The group has a wide experience in sealing glasses and glass-ceramics for ceramic and metallic components of very different nature and in applications that go from room temperature use to very high temperatures and extreme atmospheres.

One major challenges for the commercialization of planar solid oxide cells (SOFC) is the development of sealing materials suitable for separating the anode and cathode chambers and maintaining the gas-tightness of the system at high temperatures, 600-1000ºC. A promising combination of physical-chemical properties was obtained in RO-BaO/SrO-SiO2 systems where R= Mg and Zn. The developed glass-ceramics have shown a suitable thermo-mechanical behaviour together with a high long-term chemical stability.

4 Layers SOFC stack (FZ-Jülich) sealed with 10B(Sr) glass-ceramic

  • R.Siegel, G. C. Mather, M.Fabian, M. J. Pascual, N. Ditaranto, W. Milius, J.Senker, D. A. Agarkov, V.V. Kharton, J.M. F. Ferreira. Structure and Crystallization of Alkaline-Earth Aluminosilicate Glasses: Prevention of the Alumina Avoidance Principle. A. R. Allu, A. Gaddam, S.Ganisetti, S.Balaji. The Journal of Physical Chemistry B, 122 (17): 4737-4747 (2018). DOI: 10.1021/acs.jpcb.8b01811.
  • S. Rodríguez-López, J. Wei, , K.C. Laurenti, I. Mathias, V.M. Justo, F.C. Serbena, C. Baudín, J. Malzbender, M.J. Pascual. Mechanical properties of solid oxide fuel cell glass-ceramic sealants in the system BaO/SrO-MgO-B2O3-SiO2. Journal of the European Ceramic Society, 37 (2017) 3579-3594, http://dx.doi.org/10.1016/j.jeurceramsoc.2017.03.054).
  • Amarnath R. Allu, Sathravada Balaji, Dilshat U. Tulyaganov, Glenn C. Mather, Fabian Margit, Maria J. Pascual, Renée Siegel, Wolfgang Milius, Jürgen Senker, Dmitry A. Agarkov, Vladislav V. Kharton, José M. F. Ferreira. Understanding the formation of CaAl2Si2O8 in melilite based glass-ceramics: Combined diffraction and spectroscopic studies. ACS Omega 2 (2017) 6233−6243, DOI:10.1021/acsomega.7b00598
  • L.D. Silva, A. M. Rodrigues, A.C.M. Rodrigues, M.J Pascual, A. Durán, A. A.Cabral. Sintering and crystallization of SrO-CaO-B2O3-SiO2 glass-ceramic with different TiO2 contents.Journal of Non-crystalline solids 473 (2017) 33–40, http://dx.doi.org/10.1016/j.jnoncrysol.2017.07.021.
  • S. Rodriguez, V.A.C. Haanappel, A.Durán, F.Muñoz, G.C. Mather, M.J.Pascual, S.Gross. Glass-ceramics in the system MgO-BaO-B2O3-SiO2 under simulated SOFC conditions. International Journal of Hydrogen Energy 41, 15335-15345 (2016). http://dx.doi.org/10.1016/j.ijhydene.2016.07.051).
  • A. Gaddam, H. Fernandes, M.J.Pascual, J.M.F.Ferreira. Influence of Al2O3 and B2O3 on sintering and crystallization of lithium silicate glass system. Journal of the American Ceramic Society, 99 [3] 833-840 (2016). DOI: 10.1111/jace.14040
  • S. Rodríguez-López, R. Comesaña, J. del Val, A. Durán, V.M.Justo, F. C. Serbena, M. J. Pascual. Laser cladding of glass-ceramic sealants for SOFC. Journal of the European Ceramic Society, 53, 16, 4475-4484 (2015). http://dx.doi.org/10.1016/j.jeurceramsoc.2015.08.009.
  • Q. Zhang, L. Fang, J. Shen, M. J. Pascual, T. Zhang. Tuning the Interfacial Reaction between Bismuth-containing Sealing Glass and Cr-containing Interconnect: Effect of ZnO. Journal of the American Ceramic Society, 98, 12, 3797-3806 (2015). DOI: 10.1111/jace.13779.
