuel cells for highly active FeNC catalysts
journal, January 2013
- Jaouen, F.; Goellner, V.; Lefèvre, M.
- Electrochimica Acta, Vol. 87
Nanocasting: A Versatile Strategy for Creating Nanostructured Porous Materials
journal, July 2006
- Lu, A. -H.; Schüth, F.
- Advanced Materials, Vol. 18, Issue 14
Ordered mesoporous carbons with controlled particle sizes as catalyst supports for direct methanol fuel cell cathodes
journal, December 2008
- Joo, Sang Hoon; Lee, Hyung Ik; You, Dae Jong
- Carbon, Vol. 46, Issue 15
Synthesis and characterization of mesoporous carbon for fuel cell applications
journal, January 2007
- Chang, Hyuk; Joo, Sang Hoon; Pak, Chanho
- Journal of Materials Chemistry, Vol. 17, Issue 30
Preparation and characterization of Pt/C catalysts for PEMFC cathode: effect of different reduction methods
journal, January 2004
- Zhang, Jianlu; Wang, Xiaoli; Wu, Chuan
- Reaction Kinetics and Catalysis Letters, Vol. 83, Issue 2
Activities of Pt/C catalysts prepared by low temperature chemical reduction methods
journal, July 2006
- Zeng, Jianhuang; Lee, Jim Yang; Zhou, Weijiang
- Applied Catalysis A: General, Vol. 308
Studies on how to obtain the best catalytic activity of Pt/C catalyst by three reduction routes for methanol electro-oxidation
journal, April 2011
- Chen, Jinwei; Jiang, Chunping; Yang, Xin
- Electrochemistry Communications, Vol. 13, Issue 4
ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT
journal, June 2005
- Ravel, B.; Newville, M.
- Journal of Synchrotron Radiation, Vol. 12, Issue 4
IFEFFIT : interactive XAFS analysis and FEFF fitting
journal, March 2001
- Newville, Matthew
- Journal of Synchrotron Radiation, Vol. 8, Issue 2
Scattering-matrix formulation of curved-wave multiple-scattering theory: Application to x-ray-absorption fine structure
journal, April 1990
- Rehr, J. J.; Albers, R. C.
- Physical Review B, Vol. 41, Issue 12
Theoretical approaches to x-ray absorption fine structure
journal, July 2000
- Rehr, J. J.; Albers, R. C.
- Reviews of Modern Physics, Vol. 72, Issue 3
Impact of film drying procedures on RDE characterization of Pt/VC electrocatalysts
journal, November 2011
- Garsany, Yannick; Singer, Irwin L.; Swider-Lyons, Karen E.
- Journal of Electroanalytical Chemistry, Vol. 662, Issue 2
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996
- Kresse, G.; Furthmüller, J.
- Physical Review B, Vol. 54, Issue 16, p. 11169-11186
Ab initiomolecular dynamics for liquid metals
journal, January 1993
- Kresse, G.; Hafner, J.
- Physical Review B, Vol. 47, Issue 1, p. 558-561
Projector augmented-wave method
journal, December 1994
- Blöchl, P. E.
- Physical Review B, Vol. 50, Issue 24, p. 17953-17979
Generalized Gradient Approximation Made Simple
journal, October 1996
- Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
- Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
Special points for Brillouin-zone integrations
journal, June 1976
- Monkhorst, Hendrik J.; Pack, James D.
- Physical Review B, Vol. 13, Issue 12, p. 5188-5192
Bimetallic IrNi core platinum monolayer shell electrocatalysts for the oxygen reduction reaction
journal, January 2012
- Kuttiyiel, Kurian A.; Sasaki, Kotaro; Choi, YongMan
- Energy Environ. Sci., Vol. 5, Issue 1
Density-functional calculation of CeO2 surfaces and prediction of effects of oxygen partial pressure and temperature on stabilities
journal, August 2005
- Jiang, Yong; Adams, James B.; van Schilfgaarde, Mark
- The Journal of Chemical Physics, Vol. 123, Issue 6
Enhancement of the oxygen reduction on nitride stabilized pt-M (M=Fe, Co, and Ni) core–shell nanoparticle electrocatalysts
journal, April 2015
- Kuttiyiel, Kurian A.; Choi, YongMan; Hwang, Sun-Mi
- Nano Energy, Vol. 13
Oxygen Reduction on Well-Defined Core−Shell Nanocatalysts: Particle Size, Facet, and Pt Shell Thickness Effects
journal, December 2009
- Wang, Jia X.; Inada, Hiromi; Wu, Lijun
- Journal of the American Chemical Society, Vol. 131, Issue 47
Works referencing / citing this record:
Stabilization of Iron-Based Fuel Cell Catalysts by Non-Catalytic Platinum
journal, January 2018
- Mechler, Anna K.; Sahraie, Nastaran Ranjbar; Armel, Vanessa
- Journal of The Electrochemical Society, Vol. 165, Issue 13
Oxygen Reduction Reaction Catalyzed by Noble Metal Clusters
journal, February 2018
- Tang, Zhenghua; Wu, Wen; Wang, Kai
- Catalysts, Vol. 8, Issue 2