Durable and self-hydrating tungsten carbide-based composite polymer electrolyte membrane fuel cells

Zheng, Weiqing; Wang, Liang; Deng, Fei; Giles, Stephen A.; Prasad, Ajay K.; Advani, Suresh G.; Yan, Yushan; Vlachos, Dionisios G.

doi:10.1038/s41467-017-00507-6

Title: Durable and self-hydrating tungsten carbide-based composite polymer electrolyte membrane fuel cells

Journal Article · Mon Sep 04 00:00:00 EDT 2017 · Nature Communications

DOI:https://doi.org/10.1038/s41467-017-00507-6· OSTI ID:1425195

Zheng, Weiqing ^[1];

^[2]; Deng, Fei ^[3]; Giles, Stephen A. ^[1]; Prasad, Ajay K. ^[2]; Advani, Suresh G. ^[2]; Yan, Yushan ^[1]; Vlachos, Dionisios G. ^[1]

Univ. of Delaware, Newark, DE (United States). Dept. of Chemical and Biomolecular Engineering and Catalysis Center for Energy Innovation and Center for Catalytic Science and Technology
Univ. of Delaware, Newark, DE (United States). Dept. of Mechanical Engineering and Center for Full Cell Research
Univ. of Delaware, Newark, DE (United States). Dept. of Materials Science and Engineering

Proton conductivity of the polymer electrolyte membranes in fuel cells dictates their performance and requires sufficient water management. Here, we report a simple, scalable method to produce well-dispersed transition metal carbide nanoparticles. We demonstrate that these, when added as an additive to the proton exchange Nafion membrane, provide significant enhancement in power density and durability over 100 hours, surpassing both the baseline Nafion and platinum-containing recast Nafion membranes. Using focused ion beam/scanning electron microscope tomography reveals the key membrane degradation mechanism. Density functional theory exposes that OH• and H• radicals adsorb more strongly from solution and reactions producing OH• are significantly more endergonic on tungsten carbide than on platinum. Consequently, tungsten carbide may be a promising catalyst in self-hydrating crossover gases while retarding desorption of and capturing free radicals formed at the cathode, resulting in enhanced membrane durability.

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Research Organization:: Univ. of Delaware, Newark, DE (United States); Energy Frontier Research Centers (EFRC) (United States). Catalysis Center for Energy Innovation (CCEI)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0001004

OSTI ID:: 1425195

Journal Information:: Nature Communications, Vol. 8, Issue 1; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 38 works

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References (45)

