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Title: Quantifying and elucidating the effect of CO 2 on the thermodynamics, kinetics and charge transport of AEMFCs

Abstract

It has been long-recognized that carbonation of anion exchange membrane fuel cells (AEMFCs) would be an important practical barrier for their implementation in applications that use ambient air containing atmospheric CO2. Most literature discussion around AEMFC carbonation has hypothesized: (1) that the effect of carbonation is limited to an increase in the Ohmic resistance because carbonate has lower mobility than hydroxide; and/or (2) that the so-called “self-purging” mechanism could effectively decarbonate the cell and eliminate CO2-related voltage losses during operation at a reasonable operating current density (>1 A cm-2). However, this study definitively shows that neither of these assertions are correct. This work, the first experimental examination of its kind, studies the dynamics of cell carbonation and its effect on AEMFC performance over a wide range of operating currents (0.2–2.0 A cm-2), operating temperatures (60–80 °C) and CO2 concentrations in the reactant gases (5–3200 ppm). The resulting data provide for new fundamental relationships to be developed and for the root causes of increased polarization in the presence of CO2 to be quantitatively probed and deconvoluted into Ohmic, Nernstian and charge transfer components, with the Nernstian and charge transfer components controlling the cell behavior under conditions of practical interest.

Authors:
 [1]; ORCiD logo [1];  [1]; ORCiD logo [2]; ORCiD logo [2];  [3]; ORCiD logo [1]
  1. Department of Chemical Engineering, University of South Carolina, Columbia, USA
  2. National Renewable Energy Laboratory, Golden, USA
  3. Department of Chemistry, University of Surrey, Guildford, UK
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Sustainable Transportation Office. Hydrogen Fuel Cell Technologies Office
OSTI Identifier:
1543357
Alternate Identifier(s):
OSTI ID: 1569451
Report Number(s):
NREL/JA-5900-75049
Journal ID: ISSN 1754-5692; EESNBY
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Published Article
Journal Name:
Energy & Environmental Science
Additional Journal Information:
Journal Name: Energy & Environmental Science Journal Volume: 12 Journal Issue: 9; Journal ID: ISSN 1754-5692
Publisher:
Royal Society of Chemistry (RSC)
Country of Publication:
United Kingdom
Language:
English
Subject:
30 DIRECT ENERGY CONVERSION; alkaline fuel cells; carbonation; charge transfer; ion exchange membranes; ohmic contacts; thermodynamics

Citation Formats

Zheng, Yiwei, Omasta, Travis J., Peng, Xiong, Wang, Lianqin, Varcoe, John R., Pivovar, Bryan S., and Mustain, William E. Quantifying and elucidating the effect of CO 2 on the thermodynamics, kinetics and charge transport of AEMFCs. United Kingdom: N. p., 2019. Web. doi:10.1039/C9EE01334B.
Zheng, Yiwei, Omasta, Travis J., Peng, Xiong, Wang, Lianqin, Varcoe, John R., Pivovar, Bryan S., & Mustain, William E. Quantifying and elucidating the effect of CO 2 on the thermodynamics, kinetics and charge transport of AEMFCs. United Kingdom. https://doi.org/10.1039/C9EE01334B
Zheng, Yiwei, Omasta, Travis J., Peng, Xiong, Wang, Lianqin, Varcoe, John R., Pivovar, Bryan S., and Mustain, William E. Thu . "Quantifying and elucidating the effect of CO 2 on the thermodynamics, kinetics and charge transport of AEMFCs". United Kingdom. https://doi.org/10.1039/C9EE01334B.
@article{osti_1543357,
title = {Quantifying and elucidating the effect of CO 2 on the thermodynamics, kinetics and charge transport of AEMFCs},
author = {Zheng, Yiwei and Omasta, Travis J. and Peng, Xiong and Wang, Lianqin and Varcoe, John R. and Pivovar, Bryan S. and Mustain, William E.},
abstractNote = {It has been long-recognized that carbonation of anion exchange membrane fuel cells (AEMFCs) would be an important practical barrier for their implementation in applications that use ambient air containing atmospheric CO2. Most literature discussion around AEMFC carbonation has hypothesized: (1) that the effect of carbonation is limited to an increase in the Ohmic resistance because carbonate has lower mobility than hydroxide; and/or (2) that the so-called “self-purging” mechanism could effectively decarbonate the cell and eliminate CO2-related voltage losses during operation at a reasonable operating current density (>1 A cm-2). However, this study definitively shows that neither of these assertions are correct. This work, the first experimental examination of its kind, studies the dynamics of cell carbonation and its effect on AEMFC performance over a wide range of operating currents (0.2–2.0 A cm-2), operating temperatures (60–80 °C) and CO2 concentrations in the reactant gases (5–3200 ppm). The resulting data provide for new fundamental relationships to be developed and for the root causes of increased polarization in the presence of CO2 to be quantitatively probed and deconvoluted into Ohmic, Nernstian and charge transfer components, with the Nernstian and charge transfer components controlling the cell behavior under conditions of practical interest.},
doi = {10.1039/C9EE01334B},
journal = {Energy & Environmental Science},
number = 9,
volume = 12,
place = {United Kingdom},
year = {Thu Sep 12 00:00:00 EDT 2019},
month = {Thu Sep 12 00:00:00 EDT 2019}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1039/C9EE01334B