  • A.A. Reddy, D.Tulyaganov, G. Mather, S. Rodríguez-López, S. Das, M.J. Pascual, F. Muñoz, R. Siegel, J.Senker, J.M.F Ferreira. Influence of strontium oxide on structural transformations in diopside-based glass-ceramics assessed by diverse structural tools. Journal of Physical Chemistry C 119 (2015) 11482-11492. http://dx.doi.org/10.1021/acs.jpcc.5b02475
  • Anuraag Gaddam, Hugo R. Fernandes,Dilshat U. Tulyaganov, Maria J. Pascual, José M.F. Ferreira. Role of manganese on the structure, crystallization and sintering of non-stoichiometric lithium disilicate glasses. RSC Adv., 4, 13581-13592 (2014). DOI:10.1039/C3RA46393A.
  • Allu Amarnath Reddy, Neda Eghtesadi, Dilshat U. Tulyaganov, Maria J.Pascual, Luis F.Santos, Surendran Rajesh, Fernando M.B.Marques, José M.F.Ferreira. Bi-layer glass-ceramic sealant for solid oxide fuel cells.Journal of the European Ceramic Society 34, 5, 1449-1455 (2014).(http://dx.doi.org/10.1016/j.jeurceramsoc.2013.11.012)
  • Allu Amarnath Reddy, Dilshat U. Tulyaganov, G.C.Mather, Maria J. Pascual, Vladislav Kharton, Sergey I. Bredikhin, Vladislav A.Kolotygin, José M.F. Ferreira. Effect of strontium to calcium ratio on the structure, crystallization behavior and functional properties of diopside based glasses. International Journal of Hydrogen Energy 39, 7, 3552-3563 (2014) (http://dx.doi.org/10.1016/j.ijhydene.2013.12.104)
  • Allu Amarnath Reddy, Ashutosh Goel, Dilshat U. Tulyaganov, Mariana Sardo, Luis Mafra, Maria J. Pascual, Vladislav V. Kharton, Ekaterina V. Tsipis, Vladislav A. Kolotygin, and José M. F. Ferreira. Thermal and mechanical stability of lanthanide–containing glass–ceramic sealants for solid oxide fuel cells. Journal of Materials Chemistry A, 2, 6, 1834-1846 (2014). (DOI: 10.1039/c3ta13196c).
  • H.R. Fernandez, D. U. Tulyaganov, M.J.Pascual, J.M.F.Ferreira. Structure-property relationships and densification-crystallization behaviours of simplified lithium disilicate glass compositions. Ceramics International 40, 1, 129-140 (2014). http://dx.doi.org/10.1016/j.ceramint.2013.05.113.
  • Allu Amarnath Reddy, Dilshat U. Tulyaganov, Maria J. Pascual, Vladislav V. Kharton, Ekaterina V. Tsipis, Vladislav A. Kolotygin, José M.F. Ferreira. SrO–Containing Diopside Glass–Ceramic Sealants for Solid Oxide Fuel Cells: Mechanical Reliability and Thermal Shock Resistance. Fuel Cells 13, 5 (2013) 689-694 (DOI: 10.1002/fuce.201200237). Issue October 2013.
  • Allu Amarnath Reddy, Dilshat U. Tulyaganov, Ashutosh Goel, Mariana Sardo, Paul V.Wiper, Maria J.Pascual, Vladislav V. Kharton, Vladislav A. Kolotygin, Ekaterina V. Tsipis, Luis Mafra, Jose M.F. Ferreira. Melilite glass-ceramic sealants for solid oxide fuel cells: Effects of ZrO2 additions assessed by microscopy, diffraction and solid state NMR. Journal of Materials Chemistry A, 1, 21, 6471-6480 (2013), DOI: 10.1039/c3ta10789b.
  • Allu Amarnath Reddy, Dilshat U. Tulyaganov, Ashutosh Goel, Saurabh Kapoor, Maria J. Pascual, José M.F. Ferreira. Sintering and devitrification of glass-powder compacts in the akermanite – gehlenite system. Journal of Materials Science, 48, 11, 4128-4136 (2013). DOI: 10.1007/s10853-013-7225-9.
  • Allu Amarnath Reddy, Ashutosh Goel, Dilshat U. Tulyaganov, Saurabh Kapoor, Pradeesh Kannan, Maria J. Pascual, José M. F. Ferreira. Study of calcium-magnesium-aluminum-silicate (CMAS) glass and glass-ceramic sealant for solid oxide fuel cells. Journal of Power Sources 231, 1, 203-212 (2013). http://dx.doi.org/10.1016/j.jpowsour.2012.12.055.