Nafion-Teflon-Zr(HPO[sub 4])[sub 2] Composite Membranes for High-Temperature PEMFCs Si, Yongchao; Kunz, H. Russell; Fenton, James M. Journal of The Electrochemical Society, Vol. 151, Issue 4 https://doi.org/10.1149/1.1651527	journal	January 2004
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
In-situ spin trap electron paramagnetic resonance study of fuel cell processes Panchenko, Alexander; Dilger, Herbert; Kerres, Jochen Physical Chemistry Chemical Physics, Vol. 6, Issue 11 https://doi.org/10.1039/b404253k	journal	January 2004
Experimental and Theoretical Investigation of Molybdenum Carbide and Nitride as Catalysts for Ammonia Decomposition Zheng, Weiqing; Cotter, Thomas P.; Kaghazchi, Payam Journal of the American Chemical Society, Vol. 135, Issue 9 https://doi.org/10.1021/ja309734u	journal	February 2013
Hydrothermal carbon from biomass: a comparison of the local structure from poly- to monosaccharides and pentoses/hexoses Titirici, Maria-Magdalena; Antonietti, Markus; Baccile, Niki Green Chemistry, Vol. 10, Issue 11 https://doi.org/10.1039/b807009a	journal	January 2008
Projector augmented-wave method Blöchl, P. E. Physical Review B, Vol. 50, Issue 24, p. 17953-17979 https://doi.org/10.1103/PhysRevB.50.17953	journal	December 1994
Tungsten Carbide Microspheres as a Noble-Metal-Economic Electrocatalyst for Methanol Oxidation Ganesan, Raman; Lee, Jae Sung Angewandte Chemie International Edition, Vol. 44, Issue 40 https://doi.org/10.1002/anie.200501272	journal	October 2005
Polymer Electrolyte Membranes Incorporated with Nanometer-Size Particles of Pt and/or Metal-Oxides: Experimental Analysis of the Self-Humidification and Suppression of Gas-Crossover in Fuel Cells Watanabe, Masahiro; Uchida, Hiroyuki; Emori, Masaomi The Journal of Physical Chemistry B, Vol. 102, Issue 17 https://doi.org/10.1021/jp973477e	journal	April 1998
Engineering Non-sintered, Metal-Terminated Tungsten Carbide Nanoparticles for Catalysis Hunt, Sean T.; Nimmanwudipong, Tarit; Román-Leshkov, Yuriy Angewandte Chemie, Vol. 126, Issue 20 https://doi.org/10.1002/ange.201400294	journal	April 2014
A review of polymer electrolyte membrane fuel cells: Technology, applications, and needs on fundamental research Wang, Yun; Chen, Ken S.; Mishler, Jeffrey Applied Energy, Vol. 88, Issue 4 https://doi.org/10.1016/j.apenergy.2010.09.030	journal	April 2011
Platinum-Like Behavior of Tungsten Carbide in Surface Catalysis Levy, R. B.; Boudart, M. Science, Vol. 181, Issue 4099 https://doi.org/10.1126/science.181.4099.547	journal	August 1973
N-doped carbon nanomaterials are durable catalysts for oxygen reduction reaction in acidic fuel cells Shui, Jianglan; Wang, Min; Du, Feng Science Advances, Vol. 1, Issue 1 https://doi.org/10.1126/sciadv.1400129	journal	February 2015
From ultrasoft pseudopotentials to the projector augmented-wave method Kresse, G.; Joubert, D. Physical Review B, Vol. 59, Issue 3, p. 1758-1775 https://doi.org/10.1103/PhysRevB.59.1758	journal	January 1999
Fuel Cells and Precious-Metal Catalysts Berger, D. J. Science, Vol. 286, Issue 5437 https://doi.org/10.1126/science.286.5437.49c	journal	October 1999
Scientific Aspects of Polymer Electrolyte Fuel Cell Durability and Degradation Borup, Rod; Meyers, Jeremy; Pivovar, Bryan Chemical Reviews, Vol. 107, Issue 10 https://doi.org/10.1021/cr050182l	journal	October 2007
Tungsten Carbide Microspheres as a Noble-Metal-Economic Electrocatalyst for Methanol Oxidation Ganesan, Raman; Lee, Jae Sung Angewandte Chemie, Vol. 117, Issue 40 https://doi.org/10.1002/ange.200501272	journal	October 2005
Über die Entstehung der Kohlen. II. Die Inkohlung von Cellulose und Lignin in neutralem Medium Berl, E.; Schmidt, A. Justus Liebig's Annalen der Chemie, Vol. 493, Issue 1 https://doi.org/10.1002/jlac.19324930106	journal	January 1932
Nafion/ZrSPP composite membrane for high temperature operation of PEMFCs Kim, Young-Taek; Song, Min-Kyu; Kim, Ki-Hyun Electrochimica Acta, Vol. 50, Issue 2-3 https://doi.org/10.1016/j.electacta.2003.12.079	journal	November 2004
Radical (HO●, H● and HOO●) Formation and Ionomer Degradation in Polymer Electrolyte Fuel Cells Gubler, Lorenz; Dockheer, Sindy M.; Koppenol, Willem H. Journal of The Electrochemical Society, Vol. 158, Issue 7 https://doi.org/10.1149/1.3581040	journal	January 2011
High-precision sampling for Brillouin-zone integration in metals Methfessel, M.; Paxton, A. T. Physical Review B, Vol. 40, Issue 6 https://doi.org/10.1103/PhysRevB.40.3616	journal	August 1989
Chemical Degradation of Nafion Membranes under Mimic Fuel Cell Conditions as Investigated by Solid-State NMR Spectroscopy Ghassemzadeh, Lida; Kreuer, Klaus-Dieter; Maier, Joachim The Journal of Physical Chemistry C, Vol. 114, Issue 34 https://doi.org/10.1021/jp102533v	journal	August 2010
Nafion® 115/zirconium phosphate composite membranes for operation of PEMFCs above 100°C Costamagna, P.; Yang, C.; Bocarsly, A. B. Electrochimica Acta, Vol. 47, Issue 7 https://doi.org/10.1016/S0013-4686(01)00829-5	journal	January 2002
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
