Numerical Investigations on Ethanol Electrolysis for Production of Pure Hydrogen From Renewable...

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Numerical investigations on ethanol electrolysis for production of pure

hydrogen from renewable sources

S. Mohsen Mousavi Ehteshami a,⇑, S. Vignesh b, R.K.A. Rasheed b, S.H. Chan a

a Energy Research Institute at Nanyang Technological University, Singaporeb School of Mechanical and Aerospace Engineering, Nanyang Technological University, Singapore

h i g h l i g h t s

Ethanol electrolysis process to produce hydrogen was investigated numerically.

The model considers the transport phenomena and electrochemical reactions in the cell.

Reasonable agreement was found between the experimental data and numerical results.

Optimal operating potential for the electrolytic cell is proposed to be 0.94 V.

a r t i c l e i n f o

Article history:

Received 16 September 2015

Received in revised form 10 January 2016

Accepted 2 March 2016

Available online 11 March 2016

Keywords:

EthanolElectrolysis

Hydrogen production

Fuel cell

a b s t r a c t

Hydrogen and fuel cells have the potential to play a significant role in the energy-mix network and pro-

viding a more sustainable future. Hydrogen is mainly produced from steam-reforming of natural gas and

water electrolysis. However, it is suspected that the production of hydrogen through the electrolysis of

ethanol is more energy efficient and more environmentally friendly. In this study, to gain a good insight

of ethanol electrolysis process, we have investigated the ethanol electrolysis in a polymer electrolyte

membrane (PEM) reactor numerically. A two-dimensional, isothermal, and single phase ethanol elec-

trolyzer numerical model, taking into account the transport phenomena and electrochemical reactions,

has been developed for such purpose. Besides, a systematic parametric study is carried out to elucidate

the effect of operating temperature, flow rate and the thickness of the membrane on the performance of

the electrolytic cell. A reasonable agreement is found between the numerical data and the experimental

results available in the literature indicating the predictive capability of the model.

2016 Elsevier Ltd. All rights reserved.

1. Introduction

The significant growth of demand for clean energy has moti-

vated scientists in the field of energy science to pursue alternative

methods for power generation [1–7]. Hydrogen has been consid-

ered as a promising energy carrier as it possesses substantial

energy density. Moreover, hydrogen is environmentally friendly

and certainly can contribute to a clean and sustainable environ-

ment [8–11]. There are several ways to produce hydrogen, prefer-

ably from renewable energy sources. Currently, steam reforming of

hydrocarbons or alcohols is widely used for the mass production of

hydrogen [12–17]. Nevertheless, there is a desire to develop

renewable hydrogen production technologies. Hence, electrolysis

has been explored as a potential method to produce hydrogen

because the energy input to the electrolysis process can be derived

from renewable energy sources [12]. In recent years, various stud-

ies have been conducted on the electrolysis of water as a source of

pure hydrogen production [18–23]. However, the amount of

energy required for the water electrolysis is significantly higher.

The theoretical cell potential for hydrogen evolution through water

electrolysis process is 1.229 V. Therefore, the electrolysis of alter-

native liquids like alcohols has been explored to reduce the

amount of energy needed [24,25]. Moreover, the electrolysis of

alcohols can be considered environmentally friendly if bio-

alcohol is used as the fuel [11,26]. There are several studies done

on hydrogen generation through methanol electrolysis [27–29].

However, methanol is very toxic in nature. Among all the other

alcohols, ethanol is a suitable candidate for transportation and sta-

tionary applications, due to its high energy density and non-

toxicity compared with methanol. The energy densities of ethanol

and methanol (LHV) are 29 MJ/kg and 19.7 MJ/kg, respectively.

http://dx.doi.org/10.1016/j.apenergy.2016.03.001

0306-2619/ 2016 Elsevier Ltd. All rights reserved.

⇑ Corresponding author at: 50 Nanyang Ave, Singapore 639798, Singapore. Tel.:

+65 90386261; fax: +65 6694 6217.

E-mail addresses: [email protected], [email protected]

(S.M.M. Ehteshami).

Applied Energy 170 (2016) 388–393

Contents lists available at ScienceDirect

Applied Energy

j o u r n a l h o m e p a g e : w w w . e l s e v i e r . c o m / l o c a t e / a p e n e r g y

http://dx.doi.org/10.1016/j.apenergy.2016.03.001mailto:[email protected]:[email protected]:[email protected]://dx.doi.org/10.1016/j.apenergy.2016.03.001http://www.sciencedirect.com/science/journal/03062619http://www.elsevier.com/locate/apenergyhttp://www.elsevier.com/locate/apenergyhttp://www.sciencedirect.com/science/journal/03062619http://dx.doi.org/10.1016/j.apenergy.2016.03.001mailto:[email protected]:[email protected]://dx.doi.org/10.1016/j.apenergy.2016.03.001http://crossmark.crossref.org/dialog/?doi=10.1016/j.apenergy.2016.03.001&domain=pdf


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Moreover, huge potential for easy production of ethanol through

fermentation of sugar-containing materials [30] inspired us to

choose ethanol electrolysis.

