Electrochemistry Communications 54 (2015) 23–27

Contents lists available at ScienceDirect

Electrochemistry Communications

journal homepage: www.elsevier.com/locate/elecom

High performance solid oxide electrolysis cell with

impregnated electrodes
Ting Chen, Yucun Zhou, Minquan Liu, Chun Yuan, Xiaofeng Ye, Zhongliang Zhan, Shaorong Wang ⁎
CAS Key Laboratory of Materials for Energy Conversion, Shanghai Institute of Ceramics, Chinese Academy of Sciences (SICCAS), 1295 Dingxi Road, Shanghai 200050, PR China

a r t i c l e i n f o a b s t r a c t

Article history: Here we report a solid oxide electrolysis cell (SOEC) employing impregnated electrodes. The cell structure consisted
Received 9 February 2015 of a porous 430 L metal support, a Ni-Ce0.8Sm0.2O2 − δ (SDC) impregnated 430 L-zirconia stabilized zirconia (YSZ)
Accepted 25 February 2015 hydrogen electrode, a scandia stabilized zirconia (SSZ) electrolyte and a Nd2O3-Nd2NiO4+ δ (Nd2O3-NNO) impreg-
Available online 4 March 2015
nated SSZ oxygen electrode. The cell is prepared by tape casting, co-firing and impregnation techniques. At an
applied voltage of 1.3 V and 50% steam content, current density of 2.05 A cm−2 is obtained at 800 °C. The effect
Keywords:
Solid oxide electrolysis cell
of the variation of H2O/H2 ratio (3/97 to 70/30) on electrolysis performance at 750 °C is evaluated and the long-
Hydrogen production term stability in electrolysis mode is also investigated.
Impregnated electrodes © 2015 Elsevier B.V. All rights reserved.
Metal-support
Long-term stability

1. Introduction issues such as delamination at the oxygen electrode/electrolyte inter-

Hydrogen is a clean energy carrier with the highest weight specific
energy density and has been considered as potentially the best future
alternative to fossil fuels. Of all known methods to generate hydrogen,
water electrolysis is probably the cleanest method and produces hydro-
gen with high purity and no pollution [1,2]. Water electrolysis involves
both the hydrogen evolution reaction at the cathode and the oxygen
evolution reaction at the anode. The theoretical water splitting voltage
is 1.23 V at 25 °C and 0.95 V at 900 °C [1]. Operating at high temperature
decreases the water splitting voltage and the electrical energy demand
due to lower polarization and facile reaction kinetics. Both thermody-
namic and kinetic factors result in higher current density at a given
cell voltage and steam partial pressure [3]. High temperature steam
electrolysis to hydrogen using solid oxide electrolysis cells (SOECs),
which is defined as the reverse of solid oxide fuel cells (SOFCs), has
shown higher energy efficiency for hydrogen production when compared
to alkaline or proton exchange membrane (PEM) water electrolysis [4].
Research into SOECs has increased significantly in recent years. Tietz
et al. reported a hydrogen electrode supported SOEC with a current den-
sity of −1 A cm−2 at an absolute humidity of 80 vol.% which displayed
an overall degradation rate of only 3.8% kh−1 during operation at about
778 °C for 9000 h [5]. Ebbesen et al. also studied a Ni/YSZ electrode sup-
ported SOEC stack operating at −0.25 A cm−2 at 850 °C in a 1:1 atmo-
sphere of H2O/H2 for 830 h, demanding that long-term electrolysis is
feasible without notable degradation [6]. Despite these promising
results, the development of SOECs is still at the lab-scale and stability
⁎ Corresponding author. Tel.: +86 21 5241 1520; fax: +86 21 5241 3903.
E-mail address: srwang@mail.sic.ac.cn (S. Wang).
face, coarsening and agglomeration of nickel particles require further
refinement [7]. Preparing cell electrodes via the impregnation method
can help overcome these issues [8–10]. Although the low mechanical
strength of ceramic backbones with high porosity could restrict the de-
velopment of such techniques, metal-supported solid oxide fuel cells
(MS-SOFCs) using a mechanically robust metal to support the whole
cell could effectively solve this problem [11].
In this work, we developed an intermediate temperature (650 °C–
800 °C) SOEC comprising impregnated electrodes and a metal support.
The cell consisting of a porous 430 L metal support, a Ni-SDC impregnat-
ed 430 L-YSZ hydrogen electrode, SSZ electrolyte and a Nd2O3-NNO im-
pregnated SSZ oxygen electrode, was prepared by tape casting, co-firing
and impregnation techniques. The electrochemical performance at
varying temperatures and steam contents were investigated and the
long-term stability in SOEC mode was also studied.
2. Experimental
The metal-supported solid oxide electrolysis cell (MS-SOEC) was
fabricated via a two-step procedure. Firstly, the four-layer structure—
porous 430 L (strainless steel) support | porous 430 L-8Zr0.92Y0.08O1.96
(YSZ) backbone | Zr0.88Sc0.22Ce0.01O2.12 (SSZ) electrolyte | porous SSZ
backbone—was prepared by laminating four tape-casted green tapes,
followed by co-firing in a reducing atmosphere (5% H2–95% N2) at
1300 °C for 4 h [12]. Secondly, the oxygen electrode catalyst, Nd2O3-
Nd2NiO4+ δ (Nd2O3-NNO), was introduced into the porous SSZ back-
bone using an aqueous solution containing Nd(NO3)3, Ni(NO3)2 and
citric acid in a molar ratio of 2:1:3. After drying, the Ni-Sm0.2C0.8O2 − δ
(SDC) was impregnated into the porous 430 L-YSZ backbone as