Chemical degradation of proton conducting perflurosulfonic acid ionomer membranes studied by solid-state nuclear magnetic resonance spectroscopy Ghassemzadeh, L.; Marrony, M.; Barrera, R. Journal of Power Sources, Vol. 186, Issue 2 https://doi.org/10.1016/j.jpowsour.2008.10.004	journal	January 2009
Molybdenum carbide catalysts I. Synthesis of unsupported powders Lee, J. Journal of Catalysis, Vol. 106, Issue 1 https://doi.org/10.1016/0021-9517(87)90218-1	journal	July 1987
A Direct Synthesis of Mesoporous Carbons with Bicontinuous Pore Morphology from Crude Plant Material by Hydrothermal Carbonization Titirici, Maria M.; Thomas, Arne; Yu, Shu-Hong Chemistry of Materials, Vol. 19, Issue 17 https://doi.org/10.1021/cm0707408	journal	August 2007
Mechanism for Degradation of Nafion in PEM Fuel Cells from Quantum Mechanics Calculations Yu, Ted H.; Sha, Yao; Liu, Wei-Guang Journal of the American Chemical Society, Vol. 133, Issue 49 https://doi.org/10.1021/ja2074642	journal	December 2011
Nanosized tungsten carbide synthesized by a novel route at low temperature for high performance electrocatalysis Yan, Zaoxue; Cai, Mei; Shen, Pei Kang Scientific Reports, Vol. 3, Issue 1 https://doi.org/10.1038/srep01646	journal	April 2013
Chemistry and materials options of sustainable carbon materials made by hydrothermal carbonization Titirici, Maria-Magdalena; Antonietti, Markus Chem. Soc. Rev., Vol. 39, Issue 1 https://doi.org/10.1039/B819318P	journal	January 2010
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set Kresse, G.; Furthmüller, J. Computational Materials Science, Vol. 6, Issue 1, p. 15-50 https://doi.org/10.1016/0927-0256(96)00008-0	journal	July 1996
Universality in Oxygen Evolution Electrocatalysis on Oxide Surfaces Man, Isabela C.; Su, Hai‐Yan; Calle‐Vallejo, Federico ChemCatChem, Vol. 3, Issue 7 https://doi.org/10.1002/cctc.201000397	journal	March 2011
Materials for fuel-cell technologies Steele, Brian C. H.; Heinzel, Angelika Nature, Vol. 414, Issue 6861, p. 345-352 https://doi.org/10.1038/35104620	journal	November 2001
Membrane degradation during combined chemical and mechanical accelerated stress testing of polymer electrolyte fuel cells Lim, C.; Ghassemzadeh, L.; Van Hove, F. Journal of Power Sources, Vol. 257 https://doi.org/10.1016/j.jpowsour.2014.01.106	journal	July 2014
Nanocrack-regulated self-humidifying membranes Park, Chi Hoon; Lee, So Young; Hwang, Doo Sung Nature, Vol. 532, Issue 7600 https://doi.org/10.1038/nature17634	journal	April 2016
PEM Fuel Cell Pt∕C Dissolution and Deposition in Nafion Electrolyte Bi, Wu; Gray, Gary E.; Fuller, Thomas F. Electrochemical and Solid-State Letters, Vol. 10, Issue 5 https://doi.org/10.1149/1.2712796	journal	January 2007
Special points for Brillouin-zone integrations Monkhorst, Hendrik J.; Pack, James D. Physical Review B, Vol. 13, Issue 12, p. 5188-5192 https://doi.org/10.1103/PhysRevB.13.5188	journal	June 1976
Suppression of Methanol Crossover and Distribution of Ohmic Resistance in Pt-Dispersed PEMs under DMFC Operation Uchida, Hiroyuki; Mizuno, Yohsuke; Watanabe, Masahiro Journal of The Electrochemical Society, Vol. 149, Issue 6 https://doi.org/10.1149/1.1471539	journal	January 2002
Polymer Electrolyte Fuel Cell Model Springer, T. E. Journal of The Electrochemical Society, Vol. 138, Issue 8 https://doi.org/10.1149/1.2085971	journal	January 1991
Back in the black: hydrothermal carbonization of plant material as an efficient chemical process to treat the CO2 problem? Titirici, Maria-Magdalena; Thomas, Arne; Antonietti, Markus New Journal of Chemistry, Vol. 31, Issue 6 https://doi.org/10.1039/b616045j	journal	January 2007
Solution of Schrödinger’s equation for large systems Teter, Michael P.; Payne, Michael C.; Allan, Douglas C. Physical Review B, Vol. 40, Issue 18 https://doi.org/10.1103/PhysRevB.40.12255	journal	December 1989
Self-Humidifying Polymer Electrolyte Membranes for Fuel Cells Watanabe, Masahiro Journal of The Electrochemical Society, Vol. 143, Issue 12 https://doi.org/10.1149/1.1837307	journal	January 1996
Dual-Beam (FIB-SEM) Systems Young, Richard J.; Moore, Mary V. Introduction to Focused Ion Beams https://doi.org/10.1007/0-387-23313-X_12	book	January 2005
A Water and Heat Management Model for Proton-Exchange-Membrane Fuel Cells Nguyen, Trung V. Journal of The Electrochemical Society, Vol. 140, Issue 8 https://doi.org/10.1149/1.2220792	journal	January 1993
Nafion–TiO2 hybrid membranes for medium temperature polymer electrolyte fuel cells (PEFCs) Saccà, A.; Carbone, A.; Passalacqua, E. Journal of Power Sources, Vol. 152 https://doi.org/10.1016/j.jpowsour.2004.12.053	journal	December 2005
Engineering Non-sintered, Metal-Terminated Tungsten Carbide Nanoparticles for Catalysis Hunt, Sean T.; Nimmanwudipong, Tarit; Román-Leshkov, Yuriy Angewandte Chemie International Edition https://doi.org/10.1002/anie.201400294	journal	April 2014

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Planar polymer electrolyte membrane fuel cells: powering portable devices from hydrogen Sapkota, Prabal; Boyer, Cyrille; Dutta, Rukmi Sustainable Energy & Fuels, Vol. 4, Issue 2 https://doi.org/10.1039/c9se00861f	journal	January 2020
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