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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), Transportation Office. 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. https://doi.org/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 = {2019},
month = {9}
}

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

Citation Metrics:
Cited by: 11 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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      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.