The two half-cell reactions of the electrochemical reforming of

ethanol are presented in Eq. (1).

a: CH3CH2OH þ 3H2O ! 2CO2 þ 12Hþ þ 12e

b: 2Hþ þ 2e ! H2ð1Þ

with DH = +348 kJ/mole ethanol and DG = +96.9 kJ/mole ethanol.

The number of electrons transferred during the reaction is 12.

Hence, the theoretical cell voltage for ethanol electrolysis, obtained

from the Gibbs free energy equation E EtOH = DG/n, has become

0.08 V. This leads to less energy requirement compared to waterelectrolysis resulting in higher energy efficiency.

All the studies performed in the past on electrolysis of ethanol

for hydrogen production have been purely experimental in nature

[31]. To-date, there is no mathematical modeling study on ethanol

electrolysis found in the literature. This is, perhaps, the first com-

putational fluid dynamics study on the ethanol electrolysis based

on PEM electrolytic cell. This study formulates an isothermal,

two-dimensional and single phase model of the electrolysis of

ethanol with detailed process of flow of the water–ethanol solu-

tion, electrochemical reactions and species transport within the

electrolytic cell. Furthermore, the effect of the feedstock flow rate

and operating voltage on the species composition and cell perfor-

mance is studied and discussed.

2. Theory

The two-dimensional schematic of a PEM ethanol electrolyzer

and the computational domain are shown in Fig. 1. The electrolyzer

cell includes anode and cathode flow channels of straight type,

anode and cathode electrodes and an electrolyte, which is sand-

wiched by the electrodes. Pt/C is considered to be the electrocata-

lysts used. Water–ethanol mixture is supplied to the anode side

and hydrogen is generated in the cathode compartment. Ethanol

molecules are oxidized in the presence of water molecules into car-

bon dioxide and protons as presented in Eq. (1). Twelve electrons

are involved in this electrochemical reaction. The electrons react

with protons transported through the membrane and generate

hydrogen at the cathode catalyst layer. The generated hydrogenmolecules diffuse out of the cathode electrode to the cathode flow

channel. CO2 molecules produced at the anode side are transported

out by the residual ethanol solution stream. The crossover of the

ethanol molecules from the anode side to the cathode may also

take place. Ethanol molecules transported to the cathode side are

oxidized at the cathode. The current produced due to the oxidation

of ethanol at the cathode side is considered as the parasitic current

(i p). When this occurs, there is a mixed potential at the cathode due

to concurrent oxidation and reduction processes.

Because the flows in the channels of a PEM electrolyzer have

small Reynolds number, they are assumed to be in laminar regime.

In addition, the steady state condition is considered for the compu-

tational fluid dynamics model. The charge balance is solved in the

electrodes and the membrane with Eqs. (2) and (3), respectively.

r rseff rus

¼ 0 ð2Þ

r ðrmrumÞ ¼ 0 ð3Þ

where rseff , us, rm, and um are the electric conductivity and the

potential of the porous electrodes and the membrane, respectively.

The membrane conductivity is a function of thewater content of the

membrane k, i.e., the concentration ratio of water to sulfonic acid

group in the membrane. The following experimental expression

for the conductivity of Nafion membrane has been presented by

Springer et al. [32].

r30 ¼ 0:5139k 0:326; for k > 1 ð4Þ

where r30 and k are the membrane conductivity in S m1 (mea-

sured at 30 C) and water content of the membrane, respectively.The conductivity at any given operating temperature can be calcu-

lated using Eq. (5).

rm ¼ exp 1268 1

303

1

T

r30 ð5Þ

The flow in the porous media of the gas diffusion layers of the PEM

fuel cell is modeled by Darcy’s law (Eq. (6)), where the pressure gra-

dient is the driving force.

r p ¼ lju þ

le

r2u ð6Þ

where u, k p, l, e, and p are the velocity vector, permeability of theporous media, viscosity of the fluid, porosity and pressure, respec-

tively. The governing equations and the boundary conditions aresummarized in Fig. 1b. The boundary condition for the mass and

Nomenclature

D diffusivity (m2 s1)E standard electrode potential (V)F Faraday constant (96,487 C mol1)i current density (A cm2)LHV low heating value

