Impact of iron and hydrogen peroxide on membrane degradation for polymer electrolyte membrane water electrolysis: Computational and experimental investigation on fluoride emission

Steffen Henrik Frensch, Guillaume Serre, Frédéric Fouda-Onana, Henriette Casper Jensen, Morten Lykkegaard Christensen, Samuel Simon Araya, Søren Knudsen Kær

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Resumé

Polymer electrolyte membrane (PEM) degradation in electrolysis mode is simulated through a Fenton model that includes all major involved electrochemical reactions. Supportive experimental investigations on the effect of hydrogen peroxide and iron impurities are carried out in an ex-situ set-up, where the results are utilized to fit model parameters. The experiments reveal a high dependence of fluoride emission on iron concentration, which catalyzes the reaction, and identifies hydrogen peroxide as a necessary precursor for destructive hydroxyl radical formation. Simulations of in-situ operation reveal that elevated current is favorable in terms of lower fluoride emission, as the radicals are depleted by side reactions. Temperatures above 80∘C significantly accelerate membrane thinning, where the step from 80∘C to 90∘C more than doubles thinning after 500 h.
OriginalsprogEngelsk
TidsskriftJournal of Power Sources
Vol/bind420
Sider (fra-til)54-62
Antal sider8
ISSN0378-7753
DOI
StatusUdgivet - apr. 2019

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peroxides
electrolysis
hydrogen peroxide
Fluorides
Electrolysis
Hydrogen peroxide
Hydrogen Peroxide
Electrolytes
fluorides
Polymers
Iron
electrolytes
degradation
membranes
Membranes
iron
Degradation
Water
polymers
Hydroxyl Radical

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title = "Impact of iron and hydrogen peroxide on membrane degradation for polymer electrolyte membrane water electrolysis: Computational and experimental investigation on fluoride emission",
abstract = "Polymer electrolyte membrane (PEM) degradation in electrolysis mode is simulated through a Fenton model that includes all major involved electrochemical reactions. Supportive experimental investigations on the effect of hydrogen peroxide and iron impurities are carried out in an ex-situ set-up, where the results are utilized to fit model parameters. The experiments reveal a high dependence of fluoride emission on iron concentration, which catalyzes the reaction, and identifies hydrogen peroxide as a necessary precursor for destructive hydroxyl radical formation. Simulations of in-situ operation reveal that elevated current is favorable in terms of lower fluoride emission, as the radicals are depleted by side reactions. Temperatures above 80∘C significantly accelerate membrane thinning, where the step from 80∘C to 90∘C more than doubles thinning after 500 h.",
keywords = "PEM water electrolysis aging, Membrane degradation modelling, Fenton reaction model, Hydrogen Peroxide, Fluoride emission rate",
author = "Frensch, {Steffen Henrik} and Guillaume Serre and Fr{\'e}d{\'e}ric Fouda-Onana and Jensen, {Henriette Casper} and Christensen, {Morten Lykkegaard} and {Simon Araya}, Samuel and K{\ae}r, {S{\o}ren Knudsen}",
year = "2019",
month = "4",
doi = "10.1016/j.jpowsour.2019.02.076",
language = "English",
volume = "420",
pages = "54--62",
journal = "Journal of Power Sources",
issn = "0378-7753",
publisher = "Elsevier",

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TY - JOUR

T1 - Impact of iron and hydrogen peroxide on membrane degradation for polymer electrolyte membrane water electrolysis: Computational and experimental investigation on fluoride emission

AU - Frensch, Steffen Henrik

AU - Serre, Guillaume

AU - Fouda-Onana, Frédéric

AU - Jensen, Henriette Casper

AU - Christensen, Morten Lykkegaard

AU - Simon Araya, Samuel

AU - Kær, Søren Knudsen

PY - 2019/4

Y1 - 2019/4

N2 - Polymer electrolyte membrane (PEM) degradation in electrolysis mode is simulated through a Fenton model that includes all major involved electrochemical reactions. Supportive experimental investigations on the effect of hydrogen peroxide and iron impurities are carried out in an ex-situ set-up, where the results are utilized to fit model parameters. The experiments reveal a high dependence of fluoride emission on iron concentration, which catalyzes the reaction, and identifies hydrogen peroxide as a necessary precursor for destructive hydroxyl radical formation. Simulations of in-situ operation reveal that elevated current is favorable in terms of lower fluoride emission, as the radicals are depleted by side reactions. Temperatures above 80∘C significantly accelerate membrane thinning, where the step from 80∘C to 90∘C more than doubles thinning after 500 h.

AB - Polymer electrolyte membrane (PEM) degradation in electrolysis mode is simulated through a Fenton model that includes all major involved electrochemical reactions. Supportive experimental investigations on the effect of hydrogen peroxide and iron impurities are carried out in an ex-situ set-up, where the results are utilized to fit model parameters. The experiments reveal a high dependence of fluoride emission on iron concentration, which catalyzes the reaction, and identifies hydrogen peroxide as a necessary precursor for destructive hydroxyl radical formation. Simulations of in-situ operation reveal that elevated current is favorable in terms of lower fluoride emission, as the radicals are depleted by side reactions. Temperatures above 80∘C significantly accelerate membrane thinning, where the step from 80∘C to 90∘C more than doubles thinning after 500 h.

KW - PEM water electrolysis aging

KW - Membrane degradation modelling

KW - Fenton reaction model

KW - Hydrogen Peroxide

KW - Fluoride emission rate

U2 - 10.1016/j.jpowsour.2019.02.076

DO - 10.1016/j.jpowsour.2019.02.076

M3 - Journal article

VL - 420

SP - 54

EP - 62

JO - Journal of Power Sources

JF - Journal of Power Sources

SN - 0378-7753

ER -