Citation Metrics:
Cited by: 55 works
Citation information provided by
Web of Science

Figures / Tables:

Fig. 1 Fig. 1: Illustration of the carbonate and hydroxide transport and distribution in operating AEMFCs with CO2 present in the cathode reacting gas. The top section of the diagram isolates the CO3 2- behavior in operating cells, with the color gradient representing the concentration gradient. The top section of themore » diagram shows the OH- concentration gradient, as well as the directionality for hydroxide migration and diffusion.« less

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Works referenced in this record:

Non-fluorinated pre-irradiation-grafted (peroxidated) LDPE-based anion-exchange membranes with high performance and stability
journal, January 2017

  • Wang, Lianqin; Brink, Jethro J.; Liu, Ye
  • Energy & Environmental Science, Vol. 10, Issue 10
  • DOI: 10.1039/C7EE02053H

Importance of balancing membrane and electrode water in anion exchange membrane fuel cells
journal, January 2018


Influence of Carbon Dioxide on the Performance of Anion-Exchange Membrane Fuel Cells
conference, January 2010

  • Matsui, Yu; Saito, Morihiro; Tasaka, Akimasa
  • 216th ECS Meeting, ECS Transactions
  • DOI: 10.1149/1.3315177

Preparation of radiation-grafted powders for use as anion exchange ionomers in alkaline polymer electrolyte fuel cells
journal, January 2014

  • Poynton, Simon D.; Slade, Robert C. T.; Omasta, Travis J.
  • J. Mater. Chem. A, Vol. 2, Issue 14
  • DOI: 10.1039/C4TA00558A

Hydrogen and Methanol Oxidation Reaction in Hydroxide and Carbonate Alkaline Media
journal, January 2011

  • Vega, Jose A.; Smith, Shawna; Mustain, William E.
  • Journal of The Electrochemical Society, Vol. 158, Issue 4
  • DOI: 10.1149/1.3543918

Composite Poly(norbornene) Anion Conducting Membranes for Achieving Durability, Water Management and High Power (3.4 W/cm 2 ) in Hydrogen/Oxygen Alkaline Fuel Cells
journal, January 2019

  • Huang, Garrett; Mandal, Mrinmay; Peng, Xiong
  • Journal of The Electrochemical Society, Vol. 166, Issue 10
  • DOI: 10.1149/2.1301910jes

Impact of carbonation processes in anion exchange membrane fuel cells
journal, February 2018


Poly(aryl piperidinium) membranes and ionomers for hydroxide exchange membrane fuel cells
journal, April 2019


