Half-cell electrode assessments of a crossover-tolerant direct methanol fuel cell with a platinum group metal-free cathode

Abdelrahman, Mohamed E.; Zhang, Hanguang; Wu, Gang; Li, Xianglin; Litster, Shawn

doi:10.1016/j.electacta.2022.140262

Half-cell electrode assessments of a crossover-tolerant direct methanol fuel cell with a platinum group metal-free cathode

Journal Article · Mon Mar 21 00:00:00 EDT 2022 · Electrochimica Acta

DOI:https://doi.org/10.1016/j.electacta.2022.140262· OSTI ID:1857905

Abdelrahman, Mohamed E. ^[1]; Zhang, Hanguang ^[2]; Wu, Gang ^[2]; Li, Xianglin ^[3]; Litster, Shawn ^[1]

Carnegie Mellon Univ., Pittsburgh, PA (United States)
Univ. at Buffalo, NY (United States)
Univ. of Kansas, Lawrence, KS (United States)

In this work, a platinum group metal- free (PGM-free) Fe-N-C oxygen reduction reaction (ORR) catalyst derived from metal organic framework precursors (Fe-MOF) is evaluated at the cathode side of a direct methanol fuel cell (DMFC). A wide range of methanol concentrations were used, and the performance of the DMFC using air was evaluated and compared to a commercial Pt/C cathode. We conducted our tests with a custom, integrated H₂ reference electrode that separately provided the anode and cathode overpotentials. This allowed us to perform a Tafel analysis on both electrodes and understand the dominant polarizations involved at the PGM-free cathode and the PtRu/C anode. Overall, we achieved a high cell performance using a Fe-N-C based catalyst under liquid methanol and air operation with a peak power density of 111 mW/cm², where the cathode presented a markedly larger contribution to the voltage loss versus the anode. Additionally, we used nanoscale X-ray computed tomography (nano-CT) to image the Fe-N-C cathode and investigate the ionomer and pore size distributions allowing us to identify areas of improvement for catalyst layer fabrication.

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Research Organization:: Univ. of Kansas, Lawrence, KS (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: EE0008440

OSTI ID:: 1857905

Alternate ID(s):: OSTI ID: 2568161

Journal Information:: Electrochimica Acta, Journal Name: Electrochimica Acta Vol. 416; ISSN 0013-4686

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (42)