http://dx.doi.org/10.1016/j.elecom.2015.02.015
1388-2481/© 2015 Elsevier B.V. All rights reserved.
24 T. Chen et al. / Electrochemistry Communications 54 (2015) 23–27

25000
observed, previous studies have shown that it does not affect the cath-
(a) ode performance [14,15].
20000
For electrochemical measurements, silver paste was painted onto
Intensity/a.u.

15000 the electrode surfaces as the current collector. Steam was produced
using a bubbler with precise temperature control and the ratio of
10000
steam to the fuel gas (H2) was controlled by setting the bubbler temper-
5000 ature according to saturated steam pressure curve. The effective oxygen
electrode active area of the single cell was 0.35 cm2. The cell was evaluat-
0 ed in SOEC mode with different partial pressures of H2O/H2 (3/97-70/30)
20 30 40 50 60 70 80 and applied voltages (0.3–1.6 V) at a scan rate of 20 mV s−1. Electro-
2 /degree chemical impedance spectra (EIS) were measured with an IM6 Electro-
chemical Workstation (ZAHNER, Germany) employing a sinusoidal
(b) amplitude signal of 20 mV in the frequency range of 50 mHz to
100 kHz. Microstructures of the SOEC were examined by scanning elec-
tron microscopy (SEM) using a Hitachi SU-8220 microscope.
Nd2O3-NNO-SSZ

Ni-SDC-430L-YSZ

3. Results and discussion

SSZ

430L

Fig. 1(b) shows the cross-sectional SEM micrograph of SOEC con-

taining a porous Nd2O3-NNO impregnated SSZ oxygen electrode
(≈30 μm), a dense SSZ electrolyte (≈15 μm), a porous Ni-SDC impreg-
nated YSZ-430 L composite hydrogen electrode (≈50 μm) and a porous
430 L substrate (≈ 200 μm). Good adherence between the different

