Cost-effective design of the alkaline

electrolyser for enhanced electrochemical

performance and reduced electrode
degradation
..............................................................................................................................................................

Daniel Symes*, Bushra Al-Duri, Waldemar Bujalski and Aman Dhir

Centre for Hydrogen and Fuel Cell Research, School of Chemical Engineering, University of
Birmingham, B15 2TT, UK
.............................................................................................................................................
Abstract
An alkaline electrolyser was developed and characterized. Three different metals, working as the electrode,
were analysed using electrochemical methods to determine the best electrochemical performance. The
performance of the Stainless Steel (SS316) electrode and the nickel electrode is much better than that of
the conventional iron electrode. Degradation analysis of the electrode materials highlighted the need for
the material to be durable and resistant to corrosion from an alkaline environment. Through SEM and
mass analysis, it is shown that Nickel exhibits the strongest long-term resistance to surface and
electrochemical performance degradation, when compared with Mild Steel (Iron) and SS316.

Keywords: electrolyser; electrode degradation; electrolysis; water electrolysis; alkaline electrolyser

*Corresponding author:
[email protected] Received 4 July 2012; revised 2 November 2012; accepted 29 March 2013
................................................................................................................................................................................

1 INTRODUCTION
Approximately 94% of current hydrogen is obtained from
The global demand of energy is leading to the inevitable short- fossil fuels from a process called steam reforming. These pro-
age of fossil fuels, which is the primary resource for our energy cesses produce greenhouse gases and do not produce as high a
requirements. Fossil fuels are formed by the anaerobic decom- purity of hydrogen that water electrolysis produces [4].
position of dead organisms in the planet’s crust and are a finite Water electrolysis currently accounts for 4% of global hydro-
resource, which has led to increased research into new sources of gen production and involves the passing of an electrical current
energy. When they eventually become obsolete, we will have to through water-based solutions which produce hydrogen and
get our energy from other sources [1]. oxygen as the only products, therefore no greenhouse gas emis-
A shift in focus to the production of energy from renewable sions [5]. If the electricity supplied to the electrolysis cell comes
resources has increased the public awareness of potential energy from renewable resources, the whole process is carbon neutral,
shortcomings due to depleting fossil fuel resources. Hydrogen is i.e. no greenhouse gas emissions.
an effective energy carrier for renewable resources, and this Electrolysers use electrical current to split water into its consti-
energy can be extracted from hydrogen through fuel cells and in- tuents, and there are two main types of electrolysers, alkaline elec-
ternal combustion engines. Hydrogen can also be used for trolysers and polymer electrolyte membrane (PEM) electrolysers.
energy storage, for example, during off-peak hours, excess elec- Water has a very high electrical resistance and cannot be dir-
trical energy, instead of being wasted, could be stored in the ectly split into hydrogen and oxygen. This can only occur when
form of hydrogen via electrolysis [2]. extremely high electrical currents are applied to the system,
Many academics believe that the only realistic way to produce which is impractical. Therefore, the addition of an electrolyte
hydrogen without creating any greenhouse gases is through the lowers the electrical energy required to initiate the reaction [6].
use of renewable energy sources. These include solar, wind and Alkaline electrolysers use a liquid electrolyte in the form of an
hydro energy sources. It is important to remember that hydro- acid/base/salt to produce hydrogen, whereas PEM electrolysers
gen is an energy carrier, not a primary energy source [3]. use a solid polymer electrolyte in the form of a membrane to

International Journal of Low-Carbon Technologies 2015, 10, 452– 459

# The Author 2013. Published by Oxford University Press.
This is an Open Access article distributed under the terms of the Creative Commons Attribution Non-Commercial License (http://creativecommons.org/licenses/by-
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doi:10.1093/ijlct/ctt034 Advance Access Publication 27 May 2013 452
 Cost effective design of an alkaline electrolyser