M molar mass (kg mol1)n molar flux (mol s1)P pressure (Pa)Q electrical power (J s1)T temperature (K)u velocity vector (m s1)V specific rate of generation/consumption

Greek charactersr conductivity (S m1)u potential (V)e porosityg over-potential (V)

k membrane water contentl viscosity (kg m1 s1)q density (kg m3)x weight fractionc efficiency

Subscripts and superscriptsa anodeact activationcath cathodeE ethanoleff effectivem membrane p parasitics gas distribution electrode

S. Mohsen Mousavi Ehteshami et al./ Applied Energy 170 (2016) 388–393 389

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species at the anode membrane/catalyst layer interface are pre-

sented in Eqs. (7) and (8).

quE ¼

i

12F M H2O þ M E M CO2ð Þ nH2O nE ð7Þ

quxE qDE @ xE @ y

¼ i þ i p12F

M E ð8Þ

where the fluxes of ethanol and water through the membrane and i pare calculated by Eqs. (9)–(11), respectively.

nE ¼iM E F aH2OxE þ

qDE xE xcathE t mem

ð9Þ

nH2O ¼iM H2OF aH2O ð10Þ

i p ¼ 12FnE M E ð11Þ

The parameters used in the simulation of ethanol PEM electrolyzer

are presented in Table 1. The relationship between the current den-

sity and the cell potential are studied combining the electrochemi-

cal and computational fluid dynamics. The electrochemical

potential of the PEM ethanol electrolyzer can be calculated by Eq.

(12).

V ¼ E þ gohmic þ gact ;a þ gact ; ð12Þ

where E , gohmic , gact ,a and gact ,c are the equilibrium potential, theohmic overpotential, the anode activation overpotential and the

cathode overpotential, respectively. The activation overpotentials

are dependent on the kinetics of the reactions at the anode and

cathode electrodes. The relationship between the cell overpoten-

tials and current density are expressed by Butler–Volmer equation

[33]. The ohmic overpotential, representing the potential loss due

to electrons and ions transport, is calculated using Ohm’s law.

3. Numerical method

The governing equations are solved numerically using finite ele-

ment method. There is coupling between the flow velocity and the

species transport and current distribution modules. Once the

velocity field is obtained, the species transport and current distri-

bution equations are solved. The former determines the concentra-

tion of species at different components of the cell. The fluid

properties including density, thermal conductivity and diffusivityare updated according to the calculated compositions at each iter-

(a)

Ethanol-water solution

y

sedor tcelE

x

Hydrogen

(b)

p=pref

= − =

Anode Channel

= 0

Anode electrode

∇

= 0

membrane Cathode electrode

∇

= 0

Cathode Channel

= 0

p=pref

Membrane

Cathode channel

Anode channel

Fig. 1. (a) The schematic of the electrolyzer cell. (b) The computational domain and governing transport phenomena equations and boundary conditions.

Table 1

Properties and geometric parameters.

Parameter (unit) Value Ref.

Temperature (K) 303 –

Pressure (atm) 1 –

Length of the anode/cathode channels (cm) 2 –

Ethanol solution flow rate (ml min1) 5 –

Ethanol molar concentration at the inlet (M) 6 –

Thickness of the diffusion layer (cm) 0.03 –

Thickness of the membrane (cm) 0.0183 –

GDL permeability (m2) 1.76 1011 –

Ethanol diffusion coefficient (m2 s1) 0.84 109 [28]

Porosity 0.7 –

Faraday constant (A s mol1) 96,485 –

Ethanol viscosity at 25 C (MPa s) 1.082 [29]

Ethanol density (kg m3) 789 –

Universal gas constant (J K1 mol1) 8.314 –

Hydrogen density at stp (kg m3) 898 –

Electro-osmosis water transport coefficient 0.25 [30]

Hydrogen viscosity (MPa s) 0.009 –

390 S. Mohsen Mousavi Ehteshami et al. / Applied Energy 170 (2016) 388–393


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ation. It should be reminded that the local current density values

obtained from current distribution module are used as the source

terms in other modules. The iterations are continued till conver-

gence is reached for the governing equations. The ethanol elec-

trolyzer model was developed and solved using COMSOL

multiphysics. The grid independency has been checked in this

study. It was concluded that the results do not change remarkably

when the number of mesh elements is more than 14,000.