(c) (d)
Ni-SDC Ni-SDC

430L-YSZ
430L-YSZ
Before After 146 h

(e) (f) SSZ

SSZ
Nd2O3-NNO Nd2O3-NNO

Before After 146 h

Fig. 1. (a): XRD pattern of the Nd2NiO4+ δ impregnated YSZ composite measured at 800 °C.
(b): SEM micrograph of the cross-section of the MS-SOEC. (c) and (d): Ni-SDC impregnat-
ed 430 L-YSZ composite hydrogen electrode before and after long-term durability electrol-
ysis tests. (e) and (f): NNO impregnated SSZ composite oxygen electrode before and after
long-term durability electrolysis tests.

the hydrogen electrode catalyst at a weight ratio of 2:8 [13]. Both

catalysts were impregnated into the porous SSZ backbone and porous
430 L-8YSZ backbone for each experiment. Heat treatment of the elec-
trodes was conducted at 350 °C in air for 0.5 h. The loadings of impreg-
nated catalysts were controlled using a micro-liter syringe and the
impregnation/heat treating cycle was repeated to achieve the desired
loadings (30 wt.% catalyst loading for the oxygen electrode and
10 wt.% catalyst loading for the hydrogen electrode). The final sintering
of the impregnated catalysts was conducted at 800 °C for 2 h in-situ Fig. 2. (a): I–V curves of the single cell in electrolysis mode (H2O/H2 = 50/50) measured at
before the cell testing process. The desired NNO phase was confirmed 650 °C–800 °C. (b): Electrochemical impedance spectra measured at open circuit
by X-ray diffraction as shown in Fig. 1(a). Although the Nd2O3 phase is potential.
 T. Chen et al. / Electrochemistry Communications 54 (2015) 23–27 25

layers was obtained which can decrease the degree of delamination of
the oxygen electrode in electrolysis mode. SEM images of the porous
YSZ-430 L backbone impregnated with Ni-SDC coatings before and
after 146 h of electrolysis testing at 650 °C is shown in Fig. 1(c) and
(d), respectively, with no significant morphological changes observed.
Ni-SDC was adopted as the hydrogen electrode due to its high catalytic
activity and good stability, which has been shown to exhibit stable po-
larization resistance in a 1200 h durability test [13]. SEM images of the
porous SSZ backbone impregnated with Nd2O3-NNO coatings before
and after long-term electrolysis testing at 650 °C are shown in
Fig. 1(e) and (f) and also show no obvious growth of the infiltrated
particles. NNO was used as the oxygen electrode due to its high surface
exchange and oxygen diffusion coefficients [16].
Fig. 2 shows the steam electrolysis performance of the Nd2O3-NNO-
SSZ|SSZ|Ni-SDC-YSZ-430 L|430 L cell measured between 650 °C and
800 °C. A 1:1 mixture of H2 and steam was fed as the inlet gas to the
hydrogen electrode and the other was exposed to an air atmosphere
with a flow rate of 100 mL min−1. The I–V response measured as a func-
tion of temperature is displayed in Fig. 2(a). The open circuit voltage
(OCV) values of the cell in SOEC mode were 0.95, 0.95, 0.98 and 0.99 V
at temperatures of 800 °C, 750 °C, 700 °C and 650 °C, respectively. At
an electrolysis voltage of 1.3 V, the current densities were 2.05, 1.62,