Bicarbonate and chloride anion transport in anion exchange membranes
journal, September 2016


Mathematical Modeling of the Concentration Profile of Carbonate Ions in an Anion Exchange Membrane Fuel Cell
conference, January 2010

  • Siroma, Zyun; Watanabe, Shin; Yasuda, Kazuaki
  • 218th ECS Meeting, ECS Transactions
  • DOI: 10.1149/1.3484685

Along-the-Channel Impacts of Water Management and Carbon-Dioxide Contamination in Hydroxide-Exchange-Membrane Fuel Cells: A Modeling Study
journal, January 2019

  • Gerhardt, Michael R.; Pant, Lalit M.; Weber, Adam Z.
  • Journal of The Electrochemical Society, Vol. 166, Issue 7
  • DOI: 10.1149/2.0171907jes

Carbonate Dynamics and Opportunities With Low Temperature, Anion Exchange Membrane-Based Electrochemical Carbon Dioxide Separators
journal, May 2017

  • Rigdon, William A.; Omasta, Travis J.; Lewis, Connor
  • Journal of Electrochemical Energy Conversion and Storage, Vol. 14, Issue 2
  • DOI: 10.1115/1.4033411

Cationic Contamination Effects on Polymer Electrolyte Membrane Fuel Cell Performance
journal, January 2011

  • Kienitz, Brian; Pivovar, Bryan; Zawodzinski, Tom
  • Journal of The Electrochemical Society, Vol. 158, Issue 9
  • DOI: 10.1149/1.3610986

Intrinsic kinetic equation for oxygenreduction reaction in acidic media: the double Tafel slope and fuelcell applications
journal, January 2009

  • Wang, Jia X.; Uribe, Francisco A.; Springer, Thomas E.
  • Faraday Discuss., Vol. 140
  • DOI: 10.1039/B802218F

High performance aliphatic-heterocyclic benzyl-quaternary ammonium radiation-grafted anion-exchange membranes
journal, January 2016

  • Ponce-González, Julia; Whelligan, Daniel K.; Wang, Lianqin
  • Energy & Environmental Science, Vol. 9, Issue 12
  • DOI: 10.1039/C6EE01958G

Beyond catalysis and membranes: visualizing and solving the challenge of electrode water accumulation and flooding in AEMFCs
journal, January 2018

  • Omasta, Travis J.; Park, Andrew M.; LaManna, Jacob M.
  • Energy & Environmental Science, Vol. 11, Issue 3
  • DOI: 10.1039/C8EE00122G

Interplay between water uptake, ion interactions, and conductivity in an e-beam grafted poly(ethylene-co-tetrafluoroethylene) anion exchange membrane
journal, January 2015

  • Pandey, Tara P.; Maes, Ashley M.; Sarode, Himanshu N.
  • Physical Chemistry Chemical Physics, Vol. 17, Issue 6
  • DOI: 10.1039/C4CP05755D

Modeling Water Management and Carbon-Dioxide Contamination Effects in Anion-Exchange Membrane Fuel Cells
journal, July 2018

  • Gerhardt, Michael R.; Pant, Lalit M.; Shiau, Huai-Suen
  • ECS Transactions, Vol. 86, Issue 13
  • DOI: 10.1149/08613.0015ecst

A novel reference electrode for application in alkaline polymer electrolyte membrane fuel cells
journal, June 2010


Kinetic Equilibrium Study of CO 2 Poisoning Observed in Anion Exchange Membranes When Exposed to Ambient Air and Varying Levels of CO 2 ppm
journal, July 2018

  • Divekar, Ashutosh G.; Pivovar, Bryan S.; Herring, Andrew M.
  • ECS Transactions, Vol. 86, Issue 13
  • DOI: 10.1149/08613.0643ecst

Water Uptake and Ion Mobility in Cross-Linked Bis(terpyridine)ruthenium-Based Anion Exchange Membranes
journal, November 2013