4. Results and discussion

4.1. Model validation

To validate the numerical model, the results obtained from the

modeling are compared with the experimental data obtained from

the literature [31] under the same conditions. The simulations are

carried out at 20 C and atmospheric pressure. The flow rate of

ethanol mixture is 2 ml min1. Fig. 2 presents the numerical results

compared with the experimental data obtained from [31]. It can be

seen that there is a reasonable agreement between the experimen-

tal data and simulation results. The discrepancy between the sim-

ulation and experimental data is more obvious in the high current

density end. This could be due to the mass transport losses in the

presence of carbon dioxide bubbles generated in the anode side.

The dynamic of carbon dioxide bubbles is not taken into account

in the simulation study.

Fig. 3 shows the local current density distribution in the ethanol

electrolyzer operating at potentials of 0.8 V and 1 V. It can be seen

that the current density increases along the electrode length with

the increase in operating potential. Also, the local current density

decreases along the cell length. This is due to the consumption of

ethanol and formation of products (protons and carbon dioxide)

according to Eq. (1). It should be noted that Eq. (1) is the ideal etha-

nol oxidation reaction. In practice, it has been found, evidenced

with in situ infrared spectroscopy and chromatography analysis,

that ethanol oxidation in this potential domain produced mainlyacetaldehyde (2H+) and acetic acid (4H+) [34,35].

The effect of inlet flow rate on the local current density distribu-

tions at operating potential of 1 V is presented in Fig. 4. In the case

of different inlet flow rates, the local current densities along the

electrode length do not show any remarkable differences. The local

current density, at higher inlet flow rate, decreases less signifi-

cantly along the cell length compared to that of lower inlet flow

rate.

Fig. 5 presents the ethanol mass fraction along the electrode

length over diffusion layer/catalyst layer interface for ethanol inlet

velocities of 0.005 m/s, 0.01 m/s, 0.03 m/s and 0.05 m/s. The mass

fraction drop increases with decreasing the inlet velocity. This is

due to higher consumption of ethanol at a lower velocity since

the detention time of the ethanol would be higher at a lower inlet

flow velocity.

Current density/ (A.cm-2)

0.00 0.02 0.04 0.06 0.08 0.10 0.12 0.14

P o t e n t i a l / V

0.3

0.4

0.5

0.6

0.7

0.8

0.9

1.0

1.1

ExperimentalSimulation

Fig. 2. Comparison of the predicted polarization curve and the experimental datafrom [31].

Position on the length of the cell/ m

0.000 0.005 0.010 0.015 0.020

L o c a l c u r r e

n t d e n s i t y / ( A . m

- 2 )

0

200

400

600

800

1000

1200

1 V0.8 V

Fig. 3. Distribution of local current density along the cell length.


0.000 0.005 0.010 0.015 0.020

L o c a l c u r r e n t d e n s i t y / ( A . m

- 2 )

0

200

400

600

800

1000

3 ml.min-1-1

2 ml.min-1

Fig. 4. The effect of inlet flow rate on the local current density distributions at

operating potential of 1 V.


0.000 0.005 0.010 0.015 0.020 E t O H m

a s s f r a c t i o n a l o n g t h e c a t a l y s t

l a y e r a x i s

0.00

0.01

0.02

0.03

...... 0.05 m/s _ _ _0.01 m/s

___ 0.005 m/s _ . _ . 0.03 m/s

Fig. 5. The ethanol mass fraction along the diffusion layer-catalyst layer interface

for ethanol inlet velocities of 0.005 m/s, 0.01 m/s, 0.03m/s and 0.05m/s.

S. Mohsen Mousavi Ehteshami et al. / Applied Energy 170 (2016) 388–393 391

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The effect of the operating temperature on the electrolyzer cellperformance is presented in Fig. 6. Apparently, the increase in the

operating temperature improves the performance of the cell. It can

be seen that the activation overpotential reduces at higher temper-

atures, which is due to the improvement of reaction kinetics at

higher temperatures.

The impact of membrane thickness on the electrolyzer perfor-

mance was studied using three different thickness; Nafion 112

(0.076 mm thickness), Nafion 115 (0.127 mm thickness), and

Nafion 117 (0.174 mm thickness). From Fig. 7, the cell performance

is found to follow the order: Nafion 117 > Nafion 115 > Nafion 112.

The shapes of the polarization curves imply that the surface resis-

tances corresponding to the three membranes used are close to

each other. The difference in the performance is mainly due to

the fact that thicker membranes reduce the ethanol crossover

and, thereby reducing the parasitic losses and improving the cell

performance. In other words, the parasitic loss due to ethanol

crossover outnumbers the effect of reduced ohmic loss with thin-

ner membrane. It is observed that there is a remarkable gap in per-

formance between of the cell made of Nafion 115 and that of

Nafion 117. Applying Nafion 117 brings about a significant differ-

ence in the cell performance as compared to Nafion 115.

