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Title: Anode-Design Strategies for Improved Performance of Polymer-Electrolyte Fuel Cells with Ultra-Thin Electrodes

Abstract

We report results of systematic, holistic, diagnostic, and cell studies to elucidate the mechanistic role of the experimentally determined influence of the anode gas-diffusion layer (GDL) on the performance of ultra-thin electrode polymer-electrolyte fuel cells, which can further enable fuel-cell market penetration. Measurements of product water balance and in situ neutron imaging of operational membrane-electrode-assembly water profiles demonstrate how improved performance is due to a novel anode GDL fiber-density modulated structure at the micrometer scale that removes water preferentially out of the anode, a key strategy to manage water in these cells. The banded structure results in low transport-resistance pathways, which affect water-droplet removal from the GDL surface. This interfacial effect is unexpectedly shown to be critical for decreasing overall water holdup throughout the cell. These studies demonstrate a new material paradigm for understanding and controlling fuel-cell water management and related high-power technologies or electrodes where multiphase flow occurs. Very thin electrodes enable high power density in electrochemical technologies, yet their thinness engenders issues related to buildup of products (e.g., water in polymer-electrolyte fuel cells [PEFCs]). The article explores an unexpected materials solution to the problem, which highlights the need to study such complicated systems in a holistic manner ofmore » a complete cell due to the nonlinearities existent in the highly coupled physical phenomena. The improved performance is due to an inherent unintentional manufacturing heterogeneity in the cell backing layer, which mainly affects its surface properties. With this knowledge, one can now engineer and optimize these critical heterogeneities for different architectures. The findings are relevant to those working on materials for electrochemical energy conversion and represent new key knowledge that can have significant impact in PEFCs and related electrochemical cells, especially where multiphase flow occurs. High-power electrodes in electrochemical technologies (e.g., fuel cells) typically require ultra-thin catalyst layers, which, especially when multiphase flow exists, exhibit mass-transport limitations. These have been mitigated through new backing layer structures and nontraditional removal of water out of the anode side of the cell for a new design and operation paradigm.« less

Authors:
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Publication Date:
Research Org.:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). Center for Neutron Research
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Sustainable Transportation Office. Hydrogen Fuel Cell Technologies Office (HFTO); Dept. of Commerce (United States)
OSTI Identifier:
1564422
Alternate Identifier(s):
OSTI ID: 1477693; OSTI ID: 1601647
Report Number(s):
LA-UR-17-28090
Journal ID: ISSN 2542-4351; S2542435118301375; PII: S2542435118301375
Grant/Contract Number:  
AC02-05CH11231; AI01-01EE50660; AC52-06NA25396
Resource Type:
Published Article
Journal Name:
Joule
Additional Journal Information:
Journal Name: Joule Journal Volume: 2 Journal Issue: 7; Journal ID: ISSN 2542-4351
Publisher:
Elsevier - Cell Press
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; fuel cells; ultra-thin electrodes; water management; transport phenomena; material design; heterogeneous substrate; gas diffusion layer; neutron radiography; x-ray computed tomography