split pure water into hydrogen and oxygen without the need for heat according to Ohm’s law. In water electrolysis, the forms of
any harmful acids/alkalis [7]. electrical resistance in the system are from the resistances in elec-
This work herein examines the potential for improving an trical circuits. The transfer of ions with the electrolyte depends
existing alkaline electrolyser from electrochemistry first princi- on the electrolyte concentration (if liquid), membrane (if solid)
ples by manipulating the electrodes. and separation distance between the cathode and the anode [11].
The presence of bubbles on the electrode surfaces creates resis-
tances to the ionic transfer and thus the electrochemical reaction.
2 THEORY The aims of this research are to increase mass transfer on the
electrode surface. This, however, could hinder the production rate
At standard temperature and pressure (S.T.P., 298 K, 1 atm), Gibbs of hydrogen. Increasing mass transfer on the electrodes will create a
free energy of formation is defined as a point of zero energy and is larger volume of bubble formation. This additional bubble forma-
used to calculate the change in energy of a system. The open- tion could reduce the contact area between the electrolyte and the
circuit voltage (minimum) potential required electrolysing water electrode and therefore limit the number of active sites available
into hydrogen and oxygen is determined by the change in Gibbs for nucleation. One way to minimize this effect is by the circulation
free energy of formation between reactants and products. Gibbs of electrolyte through the electrolyser. This mechanically removes
free energy changes with temperature and state (gas or liquid) [8]: bubbles from the electrode surface at a faster rate and therefore
DGo significantly reduce bubble overpotential in solution [12].
Eo ¼ ð1Þ At equilibrium (open cell voltage), there exists dynamic cur-
zF
rents, at each electrode and are a fundamental aspect of electrode
where Eo is the theoretical minimum reversible potential of an behaviour. They are known as the cathode and anode exchange
electrolysis cell, z the number of electrons transferred in the reac- current density, which can be defined as the rate of reduction
tion and F the Faraday number (96 485 Coulomb mol21). and oxidation, respectively. The exchange current density is a
At S.T.P., the Gibbs free energy of formation is quantification of an electrode ability to transfer electrons and
þ237.2 kJ mol21; therefore, Eo ¼ 1.23 V. This is the minimum occurs in both directions equally, resulting in no change in com-
potential required to split water and produce hydrogen and position of the electrode. When a small exchange current
oxygen. Under adiabatic conditions, the total enthalpy must be density exists, it represents slow reaction kinetics and a slow rate
provided by the electrical energy [9]. In this case, the thermo- of electron transfer. A large exchange current density symbolizes
neutral voltage is required to maintain the electrochemical reac- fast reaction kinetics and a fast rate of electron transfer [13].
tion without heat generation. For the electrochemical reaction to proceed on an electrodes
The actual potential (Ecell ) required to split water will require surface, an energy barrier must be overcome. This is the activation
Ecell to be greater than Eo. The difference is known as overpoten- energy and results in activation overpotential in electrochemical
tial, losses or polarization [10]. Thus, hydrogen evolution does reactions; these losses are irreversible. The activation overpotential
not occur at the reversible potential (1.23 V). These are resis- is the additional voltage required to overcome the energy barrier
tances in the cell that result in a higher potential being required of the rate determining the step of the electrochemical reaction to
to split water in order to overcome these resistances. a value at which the reaction will proceed at a suitable rate [13].
The electrical circuit analogy can be used to illustrate the
various resistances encountered during the electrolysis process
(Figure 1) [11]. 3 METHODS
There are three main types of resistance in the electrolysis
cell: electrical resistances, transport resistances and electrochem- Electrochemical overpotential analysis was completed using a
ical reaction resistances. These are shown below: simple experimental procedure as shown in Figure 2. The elec-
trodes of choice were placed 10 mm apart for each experiment,
Rcell ¼R1 þ R01 þ Rbubble;O2 þ Rbubble;H2 þ Rions keeping the ohmic resistance constant. The electrolyte concen-
ð2Þ
þ Rmembrane þ Ranode þ Rcathode tration was kept at 0.1 M KOH, maintaining the concentration
overpotential constant. Consequently, by varying the electrode
Electrical resistances (R1 and R01 ) directly result in heat gener- material, the only variation in electrochemical performance
ation which leads to the waste electrical energy in the form of would be a result of the activation overpotential. The potation

Figure 1. Electrical circuit analogy of water electrolysis [11].