High-Performance Direct Methanol Fuel Cells with Precious-Metal-Free Cathode Li, Qing; Wang, Tanyuan; Havas, Dana Advanced Science, Vol. 3, Issue 11 https://doi.org/10.1002/advs.201600140	journal	June 2016
The Solid-Phase Synthesis of an Fe-N-C Electrocatalyst for High-Power Proton-Exchange Membrane Fuel Cells Liu, Qingtao; Liu, Xiaofang; Zheng, Lirong Angewandte Chemie International Edition, Vol. 57, Issue 5 https://doi.org/10.1002/anie.201709597	journal	January 2018
High Performance and Cost-Effective Direct Methanol Fuel Cells: Fe-N-C Methanol-Tolerant Oxygen Reduction Reaction Catalysts Sebastián, David; Serov, Alexey; Artyushkova, Kateryna ChemSusChem, Vol. 9, Issue 15 https://doi.org/10.1002/cssc.201600583	journal	July 2016
Direct methanol fuel cells : Methanol crossover and its influence on single DMFC performance Song, S. Q.; Zhou, W. J.; Li, W. Z. Ionics, Vol. 10, Issue 5-6 https://doi.org/10.1007/BF02378008	journal	September 2004
Kinetic study of methanol oxidation on carbon-supported PtRu electrocatalyst Gojković, S. Lj.; Vidaković, T. R.; Đurović, D. R. Electrochimica Acta, Vol. 48, Issue 24 https://doi.org/10.1016/S0013-4686(03)00481-X	journal	October 2003
Performance of a direct methanol polymer electrolyte fuel cell Hwan Jung, Doo; Hyeong Lee, Chang; Soo Kim, Chang Journal of Power Sources, Vol. 71, Issue 1-2 https://doi.org/10.1016/S0378-7753(97)02793-6	journal	March 1998
Measurement of methanol crossover in direct methanol fuel cell Hikita, S. JSAE Review, Vol. 22, Issue 2 https://doi.org/10.1016/S0389-4304(01)00086-8	journal	April 2001
Performance analysis of a non-platinum group metal catalyst based on iron-aminoantipyrine for direct methanol fuel cells Sebastián, David; Baglio, Vincenzo; Aricò, Antonino S. Applied Catalysis B: Environmental, Vol. 182 https://doi.org/10.1016/j.apcatb.2015.09.043	journal	March 2016
Performance of a Fe-N-C catalyst for the oxygen reduction reaction in direct methanol fuel cell: Cathode formulation optimization and short-term durability Osmieri, Luigi; Escudero-Cid, Ricardo; Monteverde Videla, Alessandro H. A. Applied Catalysis B: Environmental, Vol. 201 https://doi.org/10.1016/j.apcatb.2016.08.043	journal	February 2017
Activity and degradation study of an Fe-N-C catalyst for ORR in Direct Methanol Fuel Cell (DMFC) Martinaiou, Ioanna; Monteverde Videla, Alessandro H. A.; Weidler, Natascha Applied Catalysis B: Environmental, Vol. 262 https://doi.org/10.1016/j.apcatb.2019.118217	journal	March 2020
Cobalt-polypyrrole-multiwalled carbon nanotube catalysts for hydrogen and alcohol fuel cells Mohana Reddy, Arava Leela; Rajalakshmi, Natarajan; Ramaprabhu, Sundara Carbon, Vol. 46, Issue 1 https://doi.org/10.1016/j.carbon.2007.10.021	journal	January 2008
Synthesis of nitrogen-doped onion-like carbon and its use in carbon-based CoFe binary non-precious-metal catalysts for oxygen-reduction Wu, Gang; Nelson, Mark; Ma, Shuguo Carbon, Vol. 49, Issue 12 https://doi.org/10.1016/j.carbon.2011.05.036	journal	October 2011
Positioning the reference electrode in proton exchange membrane fuel cells: calculations of primary and secondary current distribution Liu, Zhenyu; Wainright, J. S.; Huang, Weiwei Electrochimica Acta, Vol. 49, Issue 6 https://doi.org/10.1016/j.electacta.2003.10.004	journal	March 2004
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 Médard, C.; Lefèvre, M.; Dodelet, J. P. Electrochimica Acta, Vol. 51, Issue 16, p. 3202-3213 https://doi.org/10.1016/j.electacta.2005.09.012	journal	April 2006
Metal-free catalysts for oxygen reduction in alkaline electrolytes: Influence of the presence of Co, Fe, Mn and Ni inclusions Masa, Justus; Zhao, Anqi; Xia, Wei Electrochimica Acta, Vol. 128 https://doi.org/10.1016/j.electacta.2013.11.026	journal	May 2014
Oxygen reduction on non-noble metal electrocatalysts supported on N-doped carbon aerogel composites Wei, Yang; Shengzhou, Chen; Weiming, Lin International Journal of Hydrogen Energy, Vol. 37, Issue 1 https://doi.org/10.1016/j.ijhydene.2011.03.103	journal	January 2012
Ethanol crossover phenomena and its influence on the performance of DEFC Song, S.; Zhou, W.; Tian, J. Journal of Power Sources, Vol. 145, Issue 2 https://doi.org/10.1016/j.jpowsour.2004.12.065	journal	August 2005
Morphological features (defects) in fuel cell membrane electrode assemblies Kundu, S.; Fowler, M. W.; Simon, L. C. Journal of Power Sources, Vol. 157, Issue 2 https://doi.org/10.1016/j.jpowsour.2005.12.027	journal	July 2006
Transient and steady-state analysis of catalyst poisoning and mixed potential formation in direct methanol fuel cells Gerteisen, Dietmar Journal of Power Sources, Vol. 195, Issue 19 https://doi.org/10.1016/j.jpowsour.2010.04.004	journal	October 2010
