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Title: Operando X-ray tomography and sub-second radiography for characterizing transport in polymer electrolyte membrane electrolyzer

Abstract

Utilizing hydrogen gas as an energy carrier and enabling a hydrogen economy is a promising step towards decarbonization. Water electrolysis is a key process in hydrogen generation, but electrolyzers face a couple technological hurdles before widespread integration could occur. Understanding morphology evolution and transport processes in an operating polymer electrolyte membrane (PEM) electrolyzer is key to reducing cost and increasing efficiency. In this study, combined operando X-ray computed tomography and radiography are used to study transport and degradation in PEM electrolyzers subject to applied current densities. Tomography enables three-dimensional steady-state imaging but does not capture transport subtleties. Radiography is limited to two-dimensions but does capture transient phenomena. The tomography results depict degradation of the catalyst layer on the anode side of the electrolyzer. The rate of degradation was observed to increase as the applied current density increased. The catalyst particle detachment is due to autonomous propulsion during the oxygen evolution reaction. Particles that mechanically rip off the membrane were observed to be redeposited into the porous transport layer. During radiography, sub-second exposure time is required to capture the transient behavior of oxygen evolution, even at the lower current densities (50-200 mAcm-2). Various flow regimes were observed in the channel rangingmore » from bubbly to slug flow depending on current density. In conclusion, experimental observations agree with a model that an increase in current density increases oxygen bubble diameter and decreases bubble residence time within the electrolyzer channel.« less

Authors:
 [1];  [1];  [1];  [1];  [2];  [3];  [1]
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  1. Tufts Univ., Medford, MA (United States)
  2. Johns Hopkins Univ., Baltimore, MD (United States)
  3. Argonne National Lab. (ANL), Lemont, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
National Science Foundation (NSF); USDOE
OSTI Identifier:
1480988
Alternate Identifier(s):
OSTI ID: 1548459
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Electrochimica Acta
Additional Journal Information:
Journal Volume: 276; Journal Issue: C; Journal ID: ISSN 0013-4686
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; oxygen evolution reaction; polymer electrolyte membrane electrolyzer; radiography; two-phase flow; x-ray computed tomography

Citation Formats

Leonard, Emily, Shum, Andrew D., Normile, Stanley, Sabarirajan, Dinesh C., Yared, Dominic G., Xiao, Xianghui, and Zenyuk, Iryna V. Operando X-ray tomography and sub-second radiography for characterizing transport in polymer electrolyte membrane electrolyzer. United States: N. p., 2018. Web. doi:10.1016/j.electacta.2018.04.144.
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Leonard, Emily, Shum, Andrew D., Normile, Stanley, Sabarirajan, Dinesh C., Yared, Dominic G., Xiao, Xianghui, & Zenyuk, Iryna V. Operando X-ray tomography and sub-second radiography for characterizing transport in polymer electrolyte membrane electrolyzer. United States. https://doi.org/10.1016/j.electacta.2018.04.144
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Leonard, Emily, Shum, Andrew D., Normile, Stanley, Sabarirajan, Dinesh C., Yared, Dominic G., Xiao, Xianghui, and Zenyuk, Iryna V. Wed . "Operando X-ray tomography and sub-second radiography for characterizing transport in polymer electrolyte membrane electrolyzer". United States. https://doi.org/10.1016/j.electacta.2018.04.144. https://www.osti.gov/servlets/purl/1480988.
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@article{osti_1480988,
title = {Operando X-ray tomography and sub-second radiography for characterizing transport in polymer electrolyte membrane electrolyzer},
author = {Leonard, Emily and Shum, Andrew D. and Normile, Stanley and Sabarirajan, Dinesh C. and Yared, Dominic G. and Xiao, Xianghui and Zenyuk, Iryna V.},
abstractNote = {Utilizing hydrogen gas as an energy carrier and enabling a hydrogen economy is a promising step towards decarbonization. Water electrolysis is a key process in hydrogen generation, but electrolyzers face a couple technological hurdles before widespread integration could occur. Understanding morphology evolution and transport processes in an operating polymer electrolyte membrane (PEM) electrolyzer is key to reducing cost and increasing efficiency. In this study, combined operando X-ray computed tomography and radiography are used to study transport and degradation in PEM electrolyzers subject to applied current densities. Tomography enables three-dimensional steady-state imaging but does not capture transport subtleties. Radiography is limited to two-dimensions but does capture transient phenomena. The tomography results depict degradation of the catalyst layer on the anode side of the electrolyzer. The rate of degradation was observed to increase as the applied current density increased. The catalyst particle detachment is due to autonomous propulsion during the oxygen evolution reaction. Particles that mechanically rip off the membrane were observed to be redeposited into the porous transport layer. During radiography, sub-second exposure time is required to capture the transient behavior of oxygen evolution, even at the lower current densities (50-200 mAcm-2). Various flow regimes were observed in the channel ranging from bubbly to slug flow depending on current density. In conclusion, experimental observations agree with a model that an increase in current density increases oxygen bubble diameter and decreases bubble residence time within the electrolyzer channel.},
doi = {10.1016/j.electacta.2018.04.144},
journal = {Electrochimica Acta},
number = C,
volume = 276,
place = {United States},
year = {Wed Apr 25 00:00:00 EDT 2018},
month = {Wed Apr 25 00:00:00 EDT 2018}
}
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https://doi.org/10.1016/j.electacta.2018.04.144
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    Works referencing / citing this record:

    In Situ and Operando Characterization of Proton Exchange Membrane Fuel Cells
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    Polymer Electrolyte Water Electrolysis: Correlating Porous Transport Layer Structural Properties and Performance: Part I. Tomographic Analysis of Morphology and Topology
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