International Journal of Low-Carbon Technologies 2015, 10, 452– 459 453

D. Symes et al.

difference across the plates was supplied by Thurlby Thandar production from the electrolyser without increasing the foot-
QPX1200L 1.2 kW. print (size) of the electrolyser (2000 cm3). Since the electrical
The following electrode materials were tested (Table 1). Gas input to the electrolyser would need to remain constant (12 V),
volume measurements were conducted using a gas syringe over a it was clear that the surface area of electrodes would need to in-
period of time to enable the volumetric flow rate to be calculated. crease. From redesigning the electrolyser, it has been possible to
Gas composition analysis was completed using a MKS instruments increase the surface area from 600 to 5000 cm2.
Minilab. Mass spectrometry (MS) is a measurement technique for The new electrolyser design takes into account the need for
the determination of the elemental composition of a molecule or no increase in footprint size and builds in the ability to hold up
compound. It is also used for interpreting the chemical structures to 24 electrode plates (100 mm  100 mm  1 mm), with a
of molecules. The MS principle consists of ionizing chemical com- 6-mm spacing between each plate. These 24 plates represent up
pounds to generate charged molecules or molecule fragments and to 12 electrolysis cells in the electrolyser stack.
the measurement of their mass-to-charge ratios (m/z) [13]. The casing was custom built out of Perspex (10 mm thick-
ness—for experimental purposes), which aided in bubble ana-
lysis into the reaction kinetics occurring in the electrolyser.
4 STACK DESIGN AND DEVELOPMENT Precision slots were machined, which allowed for ease of
removal and modification of each electrode. The plates were
From the defined project goals after analysis of the commercial connected in parallel using two stainless steel (SS316) bars
initial unit, an objective was to increase the rate of hydrogen (150 mm  20 mm  1 mm), which were connected to the elec-
trodes using SS316 screws.
At one end of each interconnect was an SS316 screw soldered
onto it for the electrical energy input to the electrolyser stack.
These were accompanied with two 3/800 ID nylon nozzles which
were placed symmetrically central in the electrolyser lid for the
connection of the stack to the electrolyte reservoir.
Figure 3 shows the design of the electrolyser with 6 mm sep-
aration distance between the electrodes. This small distance
should limit the quantity of ohmic resistance exhibited in the
electrolyser. No separator was used in the design of the electro-
lyser, since there is no requirement for the hydrogen and oxygen
gas to be separated for the end application. This enabled maxi-
mization of the electrode surface area in the electrolyser cell. The
constructed electrolyser is shown in Figure 4.

Figure 2. Experimental setup.

5 RESULTS
5.1 Material cost analysis
Table 1. Electrode materials and properties The electrochemical performance was plotted as a function of
Material Cost (metal exchange as Electrical resistivity in References material cost for each electrode material highlighted in Table 1.
of 21 October 2011) literature (208C) The results are shown in Figure 5.
Pt £31 400/kg 105 nV m [14– 17]
From calculating the decomposition potential for each elec-
(platinized) trode from their respective current – voltage curve and then plot-
Palladium £12 350/kg 105.4 nV m [14, 18] ting this as a function of the material cost, it can be seen that
Gold £34 144/kg 22.14 nV m [11, 19] cheaper metals such as zinc, iron and brass exhibit cost-effective
Iron £2.81/kg 96.1 nV m [13, 16] electrochemical behaviour.
Pt (shiny) £31 400/kg 105 nV m [14– 17]
Silver £717.83/kg 15.87 nV m [13, 16]
Nickel £17.40/kg 69.3 nV m [8, 20] 5.2 Current density analysis
Graphite £21.10/kg 7800 nV m [21– 23] Further material characterization was completed by applying a
Lead £4.05/kg 208 nV m [13]
SS316 £3.86/kg 100 nV m [16, 20]
potential of 12 V. From which the current per unit area (current
Magnesium £5.62/kg 43.9 nV m [11, 13] density) was calculated. The results are shown in Figure 6.
Titanium £11.95/kg 420 nV m [24] Figure 6 shows that silver exhibits the best electrical conduct-
Copper £4.13/kg 16.78 nV m [11, 13] ivity (within the material set selected) at 12 V. Silver, however, is
Aluminium £1.65/kg 28.2 nV m [16, 20] extremely expensive (Table 1) and is not economically viable for
Tin £17.17/kg 115 nV m [11, 16]
Zinc £1.18/kg 59 nV m [13]
a 1.2-kw electrolyser design. The next three materials which
exhibit good electrical conductivity are Iron (Mild Steel), Nickel

454 International Journal of Low-Carbon Technologies 2015, 10, 452–459

 Cost effective design of an alkaline electrolyser

Figure 3. CAD schematic of the electrolyser design.

Figure 4. Image of the constructed electrolyser.