Performance, methanol tolerance and stability of Fe-aminobenzimidazole derived catalyst for direct methanol fuel cells Sebastián, David; Serov, Alexey; Artyushkova, Kateryna Journal of Power Sources, Vol. 319 https://doi.org/10.1016/j.jpowsour.2016.04.067	journal	July 2016
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
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
Insights on the extraordinary tolerance to alcohols of Fe-N-C cathode catalysts in highly performing direct alcohol fuel cells Sebastián, D.; Serov, A.; Matanovic, I. Nano Energy, Vol. 34 https://doi.org/10.1016/j.nanoen.2017.02.039	journal	April 2017
High Power Density Platinum Group Metal-free Cathodes for Polymer Electrolyte Fuel Cells Uddin, Aman; Dunsmore, Lisa; Zhang, Hanguang ACS Applied Materials & Interfaces, Vol. 12, Issue 2 https://doi.org/10.1021/acsami.9b13945	journal	December 2019
Microporous Framework Induced Synthesis of Single-Atom Dispersed Fe-N-C Acidic ORR Catalyst and Its in Situ Reduced Fe-N ₄ Active Site Identification Revealed by X-ray Absorption Spectroscopy Xiao, Meiling; Zhu, Jianbing; Ma, Liang ACS Catalysis, Vol. 8, Issue 4 https://doi.org/10.1021/acscatal.8b00138	journal	February 2018
Constructing a Triple-Phase Interface in Micropores to Boost Performance of Fe/N/C Catalysts for Direct Methanol Fuel Cells Wang, Yu-Cheng; Huang, Long; Zhang, Pu ACS Energy Letters, Vol. 2, Issue 3 https://doi.org/10.1021/acsenergylett.7b00071	journal	February 2017
Effect of Transition Metals on the Structure and Performance of the Doped Carbon Catalysts Derived From Polyaniline and Melamine for ORR Application Peng, Hongliang; Liu, Fangfang; Liu, Xiaojun ACS Catalysis, Vol. 4, Issue 10 https://doi.org/10.1021/cs500744x	journal	September 2014
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
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
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
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
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
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
High-performance fuel cell cathodes exclusively containing atomically dispersed iron active sites Zhang, Hanguang; Chung, Hoon T.; Cullen, David A. Energy & Environmental Science, Vol. 12, Issue 8 https://doi.org/10.1039/C9EE00877B	journal	January 2019
Anodic engineering towards high-performance direct methanol fuel cells with non-precious-metal cathode catalysts Xia, Zhangxun; Xu, Xinlong; Zhang, Xiaoming Journal of Materials Chemistry A, Vol. 8, Issue 3 https://doi.org/10.1039/C9TA11440H	journal	January 2020
Methanol tolerance of atomically dispersed single metal site catalysts: mechanistic understanding and high-performance direct methanol fuel cells Shi, Qiurong; He, Yanghua; Bai, Xiaowan Energy & Environmental Science, Vol. 13, Issue 10 https://doi.org/10.1039/D0EE01968B	journal	January 2020
Investigation of Hydrogen Starvation of Polymer Electrolyte Fuel Cells in Freezing Condition Using Reference Electrode Hu, Leiming; Hong, Bo Ki; Oh, Jong-Gil ECS Transactions, Vol. 80, Issue 8 https://doi.org/10.1149/08008.0535ecst	journal	August 2017
Methanol Electro‐oxidation on Unsupported Pt‐Ru Alloys at Different Temperatures Chu, Deryn; Gilman, Sol Journal of The Electrochemical Society, Vol. 143, Issue 5 https://doi.org/10.1149/1.1836700	journal	May 1996
Methanol Diffusion in Perfluorinated Ion‐Exchange Membranes Verbrugge, Mark W. Journal of The Electrochemical Society, Vol. 136, Issue 2 https://doi.org/10.1149/1.2096646	journal	February 1989
Characterization of Membrane Degradation Growth in Fuel Cells Using X-ray Computed Tomography Ramani, Dilip; Singh, Yadvinder; Orfino, Francesco P. Journal of The Electrochemical Society, Vol. 165, Issue 6 https://doi.org/10.1149/2.0251806jes	journal	January 2018
PoreSpy: A Python Toolkit for Quantitative Analysis of Porous Media Images Gostick, Jeff; Khan, Zohaib; Tranter, Thomas Journal of Open Source Software, Vol. 4, Issue 37 https://doi.org/10.21105/joss.01296	journal	May 2019
Methanol-Tolerant M–N–C Catalysts for Oxygen Reduction Reactions in Acidic Media and Their Application in Direct Methanol Fuel Cells Lo Vecchio, Carmelo; Sebastián, David; Lázaro, María Catalysts, Vol. 8, Issue 12 https://doi.org/10.3390/catal8120650	journal	December 2018

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Half-cell electrode assessments of a crossover-tolerant direct methanol fuel cell with a platinum group metal-free cathode

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