Fig. 3. (a): I–V curves of the single cell in electrolysis mode measured at 750 °C as a function of the steam to hydrogen ratio (H2O/H2 = 3/97, 30/70, 50/50, 70/30). (b): EIS curves with 3%
steam content under different current loads. (c): EIS curves at 30% steam content under different current loads. (d): EIS curves at 50% steam content under different current loads.
(e): Long-term durability electrolysis test of the single cell operated at 600 °C with 30% steam content. (f): The IV response before and after a 330 h electrolysis test.
26 T. Chen et al. / Electrochemistry Communications 54 (2015) 23–27
1.06 and 0.60 A cm−2 at the temperatures of 800 °C, 750 °C, 700 °C and
650 °C, respectively, which are comparable performances to other
SOECs. For example, a Ni-YSZ electrode supported SOEC with
La0.6Sr0.4Co0.2Fe0.8O3 − δ (LSCF) impregnated YSZ oxygen electrode
exhibited a current density of 1.14 A cm− 2 at 1.3 V and 800 °C [17],
while another hydrogen electrode (Ni-YSZ) supported cell with an im-
pregnated Sm0.5Sr0.5CoO3 oxygen electrode demonstrated a current
density of 1.8 A cm−2 at 1.3 V and 750 °C [18]. Since electrode micro-
structure exhibits a significant effect on electrolytic performance [19],
the remarkable performance reported here may be due to the micro
or nano structure of the cell electrodes leading to high porosity and an
increase in triple phase boundaries which promote gas diffusion and
electrochemical reactions [20]. Furthermore, the large and irregular
pores of the 430 L substrate enhance steam absorption and diffusion.
It can be observed that the performance in SOEC mode is significantly
better than in SOFC mode, probably due to the hyperstoichiometry of
the NNO Ruddlesden–Popper phases leading to fast oxygen diffusion
through bulk the materials and rapid exchange kinetics [14,21,22]. In
addition the Nd2O3 could play a significant role at the oxygen electrode
as its presence may hinder the sintering of NNO particles, and thus
maintaining a large surface area.
Nyquist plot of the impedance data measured at OCV in electrolysis
mode is shown in Fig. 2(b). The overall polarization resistances were
0.17, 0.26, 0.40 and 0.72 Ω cm2 while the pure ohmic resistances were
0.10, 0.11, 0.16 and 0.24 Ω cm2 at 800 °C, 750 °C, 700 °C and 650 °C, re-
spectively. One of the drawbacks of the SOEC employing a metal support
is the oxidation of the metal support under high steam content [23]. The
MS-SOEC comprised of ferritic steel/Ni-YSZ/YSZ/LSCF has been demon-
strated and showed a degradation rate of 3.2% kh−1 at a steam content
of 43% and a current density of −0.3 A cm−2 at 800 °C [24].
The effect of the steam content on the cell performance was also in-
vestigated in the SOEC mode. Fig. 3(a) shows the I–V response of the
SOEC when the steam-to-H2 ratio was varied (H2O/H2 = 3/97, 30/70,
50/50 and 70/30) at 750 °C. The OCVs decrease with increasing steam/
hydrogen ratio in accordance with the Nernst equation. The electrolysis
performance significantly increased with increasing H2O/H2 ratio, as
shown previously [8,10]. Specifically, current densities of 1.62 A cm−2
and 1.70 A cm−2 were obtained at an electrolysis voltage of 1.3 V with
50% and 70% steam content, which indicate that the hydrogen produc-
tion rates were as high as 676.7 and 710.6 mL cm−2 h−1 (according to
Faraday's law and assuming 100% current efficiency). Concentration po-
larization was clearly observed at low current densities and at 3% steam
content; however, this polarization disappeared when the steam con-
