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Mass transport in a hydrogen gas diffusion electrode

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Abstract

Experimental data are presented concerning the diffusion-limited current density for hydrogen oxidation in a gas diffusion electrode (GDE) under various conditions. These current densities were obtained using mixtures of hydrogen and inert gases. To elucidate the dependence of the overall mass transport coefficient on the gas phase diffusion coefficient and the liquid phase diffusion coefficient of the hydrogen, a simplified model was derived to describe the transport of hydrogen in a GDE based on literature models. The GDE consists of a hydrophobic and a hydrophilic layer, namely a porous backing and a reaction layer. The model involves gas diffusion through the porous backing of the GDE combined with gas diffusion, gas dissolution and reaction in the reaction layer of the electrode. It was found that the transport rate of hydrogen under the experimental circumstances is determined by hydrogen gas diffusion in the pores of the porous backing, as well as in the macropores of the reaction layer. Diffusion of dissolved hydrogen in the micropores of the reaction layer, through the liquid, is shown to be of little significance.

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Abbreviations

A gd :

geometric electrode surface area (m2)

c in :

concentration of reactive component at the inlet of the gas compartment (mol m−3)

c out :

concentration of reactive component in and at the outlet of the gas compartment (mol m−3)

C SA :

concentration of sulphuric acid in the solution compartment (mol m−3)

c :

concentration of reactive component in a gas diffusion electrode (mol m−3)

D i,j (T):

interdiffusion coefficient for gas i in gas j at a temperature T (m2 s−1)

D 1 :

diffusion coefficient for electroactive species in solution (m2 s−1)

E :

electrode potential (V)

E e :

equilibrium electrode potential (V)

E t :

upper limit electrode potential (V)

F v,in :

volumetric flow rate at the inlet of the gas compartment (m3 s−1)

F v,N :

volumetric flow rate of nitrogen at the inlet of the gas compartment (m−3 s−1)

F m, in :

mass flow rate at the inlet of the gas compartment (kg s−1)

F :

Faraday constant (A s mol−1)

H :

Henry's constant defined by Equation 9 (−)

i gd,l :

diffusion limited current density for gas diffusion electrode (A m−2)

i gd,l,calc :

calculated diffusion limited current density for gas diffusion electrode (A m−2)

i 3 :

local current density for hydrogen oxidation reaction in a micropore of the gas diffusion electrode (A m−2)

I hp :

current for hydrogen production (A)

k 2 :

effective rate constant of gas transport into micropores of gas diffusion electrode per unit of macropore surface (m s−1)

k 3 :

electrochemical rate constant of the hydrogen oxidation reaction (m s−1)

k s :

mass transport coefficient (m s−1)

L :

effective length of a pore (m)

M :

effective pore concentration per unit of geometric electrode surface area (m−2)

N :

hydrogen flux (mol s−1)

n :

number of electrons involved in the electrode reaction

r :

effective pore radius (m)

S :

effective cross-sectional pore area, πr 2 (m2)

T :

temperature (K)

V m :

molar volume of gas (m3 mol−1)

α:

Bunsen coefficient (−)

η:

overpotential (V)

1:

the gas-filled macropores of the porous backing

2:

the gas-filled macropores of the reaction layer

3:

the solution-filled micropores of the reaction layer

1,2:

at the mouth of the macropores of the reaction layer at the interface of macropores of the porous backing and the macropores of the reaction layer

2,3:

at the mouth of a micropore in the reaction layer at the interface of macro and micropore in the reaction layer

G:

gas phase

L:

liquid phase

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Authors and Affiliations

  1. Faculty of Chemical Engineering, Laboratory of Instrumental Analysis, Eindhoven University of Technology, P.O. Box 513, 5600 MB, Eindhoven, The Netherlands

    J. J. T. T. Vermeijlen & L. J. J. Janssen

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  1. J. J. T. T. Vermeijlen
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  2. L. J. J. Janssen
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Vermeijlen, J.J.T.T., Janssen, L.J.J. Mass transport in a hydrogen gas diffusion electrode. J Appl Electrochem 23, 1237–1243 (1993). https://doi.org/10.1007/BF00234806

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