Figure 5. Decomposition potential of electrode materials as a function of
and Stainless Steel (SS316). As well as having good conductivity, material cost.
all three materials have economical unit costs.
Two potential electrode materials, SS316 and nickel, were
selected for further stack testing and analysis. These were tested presented here. This does not take into account the surface area
in two modes, polished and unpolished. Unpolished was no of the electrodes, where in this case this analysis is carried out
surface treatment, and polished which had been treated with for 24 SS316 plates and 20 Nickel plates.
metal polish (Brasso). This drastic increase in current flow has been attributed to
the increase in the surface area of electrode (600 ! 5000 cm2).
To analyse this further, we can electrochemically characterize the
5.3 Stack analysis electrolyser stacks as a function of the electrode surface area
This was conducted for SS316 and Nickel plates. Figure 7 shows (current density). This is shown in Figure 8.
that for the same footprint there has been an increase in current Figure 8 shows a smaller enhancement in current density at a
flow for the same potential. At 4 V, there has been a 1500% in- fixed potential. At 4 V, there is a 267% increase in performance
crease from the commercial electrolyser to the improved design from the commercial electrolyser to the new design for both

International Journal of Low-Carbon Technologies 2015, 10, 452– 459 455

D. Symes et al.

Figure 8. Electrolyser current density comparison using 0.1 M KOH solution.

Figure 6. Current density of electrode materials at 12 V.

Figure 9. Electrolyser HHO production comparison at 0.1 M KOH solution.

Figure 7. Electrolyser current comparison using 0.1 M KOH solution.

the oxide layer of the electrode, resulting in the increase in the
electrode surface area for bubble nucleation. The increase in gas
electrode materials. This enhancement observed can be attribu- productivity from electrode surface polishing can also be attrib-
ted to the decrease in resistance in the electrolyser system. It is uted to oxide layer removal. Oxide layers increase resistance in
believed the reduction in resistance is a result of the smaller sep- the electrolyser, since it limits the number of active reaction sites
aration distance between the electrodes (reducing the ohmic re- available for bubble nucleation.
sistance), and the removal of ‘neutral’ plates in the electrolyser
which prevent short circuits, but increased the resistance in the
commercial electrolyser. 5.5 Current density vs. HHO production: Faraday’s
law of electrolysis
5.4 Gas productivity Current flow per unit surface area is directly proportional to the
The gas productivity of the electrolysers was also analysed. It is rate of gas evolution. This is Faraday’s first law of electrolysis.
known that gas production rates are directly proportional to Figure 10 shows this relationship as recorded from the improved
current flow according to Faraday’s first law of electrolysis. electrolyser, for both electrode materials and surface characteristics.
Consequently, the gas production rate increases with an increas- The graph shows the directly proportional relationship
ing potential. between current density and gas productivity. To achieve the
Figure 9 shows the comparison in gas productivity from the clearly set objectives of 4LPM HHO gas for effective catalytic be-
commercial electrolyser to the new design. This increase at 4 V haviour in the combustion engine, a large current density is
from 0.5 ml s21 to 5 ml s21, a 10-fold increase. It also shows required to meet these flow rates. This can be achieved by in-
the polished (clean) electrode surfaces exhibit a higher gas pro- creasing the concentration of KOH solution, which conversely
duction rate than the unpolished (dirty) electrode surfaces. This increases the rate of electrode degradation, by increasing the po-
is a result of decreased surface tension (smoother electrode sur- tential applied to the electrolyser or increasing the electrode
faces from a polishing process) which results in the removal of surface area further.

456 International Journal of Low-Carbon Technologies 2015, 10, 452–459

 Cost effective design of an alkaline electrolyser

Figure 10. Illustration of the linear relationship between gas evolution and Figure 11. Electrolyser current and HHO production projections at 0.1 M KOH
electrical current. solution.

5.6 Performance projections

Equipment limitations meant that the operating current has
been limited to 50 A. As a result, the operating potential has
only been able to achieve 4 V. From the linear relationship
between voltage and current and gas productivity, the data can
be extrapolated up to 12 V and a projection can be made on the
resultant current and HHO gas production. This is shown in
Figure 11.
Assuming the electrolyser behaves as previous electrolyser
cells tested, the approximate current expected at 12 V is 400 A,
while this should result in a HHO gas flow rate of 8 LPM.
Figure 12. Gas composition analysis of gas produced from the electrolyser.