tent was increased, showing that the diffusion of H2O may be the rate
limiting step. Fig. 3(b), (c) and (d) shows the EIS curves at different
steam concentrations and different current loads, respectively. Concen-
tration polarization was observed under high electrolysis currents, e.g.
−1 A cm−2 with 3% steam content while this polarization disappeared
when the steam content was increased to 30% and 50%. The polarization
resistance under current load was lower than at OCV in Fig. 3(b)–(d),
consistent with the result shown in Fig. 3(a).
For another cell with the same structure, the durability in electrolysis
mode was measured at 600 °C with 30% steam content as shown in
Fig. 3(e). The I–V responses before and after long-term stability tests
are shown in Fig. 3(f), demanding that a significantly increased electrol-
ysis performance was found. The observed increase in performance is
probably due to the reorganization of particles (both in size term via
chemical reactions to form oxides) or the slight decrease in OCV, while
the polarization loss of the cell remained stable. Future work will focus
on studying the stability of the SOEC obtained here.
4. Conclusions
An SOEC comprising impregnated electrodes and a metal support
was proposed for the first time and excellent electrolysis performance
was exhibited. At an applied voltage of 1.3 V and at 50% steam content,
current densities of 2.05, 1.62, 1.06 and 0.60 A cm− 2 are obtained at
800 °C, 750 °C, 700 °C and 650 °C respectively. Furthermore, an electrol-
ysis current of 1.7 A cm−2 and a hydrogen production rate of
710.6 mL cm−2 h−1 have been achieved at 750 °C employing an elec-
trolysis voltage of 1.3 V and 70% steam content. More work is required
to further understand the long-term stability of this SOEC.
Conflict of interest
The authors declare that there are no conflicts of interest.
Acknowledgments
We gratefully acknowledge the financial support from the Chinese Gov-
ernment High Tech Developing Project (2011AA050702), the Science and
Technology commission of Shanghai Municipality (No. 12160706500)
and the National Natural Science Foundation of China (No. 51172266).
References
[1] M. Wang, Z. Wang, X. Gong, Z. Guo, The intensification technologies to water
electrolysis for hydrogen production—a review, Renew. Sust. Energ. Rev. 29
(2014) 573–588.
[2] J. Turner, G. Sverdrup, M.K. Mann, P.-C. Maness, B. Kroposki, M. Ghirardi, R.J. Evans,
D. Blake, Renewable hydrogen production, Int. J. Energy Res. 32 (2008) 379–407.
[3] M.A. Laguna-Bercero, Recent advances in high temperature electrolysis using solid
oxide fuel cells: a review, J. Power Sources 203 (2012) 4–16.
[4] M. Ni, M. Leung, D. Leung, Technological development of hydrogen production by
solid oxide electrolyzer cell (SOEC), Int. J. Hydrog. Energy 33 (2008) 2337–2354.
[5] F. Tietz, D. Sebold, A. Brisse, J. Schefold, Degradation phenomena in a solid
oxide electrolysis cell after 9000 h of operation, J. Power Sources 223 (2013)
129–135.
[6] S.D. Ebbesen, J. Høgh, K.A. Nielsen, J.U. Nielsen, M. Mogensen, Durable SOC stacks for
production of hydrogen and synthesis gas by high temperature electrolysis, Int. J.
Hydrog. Energy 36 (2011) 7363–7373.
[7] P. Moçoteguy, A. Brisse, A review and comprehensive analysis of degradation
mechanisms of solid oxide electrolysis cells, Int. J. Hydrog. Energy 38 (2013)
15887–15902.
[8] P. Kim-Lohsoontorn, Y.-M. Kim, N. Laosiripojana, J. Bae, Gadolinium doped ceria-
impregnated nickel–yttria stabilised zirconia cathode for solid oxide electrolysis