Citation Formats

Steinbach, Andrew J., Allen, Jeffrey S., Borup, Rodney L., Hussey, Daniel S., Jacobson, David L., Komlev, Andrei, Kwong, Anthony, MacDonald, James, Mukundan, Rangachary, Pejsa, Matt J., Roos, Michael, Santamaria, Anthony D., Sieracki, James M., Spernjak, Dusan, Zenyuk, Iryna V., and Weber, Adam Z. Anode-Design Strategies for Improved Performance of Polymer-Electrolyte Fuel Cells with Ultra-Thin Electrodes. United States: N. p., 2018. Web. doi:10.1016/j.joule.2018.03.022.
Steinbach, Andrew J., Allen, Jeffrey S., Borup, Rodney L., Hussey, Daniel S., Jacobson, David L., Komlev, Andrei, Kwong, Anthony, MacDonald, James, Mukundan, Rangachary, Pejsa, Matt J., Roos, Michael, Santamaria, Anthony D., Sieracki, James M., Spernjak, Dusan, Zenyuk, Iryna V., & Weber, Adam Z. Anode-Design Strategies for Improved Performance of Polymer-Electrolyte Fuel Cells with Ultra-Thin Electrodes. United States. https://doi.org/10.1016/j.joule.2018.03.022
Steinbach, Andrew J., Allen, Jeffrey S., Borup, Rodney L., Hussey, Daniel S., Jacobson, David L., Komlev, Andrei, Kwong, Anthony, MacDonald, James, Mukundan, Rangachary, Pejsa, Matt J., Roos, Michael, Santamaria, Anthony D., Sieracki, James M., Spernjak, Dusan, Zenyuk, Iryna V., and Weber, Adam Z. Sun . "Anode-Design Strategies for Improved Performance of Polymer-Electrolyte Fuel Cells with Ultra-Thin Electrodes". United States. https://doi.org/10.1016/j.joule.2018.03.022.
@article{osti_1564422,
title = {Anode-Design Strategies for Improved Performance of Polymer-Electrolyte Fuel Cells with Ultra-Thin Electrodes},
author = {Steinbach, Andrew J. and Allen, Jeffrey S. and Borup, Rodney L. and Hussey, Daniel S. and Jacobson, David L. and Komlev, Andrei and Kwong, Anthony and MacDonald, James and Mukundan, Rangachary and Pejsa, Matt J. and Roos, Michael and Santamaria, Anthony D. and Sieracki, James M. and Spernjak, Dusan and Zenyuk, Iryna V. and Weber, Adam Z.},
abstractNote = {We report results of systematic, holistic, diagnostic, and cell studies to elucidate the mechanistic role of the experimentally determined influence of the anode gas-diffusion layer (GDL) on the performance of ultra-thin electrode polymer-electrolyte fuel cells, which can further enable fuel-cell market penetration. Measurements of product water balance and in situ neutron imaging of operational membrane-electrode-assembly water profiles demonstrate how improved performance is due to a novel anode GDL fiber-density modulated structure at the micrometer scale that removes water preferentially out of the anode, a key strategy to manage water in these cells. The banded structure results in low transport-resistance pathways, which affect water-droplet removal from the GDL surface. This interfacial effect is unexpectedly shown to be critical for decreasing overall water holdup throughout the cell. These studies demonstrate a new material paradigm for understanding and controlling fuel-cell water management and related high-power technologies or electrodes where multiphase flow occurs. Very thin electrodes enable high power density in electrochemical technologies, yet their thinness engenders issues related to buildup of products (e.g., water in polymer-electrolyte fuel cells [PEFCs]). The article explores an unexpected materials solution to the problem, which highlights the need to study such complicated systems in a holistic manner of a complete cell due to the nonlinearities existent in the highly coupled physical phenomena. The improved performance is due to an inherent unintentional manufacturing heterogeneity in the cell backing layer, which mainly affects its surface properties. With this knowledge, one can now engineer and optimize these critical heterogeneities for different architectures. The findings are relevant to those working on materials for electrochemical energy conversion and represent new key knowledge that can have significant impact in PEFCs and related electrochemical cells, especially where multiphase flow occurs. High-power electrodes in electrochemical technologies (e.g., fuel cells) typically require ultra-thin catalyst layers, which, especially when multiphase flow exists, exhibit mass-transport limitations. These have been mitigated through new backing layer structures and nontraditional removal of water out of the anode side of the cell for a new design and operation paradigm.},
doi = {10.1016/j.joule.2018.03.022},
journal = {Joule},
number = 7,
volume = 2,
place = {United States},
year = {Sun Jul 01 00:00:00 EDT 2018},
month = {Sun Jul 01 00:00:00 EDT 2018}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1016/j.joule.2018.03.022

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Cited by: 39 works
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Works referenced in this record:

Capillary pressure and hydrophilic porosity in gas diffusion layers for polymer electrolyte fuel cells
journal, June 2006


Investigation of Water Transport in Perforated Gas Diffusion Layer by Neutron Radiography
journal, August 2013


Engineered Water Highways in Fuel Cells: Radiation Grafting of Gas Diffusion Layers
journal, September 2015

  • Forner-Cuenca, Antoni; Biesdorf, Johannes; Gubler, Lorenz
  • Advanced Materials, Vol. 27, Issue 41
  • DOI: 10.1002/adma.201503557

Visualization of the water distribution in perforated gas diffusion layers by means of synchrotron X-ray radiography
journal, May 2012


Implementation of a fast method for high resolution phase contrast tomography
journal, January 2006


Water Transport Mechanisms in PEMFC Gas Diffusion Layers
journal, January 2010

  • Owejan, Jon P.; Owejan, Jeanette E.; Gu, Wenbin
  • Journal of The Electrochemical Society, Vol. 157, Issue 10
  • DOI: 10.1149/1.3468615

Fuel Cell Electrocatalyst Using Polybenzimidazole-Modified Carbon Nanotubes As Support Materials
journal, February 2013


Integrated High-Efficiency Pt/Carbon Nanotube Arrays for PEM Fuel Cells
journal, May 2011

  • Zhang, Weimin; Minett, Andrew I.; Gao, Mei
  • Advanced Energy Materials, Vol. 1, Issue 4
  • DOI: 10.1002/aenm.201100092

Initial Performance and Durability of Ultra-Low Loaded NSTF Electrodes for PEM Electrolyzers
journal, January 2012

  • Debe, M. K.; Hendricks, S. M.; Vernstrom, G. D.
  • Journal of The Electrochemical Society, Vol. 159, Issue 6
  • DOI: 10.1149/2.065206jes