  • Disabb-Miller, Melanie L.; Zha, Yongping; DeCarlo, Andrew J.
  • Macromolecules, Vol. 46, Issue 23
  • DOI: 10.1021/ma401701n

Anion Exchange Membrane and Ionomer for Alkaline Membrane Fuel Cells (AMFCs)
conference, January 2008

  • Yanagi, Hiroyuki; Fukuta, Kenji
  • 214th ECS Meeting, ECS Transactions
  • DOI: 10.1149/1.2981860

Anion-exchange membranes in electrochemical energy systems
journal, January 2014

  • Varcoe, John R.; Atanassov, Plamen; Dekel, Dario R.
  • Energy & Environmental Science, Vol. 7, Issue 10, p. 3135-3191
  • DOI: 10.1039/C4EE01303D

Effects of Carbon Dioxide on the Performance of Anion-Exchange Membrane Fuel Cells
journal, January 2011


Anion exchange membrane fuel cells: Current status and remaining challenges
journal, January 2018


The Effect of Ambient Carbon Dioxide on Anion-Exchange Membrane Fuel Cells
journal, March 2018


High-Performance Hydroxide Exchange Membrane Fuel Cells through Optimization of Relative Humidity, Backpressure and Catalyst Selection
journal, January 2019

  • Wang, Teng; Shi, Lin; Wang, Junhua
  • Journal of The Electrochemical Society, Vol. 166, Issue 7
  • DOI: 10.1149/2.0361907jes

Effect of Elevated Temperature and Reduced Relative Humidity on ORR Kinetics for PEM Fuel Cells
journal, January 2005

  • Xu, Hui; Song, Ying; Kunz, H. Russell
  • Journal of The Electrochemical Society, Vol. 152, Issue 9
  • DOI: 10.1149/1.1984351

A feasibility analysis for alkaline membrane direct methanol fuel cell: thermodynamic disadvantages versus kinetic advantages
journal, August 2003


Ammonia Contamination of a Proton Exchange Membrane Fuel Cell
journal, January 2018

  • Gomez, Yasna Acevedo; Oyarce, Alejandro; Lindbergh, Göran
  • Journal of The Electrochemical Society, Vol. 165, Issue 3
  • DOI: 10.1149/2.0761803jes

Activity targets for nanostructured platinum-group-metal-free catalysts in hydroxide exchange membrane fuel cells
journal, December 2016

  • Setzler, Brian P.; Zhuang, Zhongbin; Wittkopf, Jarrid A.
  • Nature Nanotechnology, Vol. 11, Issue 12
  • DOI: 10.1038/nnano.2016.265

Anion Exchange Membrane Ionic Conductivity in the Presence of Carbon Dioxide under Fuel Cell Operating Conditions
journal, January 2017

  • Wrubel, Jacob A.; Peracchio, Aldo A.; Cassenti, Brice N.
  • Journal of The Electrochemical Society, Vol. 164, Issue 12
  • DOI: 10.1149/2.0331712jes

Rational design of polyaromatic ionomers for alkaline membrane fuel cells with >1 W cm −2 power density
journal, January 2018

  • Maurya, Sandip; Noh, Sangtaik; Matanovic, Ivana
  • Energy & Environmental Science, Vol. 11, Issue 11
  • DOI: 10.1039/C8EE02192A

Works referencing / citing this record:

In-depth understanding of the CO 2 limitation of air fed anion exchange membrane fuel cells
journal, January 2020

  • Divekar, Ashutosh G.; Yang-Neyerlin, Ami C.; Antunes, Christopher M.
  • Sustainable Energy & Fuels, Vol. 4, Issue 4
  • DOI: 10.1039/c9se01212e

Predicting the Effects of Carbon Dioxide on the Conductivity of Electrospun Anion Exchange Membranes
journal, January 2019

  • Wrubel, Jacob A.; Peracchio, Aldo A.; Cassenti, Brice N.
  • Journal of The Electrochemical Society, Vol. 166, Issue 14
  • DOI: 10.1149/2.0481914jes

Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.