The rate of hydrogen generation and the productivity ratio

defined by Eq. (13) are presented in Fig. 8.

c ¼ V H2 LHV

Q þ V E LHVE ð13Þ

where V H2, V Et , Q , LHVH2, and LHVEt are the specific hydrogen gener-ation/ethanol consumption rates (m3 s1 cm2), electrical power

consumption (kJ s1), the low heating value of hydrogen at standard

conditions (10,218 kJ m3), and heating value of ethanol

(21,560 kJ m3), respectively. The specific hydrogen generation rate

is the rate of the hydrogen generation per unit area of the elec-

trolyzer cell. The energy consumption for the electrolysis process

Q is calculated by multiplying the applied potential by the current

produced. The specific rate of hydrogen generation (calculated from

the simulation results) and the productivity ratio are plotted versus

the operating potential of the electrolytic cell operating at room

temperature in Fig. 8. The membrane is considered to be Nafion

117. It can be seen that the productivity ratio increases with the

increase in operating potential. However, it flattens at operating

potential about 0.8 V. On the other hand, the specific rate of hydro-gen generation strictly increases with the increase of the operating

potential. The operating potential of 0.94 V is considered to be the

optimum cell potential leading to reasonable productivity rate

and specific hydrogen generation rate of 1.5 cm3 min1 cm2. At

potentials higher than 0.94 V, the hydrogen generation rate

increases, while the productivity ratio does not improve and it is

almost fixed at 1.48. This also should be noted that, practically,

there is a potential limit over which the membrane electrode

assembly may detach.

5. Conclusion

Computational fluid dynamics simulation of ethanol electrolytic

cell has been carried out using finite element method. The modeldeveloped is the first numerical investigation of such electrolysis

process. The simulation leads to a better understanding of the phe-

nomena which occur in the ethanol electrolytic cell. The model is

able to predict the polarization (current–potential) behavior of

the cell, and also the current density and species distribution along

the cell at different operating conditions. The simulation results are

in reasonably good agreement with the experimental data avail-

able in the literature, especially in the low current density range.

It was found out that: (1) the cell current density increases with

increase in the operating potential; (2) the local current density

decreases along the cell length; (3) the increase in the operating

temperature improves the performance of the cell; (4) in the case

of different inlet flow rates, the local current densities do not show

any remarkable difference; (5) the cell performance was found tofollow the order: Nafion 117 > Nafion 115 > Nafion 112, which is

Current density/ (A.cm-2

)

0.00 0.02 0.04 0.06 0.08 0.10 0.12 0.14 0.16


0.3

0.4

0.5

0.6

0.7

0.8

0.9

1.0

20 °C40 °C60 °C80 °C

Fig. 6. The effect of operating temperature on the performance of the electrolyzer

cell. The ethanol–water solution with concentration of 2 M is fed to the cell at

2 ml min1.

Current density/ (A.cm-2

)

0.00 0.02 0.04 0.06 0.08 0.10 0.12 0.14


0.2

0.4

0.6

0.8

1.0

1.2

Nafion 117

Nafion 115

Nafion 112

Fig. 7. Comparison of the performance of the electrolyzer cell with differentmembranes at room temperature.

Potential/ V

0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0

P r o d u

c t i v i t y r a t i o (

)

0.8

0.9

1.0

1.1

1.2

1.3

1.4

1.5

1.6

H y d r o g e n g e n e r a t i o n r a t e / c m

3 . s

- 1

0.0

2.0e-6

4.0e-6

6.0e-6

8.0e-6

1.0e-5

1.2e-5

1.4e-5

1.6e-5

1.8e-5

γ

Vgen η

Fig. 8. The rate of hydrogen generation and the productivity ratio vs the operating

potential of the cell at room temperature.

392 S. Mohsen Mousavi Ehteshami et al. / Applied Energy 170 (2016) 388–393


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due to the fact that thicker membranes reduce the ethanol cross-

over and, thereby reducing the parasitic losses thus improving

the cell performance; (6) the productivity ratio increases with

the increase in operating potential, however, it flattens at operat-

ing potential of about 0.8 V. On the other hand, the specific rate

of hydrogen generation strictly increases with the increase of the

operating potential. (7) For the cell with Nafion 117 as the mem-

brane, the operating potential of 0.94 V is seem to be the optimum

cell potential leading to reasonable productivity rate and specific

hydrogen generation rate of 1.5 cm3 min1 cm2.

Acknowledgement

The authors wish to gratefully acknowledge the Energy

Research Institute at NTU (ERI@N) for supporting this research

work financially.

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