  • A.Schusser, M.J. Pascual, A. Prange, A. Durán and R. Conradt. Characterization of a soldering system consisting of a glass from the system CaO-Al2O3-B2O3-SiO2 and wollastonite. Ceramics International 39, 4, 3753-3758 (2013). (http://dx.doi.org/10.1016/j.ceramint.2012.10.213).
  • Allu Amarnath Reddy, Dilshat U. Tulyaganov, Maria J. Pascual, Vladislav V. Kharton, Ekaterina V. Tsipis, Vladislav A. Kolotygin, José M.F. Ferreira. Diopside–Ba disilicate glass–ceramic sealants for SOFCs: Enhanced adhesion and thermal stability by Sr for Ca substitution.International Journal of Hydrogen Energy 38, 7, 3073-3086 (2013). http://dx.doi.org/10.1016/j.ijhydene.2012.12.074.
  • H.R.Fernandes, D.U.Tulyaganov, M.J.Pascual, V.V.Kharton, A.A.Yaremchenko, J.MF.Ferreira. The role of K2O on sintering and crystallization of glass powder compacts in the system Li2O-K2O-Al2O3-SiO2. Journal of the European Ceramics Society 32 [10] 2283-2292 (2012). (doi: 10.1016/j.eurcermasoc.2012.02.003).
  • Allu Amarnath Reddy, Dilshat U. Tulyagnov, Saurabh Kapoor, Ashutosh Goel, Maria J. Pascual, Vladislav V. Kharton, José M. F. Ferreira. Study of melilite based glasses and glass-ceramics nucleated by Bi2O3 for functional application. RSC Advances 2,10955–10967(2012) (doi: 10.1039/c2ra22001f).
  • Allu Amarnath Reddy, Dilshat U. Tulyaganov, Maria J. Pascual, Vladislav V. Kharton, Ekaterina V. Tsipis, Vladislav A. Kolotygin, José M.F. Ferreira.
    Diopside–Ba disilicate glass–ceramic sealants for SOFCs: Enhanced adhesion and thermal stability by Sr for Ca substitution.
    International Journal of Hydrogen Energy 38, 7, 3073-3086 (2013). http://dx.doi.org/10.1016/j.ijhydene.2012.12.074.
  • A. Schusser, M.J. Pascual, A. Prange, A. Durán and R. Conradt.
    Characterization of a soldering system consisting of a glass from the system CaO-Al2O3-B2O3-SiO2 and wollastonite.
    Ceramics International (http://dx.doi.org/10.1016/j.ceramint.2012.10.213, on line desde el 21 November 2012).
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  • Allu Amarnath Reddy, Dilshat U. Tulyaanov, Ashutosh Goel, Maria J. Pascual, Vladislav V. Kharton, Ekaterina V.Tsipis, José M. F. Ferreira.
    Diopside – Mg orthosilicate and Diopside – Ba disilicate glass-ceramics for sealing applications in SOFC: sintering and chemical interactions studies.
    International Journal of Hydrogen Energy 37 [17] 12528-12539 (2012).
  • Ashutosh Goel, Allu Amarnath Reddy, Maria J. Pascual, Laurent Gremillard, Annie Malchere, José M.F. Ferreira.
    Sintering behavior of lanthanide-containing glass-ceramic sealants for solid oxide fuel cells.
    Journal of Materials Chemistry 22, 19 (2012) 10042-10054.
  • A.Goel, M.J.Pascual, J.M.F.Ferreira.
    Stable glass-ceramic sealants for solid oxide fuel cells: Influence of Bi2O3 doping.
    International Journal of Hydrogen Energy 35 (2010) 6911-6923.
  • S.T.Reis, M.J.Pascual, R.K.Brow, C.S.Ray, T.Zhang, W.M.Pontuschka.
    Crystallization and processing of SOFC sealing glasses.
    Journal of Non-Crystalline Solids, 356 (2010) 3009-3012.
  • J.Hatcher, M.J.Pascual, D.Poulidi, I.S.Metcalfe.
    Development and testing of an intermediate temperature glass sealant for use in mixed ionic and electronic conducting membrane reactors.
    Solid State Ionics, 181 (2010) 767-774.
  • A.Goel, D.U.Tulyaganov, M.J.Pascual, E.R.Shaaban, F.Muñoz, A.Lü, J.M.F.Ferreira.
    Sintering and crystallization kinetics of La2O3-containing diopside based glass-ceramic sealants for solid oxide fuel cells.
    Journal of Non-Crystalline Solids, 356 (2010)1070-1080.