Laser perforated fuel cell diffusion media. Part I: Related changes in performance and water content
journal, July 2011


A Highly Order-Structured Membrane Electrode Assembly with Vertically Aligned Carbon Nanotubes for Ultra-Low Pt Loading PEM Fuel Cells
journal, September 2011

  • Tian, Zhi Qun; Lim, San Hua; Poh, Chee Kok
  • Advanced Energy Materials, Vol. 1, Issue 6
  • DOI: 10.1002/aenm.201100371

Advanced Redox-Flow Batteries: A Perspective
journal, September 2015

  • Perry, Mike L.; Weber, Adam Z.
  • Journal of The Electrochemical Society, Vol. 163, Issue 1
  • DOI: 10.1149/2.0101601jes

Electrocatalyst approaches and challenges for automotive fuel cells
journal, June 2012


Investigating Evaporation in Gas Diffusion Layers for Fuel Cells with X-ray Computed Tomography
journal, December 2016

  • Zenyuk, Iryna V.; Lamibrac, Adrien; Eller, Jens
  • The Journal of Physical Chemistry C, Vol. 120, Issue 50
  • DOI: 10.1021/acs.jpcc.6b10658

Influence of Anode GDL on PEMFC Ultra-Thin Electrode Water Management at Low Temperatures
conference, January 2011

  • Steinbach, Andrew J.; Debe, Mark K.; Pejsa, Matthew J.
  • 220th ECS Meeting, ECS Transactions
  • DOI: 10.1149/1.3635579

Probing water distribution in compressed fuel-cell gas-diffusion layers using X-ray computed tomography
journal, April 2015


Coupled Thermal and Water Management in Polymer Electrolyte Fuel Cells
journal, January 2006

  • Weber, Adam Z.; Newman, John
  • Journal of The Electrochemical Society, Vol. 153, Issue 12
  • DOI: 10.1149/1.2352039

Synchrotron radiography and tomography of water transport in perforated gas diffusion media
journal, October 2013


Effective-Diffusivity Measurement of Partially-Saturated Fuel-Cell Gas-Diffusion Layers
journal, January 2012

  • Hwang, G. S.; Weber, A. Z.
  • Journal of The Electrochemical Society, Vol. 159, Issue 11
  • DOI: 10.1149/2.024211jes

Visualising Liquid Water in PEM Fuel Cells Using Neutron Imaging
journal, October 2009


Toyota MIRAI Fuel Cell Vehicle and Progress Toward a Future Hydrogen Society
journal, January 2015


Investigation of Temperature-Driven Water Transport in Polymer Electrolyte Fuel Cell: Phase-Change-Induced Flow
journal, January 2009

  • Kim, Soowhan; Mench, M. M.
  • Journal of The Electrochemical Society, Vol. 156, Issue 3
  • DOI: 10.1149/1.3046136

Long-Term Stability of Nanostructured Thin Film Electrodes at Operating Potentials
journal, January 2017

  • Ahluwalia, R. K.; Peng, J. -K.; Wang, X.
  • Journal of The Electrochemical Society, Vol. 164, Issue 4
  • DOI: 10.1149/2.0881704jes

Supportless Platinum Nanotubes Array by Atomic Layer Deposition as PEM Fuel Cell Electrode
journal, April 2014


Fabrication and Cell Analysis of a Pt/SiO 2 Platinum Thin Film Electrode
journal, January 2015

  • Inaba, Masanori; Suzuki, Takahisa; Hatanaka, Tatsuya
  • Journal of The Electrochemical Society, Vol. 162, Issue 7
  • DOI: 10.1149/2.0201507jes

Ex situ measurements of through-plane thermal conductivities in a polymer electrolyte fuel cell
journal, January 2010


Accurate measurement of the through-plane water content of proton-exchange membranes using neutron radiography
journal, November 2012

  • Hussey, D. S.; Spernjak, D.; Weber, A. Z.
  • Journal of Applied Physics, Vol. 112, Issue 10
  • DOI: 10.1063/1.4767118

Analysis of Low Platinum Loading Thin Polymer Electrolyte Fuel Cell Electrodes Prepared by Inkjet Printing
journal, February 2015


Understanding Impacts of Catalyst-Layer Thickness on Fuel-Cell Performance via Mathematical Modeling
journal, January 2016

  • Zenyuk, Iryna V.; Das, Prodip K.; Weber, Adam Z.
  • Journal of The Electrochemical Society, Vol. 163, Issue 7
  • DOI: 10.1149/2.1161607jes

Computational and Experimental Analysis of Water Transport at Component Interfaces in Polymer Electrolyte Fuel Cells
journal, January 2014

  • Zenyuk, I. V.; Taspinar, R.; Kalidindi, A. R.
  • Journal of The Electrochemical Society, Vol. 161, Issue 11
  • DOI: 10.1149/2.0161411jes