5.7 Mass spectroscopy 5.8.1 Stack lifetime

Figure 12 illustrates the gas composition for the electrolyser gas To analyse the performance of the electrolyser lifetime, the
outlet at 2 V and 1 ml s21 of the gas flow rate. current variation can be measured at a fixed potential over time.
The cycle was allowed to run on pure helium for 5 min, Figure 13 shows the current degradation in the electrolyser for
before being switched onto the electrolyser outlet feed. This SS316 and Nickel for a period of 7 h.
gives us a static background reading of the air currently in the Figure 13 shows that there is a decrease in current flow over
gas line and the electrolyser reservoir (as seen by the increase in the 7 h of operation, seen by the negative gradient for the two
Nitrogen N2). After 10 min, the electrolyser is turned on and electrode materials. The current decreases by 11% for the SS316
hydrogen is seen to be produced. At this point, the level of nitro- and 3% for the Nickel over the 7 h.
gen in the system decreases and the oxygen level increases Using the gradient of the data points, it can be approximated
further (as a result of being produced from the electrolyser). that the time it takes until zero current occurs assuming that the
After 100 min, the system reaches an equilibrium where rate of degradation remains constant. For SS316, this is 53 h,
there is 60% oxygen and 30% hydrogen gas percentage in the and for Nickel, this is 242 h. A 5-fold lifetime extension can be
electrolyser outlet. There is also a small proportion of water found for using Nickel electrodes instead of SS316.
present (vapour carry over from the electrolyser).

5.8 Degradation studies 5.8.2 Electrode surface cleaning

The lifetime of the electrolyser needs to be maintained, so it To increase the lifetime of the electrolyser, the application of
achieves the specified 250 h operation. To analyse this further, metal polish on the surface of the electrodes was investigated.
the rates of degradation were studied in in situ (in the electrolysis The polishing of the plates should theoretically remove the oxide
mode). These processes involve the application of metal polish layers formed on the plates due to exposure to alkaline solution.
to the electrodes and the electrochemical performance as a result This reduces the resistance in the electrolyser unit. The change
of the metal polish, and the current degradation analysis of the in appearance between an unpolished (top) and a polished
electrolyser over a fixed period of time. (bottom) plate can be seen in Figure 14. The cleaner surface is

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D. Symes et al.

Figure 13. Current degradation at fixed potential (4 V).

expected to give rise to a higher rate of bubble evolution due to

more active reaction sites available on the electrode surface area.
An analysis of the effect that polishing the plates has on
Nickel is presented in Figure 15. It shows for two different con-
centrations that polishing the plates increases the flow of current
between the plates and subsequently increases the rate of HHO
gas production for varying potentials.
From this analysis, the benefits of electrode surface cleaning
are evident. This can be characterized further by conducting a
current degradation evaluation to illustrate how the current
decreases over time due to an increase in resistance in the elec-
trolyser cell. This will be carried out over an 8-h period, then
switched off and leaving the KOH solution in the electrolyser
overnight (16 h), and then turning the power on for another 3 h
the following day. After this, the electrodes are then polished
(removal of the oxide layer) and the current degradation was
continued at a fixed potential for a further 3 h. This was com-
pleted for two fixed potentials and is shown in Figure 16.
Figure 14. Image of an unpolished plate (top) and a polished plate (bottom).
Figure 16 shows the long-term electrolytic behaviour of the elec-
trolyser incorporating electrode cleaning and systematic ‘no power’
periods to simulate the real-world application of this electrolyser.
There are three main behaviour patterns in Figure 16. The
first shows a steady increase in current over time during start up.
This is due to the increasing temperature of the electrolyte,
which allows the ions to move more freely. Second, once the
electrolyte temperature has achieved equilibrium, the current
starts to slowly decrease due to the build up of oxide layers on
the surface of the electrodes. This limits the number of nucle-
ation sites available for the electrochemical reaction.
Third, after the electrolyser was shutdown and left sitting in
solution for 3 h, the power was reintroduced to the electrolyser
and a decrease in current was observed from 3 h previously when
the electrolyser was at equilibrium operating temperature, which
is now at room temperature. The data show the current flow Figure 15. Electrochemical performance comparison for unpolished and
increases at a slower rate than seen before due to the presence of polished Nickel plates.
the recently formed oxide layers in the first cycle of testing.
Left for an extended period of 15 h in the shutdown mode decrease in current flow further. Reducing the formation of the
and the electrolyte still present in the electrolyser, the expected oxide layer on the electrode is imperative to the lifetime and
increase in the size of the oxide layer is expected to result in a electrochemical performance of the alkaline electrolyser.

458 International Journal of Low-Carbon Technologies 2015, 10, 452–459

 Cost effective design of an alkaline electrolyser

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