  • A.Goel, A. Ferrari, I. Kansal, M. J. Pascual, L. Barbieri, F. Bondioli, I. Lancellotti, M.J. Ribeiro, J.F. Ferreira.
    Sintering and crystallization behavior of a CaMgSi2O6-NaFeSi2O6 based glass-ceramics.
    Journal of Applied Physics, 106, 1 (2009).
  • C.Lara, M.J.Pascual, A.Durán.
    Chemical compatibility of RO-BaO-SiO2 (R= Mg, Zn) glass-ceramics sealings with SOFC components.
    Physics and Chemistry of Glasses: European Journal of Glass Science and Technology Part B, 48, 4 (2007) 218-224.
  • M.J.Pascual, A.Guillet, A.Durán.
    Optimization of glass-ceramic compositions in the system MgO-BaO-SiO2 for sealing SOFC.
    Journal of Power Sources 169, 1 (2007) 40-46.
  • M.J.Pascual, C.Lara, A.Durán.
    Non-isothermal crystallization kinetics of devitriying RO-BaO-SiO2 (R= Mg, Zn) glasses.
    Physics and Chemistry of Glasses: European Journal of Glass Science and Technology Part B, 47, 5 (2006) 572-581.
  • M. J. Pascual, V. V. Kharton, E. Tsipis, A. A. Yaremchenko, C. Lara, A. Durán, J. R. Frade.
    Transport properties of sealants for high-temperature electrochemical applications: RO-BaO-SiO2 (R= Mg, Zn) glass-ceramics.
    Journal of the European Ceramic Society, 26 (2006) 3315-3324.
  • C.Lara, M.J.Pascual, R.Keding, A.Durán.
    Electrical behaviour of glass-ceramics in the systems RO-BaO-SiO2 (R= Mg, Zn) for sealing SOFC.
    Journal of Power Sources, 157 (2006) 377-384.
  • C.Lara, M.J.Pascual, A.Durán.
    Glass-forming ability, sinterability and thermal properties in the systems RO-BaO-SiO2 (R= Mg, Zn).
    Journal of Non-Crystalline Solids, 348 (2004) 149-155.
  • C.Lara, M.J.Pascual, M.O.Prado, A.Durán.
    Sintering of glasses in the system RO-Al2O3-BaO-SiO2 (R= Ca, Mg, Zn) studied by hot-stage microscopy.
    Solid State Ionics, 170 (2004) 201-208.Descargar
  • M.J.Pascual, A. Durán, F.J. Valle, R. Berjoin, L.Pascual.
    Corrosion of borosilicate sealing glasses for molten carbonate fuel cells.
    Journal of the American Ceramic Society, 86, 11, 1918-1926 (2003).Descargar
  • M.J.Pascual, A.Durán, L.Pascual.
    Phase separation and crystallisation of glasses in the system R2O-B2O3-SiO2, R= Li, K, Na. Influence on thermal properties.
    Glastechnische Berichte. Glass Science and Technology, 75, 6 (2002).
  • M.J.Pascual, A. Durán, L.Pascual.
    Sealing glass system for molten carbonate fuel cells (MCFC).
    Glass Technology, 43C, 248-254 (2002).
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  • R.Keding, M.J.Pascual, L.Pascual, A.Durán, C.Rüssel.
    Corrosion mechanism of borosilicate sealing glasses in molten carbonates studied by impedance spectroscopy.
    Journal of Electroanalytical Chemistry, 528, 1-2, 184-189 (2002).Descargar
  • M.J.Pascual, L.Pascual, A.Durán, P.Wange, C.Rüssel.
    Alumina and zirconia as inhibitors of crystallization during sintering of borosilicate glasses.
    Glastechnische Berichte. Glass Science and Technology 75, 2, 69-74 (2002).
  • M.J.Pascual, A. Durán, L.Pascual.
    Sintering behaviour of composite materials borosilicate glass-ZrO2 fibre.
    Journal of the European Ceramic Society 22, 9-10, 1513-1524 (2002).
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  • M.J.Pascual, A.Durán, L.Pascual.
    Sintering process of glasses in the system Na2O-B2O3-SiO2.
    Journal of Non-Crystalline Solids, 306, 58-69 (2002).
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  • M.J.Pascual, A. Durán, L. Pascual.
    Viscosity and thermal properties in the system R2O-B2O3-SiO2, R= Li, K, Na.
    Physics and Chemistry of Glasses, 43, 1, 25-31 (2002).