Liquid-Water-Droplet Adhesion-Force Measurements on Fresh and Aged Fuel-Cell Gas-Diffusion Layers
journal, January 2012

  • Das, Prodip K.; Grippin, Adam; Kwong, Anthony
  • Journal of The Electrochemical Society, Vol. 159, Issue 5
  • DOI: 10.1149/2.052205jes

Stability and performance improvement of a polymer electrolyte membrane fuel cell stack by laser perforation of gas diffusion layers
journal, August 2010


In Situ High-Resolution Neutron Radiography of Cross-Sectional Liquid Water Profiles in Proton Exchange Membrane Fuel Cells
journal, January 2008

  • Hickner, M. A.; Siegel, N. P.; Chen, K. S.
  • Journal of The Electrochemical Society, Vol. 155, Issue 4
  • DOI: 10.1149/1.2826287

Redox flow batteries a review
journal, September 2011

  • Weber, Adam Z.; Mench, Matthew M.; Meyers, Jeremy P.
  • Journal of Applied Electrochemistry, Vol. 41, Issue 10, p. 1137-1164
  • DOI: 10.1007/s10800-011-0348-2

Laser Perforated Fuel Cell Diffusion Media: Engineered Interfaces for Improved Ionic and Oxygen Transport
journal, January 2012

  • Manahan, M. P.; Mench, M. M.
  • Journal of The Electrochemical Society, Vol. 159, Issue 7
  • DOI: 10.1149/2.084207jes

High voltage stability of nanostructured thin film catalysts for PEM fuel cells
journal, October 2006


Imaging of Water Profiles in PEM Fuel Cells Using Neutron Radiography: Effect of Operating Conditions and GDL Composition
journal, September 2007

  • Mukundan, R.; Davey, John R.; Rockward, Tommy
  • ECS Transactions, Vol. 11, Issue 1
  • DOI: 10.1149/1.2780955

A Mixed Wettability Pore Size Distribution Based Mathematical Model for Analyzing Two-Phase Flow in Porous Electrodes: I. Mathematical Model
journal, January 2017

  • Zhou, J.; Putz, A.; Secanell, M.
  • Journal of The Electrochemical Society, Vol. 164, Issue 6
  • DOI: 10.1149/2.0381706jes

Influence of cracks in the microporous layer on the water distribution in a PEM fuel cell investigated by synchrotron radiography
journal, September 2013


Enhancing liquid water transport by laser perforation of a GDL in a PEM fuel cell
journal, March 2008


Investigating fuel-cell transport limitations using hydrogen limiting current
journal, May 2017


A New Paradigm for PEMFC Ultra-Thin Electrode Water Management at Low Temperatures
conference, January 2010

  • Steinbach, Andrew J.; Debe, Mark K.; Wong, Jimmy
  • 218th ECS Meeting, ECS Transactions
  • DOI: 10.1149/1.3484611

Performance of Nano Structured Thin Film (NSTF) Electrodes under Partially-Humidified Conditions
journal, January 2011

  • Sinha, Puneet K.; Gu, Wenbin; Kongkanand, Anusorn
  • Journal of The Electrochemical Society, Vol. 158, Issue 7
  • DOI: 10.1149/1.3590748

Liquid-Water Interactions with Gas-Diffusion-Layer Surfaces
journal, January 2014

  • Santamaria, Anthony D.; Das, Prodip K.; MacDonald, James C.
  • Journal of The Electrochemical Society, Vol. 161, Issue 12
  • DOI: 10.1149/2.0321412jes

Dynamic Percolation and Droplet Growth Behavior in Porous Electrodes of Polymer Electrolyte Fuel Cells
journal, September 2015

  • Quesnel, Charles; Cao, Ren; Lehr, Jorge
  • The Journal of Physical Chemistry C, Vol. 119, Issue 40
  • DOI: 10.1021/acs.jpcc.5b06197

A comprehensive review on PEM water electrolysis
journal, April 2013

  • Carmo, Marcelo; Fritz, David L.; Mergel, Jürgen
  • International Journal of Hydrogen Energy, Vol. 38, Issue 12, p. 4901-4934
  • DOI: 10.1016/j.ijhydene.2013.01.151

The influence of porous transport layer modifications on the water management in polymer electrolyte membrane fuel cells
journal, July 2013


Effects of Cathode Corrosion on Through-Plane Water Transport in Proton Exchange Membrane Fuel Cells
journal, January 2013

  • Fairweather, Joseph D.; Spernjak, Dusan; Weber, Adam Z.
  • Journal of The Electrochemical Society, Vol. 160, Issue 9
  • DOI: 10.1149/2.024309jes

Measurement of liquid water content in cathode gas diffusion electrode of polymer electrolyte fuel cell
journal, June 2010