cell, Int. J. Hydrog. Energy 36 (2011) 9420–9427.
[9] K. Chen, N. Ai, S.P. Jiang, Reasons for the high stability of nano-structured
(La, Sr)MnO3 infiltrated Y2O3–ZrO2 composite oxygen electrodes of solid oxide
electrolysis cells, Electrochem. Commun. 19 (2012) 119–122.
[10] A.R. Hanifi, M.A. Laguna-Bercero, T.H. Etsell, P. Sarkar, The effect of electrode infiltra-
tion on the performance of tubular solid oxide fuel cells under electrolysis and fuel
cell modes, Int. J. Hydrog. Energy 39 (2014) 8002–8008.
[11] M.C. Tucker, Progress in metal-supported solid oxide fuel cells: a review, J. Power
Sources 195 (2010) 4570–4582.
[12] Y. Zhou, X. Xin, J. Li, X. Ye, C. Xia, S. Wang, Z. Zhan, Performance and degradation of
metal-supported solid oxide fuel cells with impregnated electrodes, Int. J. Hydrog.
Energy 39 (2014) 2279–2285.
[13] Y. Zhou, C. Yuan, T. Chen, X. Meng, X. Ye, J. Li, S. Wang, Z. Zhan, Evaluation of Ni and
Ni-Ce0.8Sm0.2O2 − δ (SDC) impregnated 430 L anodes for metal-supported solid
oxide fuel cells, J. Power Sources 267 (2014) 117–122.
[14] M.A. Laguna-Bercero, A.R. Hanifi, H. Monzon, J. Cunningham, T.H. Etsell, P. Sarkar,
High performance of microtubular solid oxide fuel cells using Nd2NiO4+ δ-based
composite cathodes, J. Mater. Chem. A 2 (2014) 9764–9770.
[15] T. Chen, Y. Zhou, C. Yuan, M. Liu, X. Meng, Z. Zhan, C. Xia, S. Wang, Impregnated
Nd2NiO4+ δ- scandia stabilized zirconia composite cathode for intermediate-
temperature solid oxide fuel cells, J. Power Sources 269 (2014) 812–817.
[16] E. Boehm, J. Bassat, P. Dordor, F. Mauvy, J. Grenier, P. Stevens, Oxygen diffusion and
transport properties in non-stoichiometric LnNiO oxides, Solid State Ionics 176
(2005) 2717–2725.
[17] H. Fan, M. Keane, N. Li, D. Tang, P. Singh, M. Han, Electrochemical stability of
La0.6Sr0.4Co0.2Fe0.8O3− δ-infiltrated YSZ oxygen electrode for reversible solid oxide
fuel cells, Int. J. Hydrog. Energy 39 (2014) 14071–14078.
[18] S.-i. Lee, J. Kim, J.-W. Son, J.-H. Lee, B.-K. Kim, H.-J. Je, H.-W. Lee, H. Song, K.J. Yoon,
High performance air electrode for solid oxide regenerative fuel cells fabricated by
infiltration of nano-catalysts, J. Power Sources 250 (2014) 15–20.
[19] L. Shao, S. Wang, J. Qian, X. Ye, T. Wen, Optimization of the electrode-supported
tubular solid oxide cells for application on fuel cell and steam electrolysis, Int. J.
Hydrog. Energy 38 (2013) 4272–4280.
[20] Z. Zhan, Y. Zhou, S. Wang, X. Liu, X. Meng, T. Wen, Nanostructure electrodes for
metal-supported solid oxide fuel cells, Solid Oxide Fuel Cells 13 (Sofc-Xiii), 57,
2013, pp. 925–931.
[21] F. Chauveau, J. Mougin, J.M. Bassat, F. Mauvy, J.C. Grenier, A new anode material for
solid oxide electrolyser: the neodymium nickelate Nd2NiO4+ δ, J. Power Sources 195
(2010) 744–749.
 T. Chen et al. / Electrochemistry Communications 54 (2015) 23–27 27

[22] M.A. Laguna-Bercero, N. Kinadjan, R. Sayers, H. El Shinawi, C. Greaves, S.J. Skinner,
Performance of La2 − xSrxCo0.5Ni0.5O4 ± δ as an oxygen electrode for solid oxide
reversible cells, Fuel Cells 11 (2011) 102–107.
[23] E. Sarasketa-Zabala, L. Otaegi, L.M. Rodriguez-Martinez, M.A. Alvarez, N. Burgos, F.
Castro, I. Villarreal, High temperature stability of porous metal substrates under
highly humidified hydrogen conditions for metal supported Solid Oxide Fuel Cells,
Solid State Ionics 222 (2012) 16–22.
[24] G. Schiller, A. Ansar, M. Lang, O. Patz, High temperature water electrolysis using
metal supported solid oxide electrolyser cells (SOEC), J. Appl. Electrochem. 39
(2008) 293–301.