Nickel catalysts for internal reforming in molten carbonate fuel cells

Natural gas may be used instead of hydrogen as fuel for the molten carbonate fuel cell (MCFC) by steam reforming the natural gas inside the MCFC, using a nickel catalyst (internal reforming). The severe conditions inside the MCFC, however, require that the catalyst has a very high stability. In order to find suitable types of nickel catalysts and to obtain more knowledge about the deactivation mechanism(s) occurring during internal reforming, a series of nickel catalysts was prepared and subjected to stability tests at 973 K in an atmosphere containing steam and lithium and potassium hydroxide vapours. All the catalysts prepared showed a significant growth of the nickel crystallites during the test, especially one based on ?-Al2O3 and a coprecipitated Ni/Al2O3 sample having a very high nickel content. However, this growth of nickel crystallites only partially explained the very strong deactivation observed in most cases. Only a coprecipitated nickel/alumina catalyst with high alumina content and a deposition-precipitation catalyst showed satisfactory residual activities. Addition of magnesium or lanthanum oxide to a coprecipitated nickel/alumina catalyst decreased the stability. Adsorption and retention of the alkali was the most important factor determining the stability of a catalyst in an atmosphere containing alkali hydroxides. This is because the catalyst bed may remain active if a small part of the catalyst bed retains all the alkali.

[1]  P. J. Anderson,et al.  Effects of water vapour on sintering of MgO , 1964 .

[2]  M. Boudart,et al.  ETHANE HYDROGENATION-CRACKING ON IRON CATALYSTS WITH AND WITHOUT ALKALI , 1954 .

[3]  Anthony B. Pinkerton,et al.  Bull. Soc. Chim. Fr. , 1957 .

[4]  V. Perrichon,et al.  Thermal stability of alkali metals deposited on oxide supports and their influence on the surface area of the support , 1988 .

[5]  T. K. Campbell,et al.  Carbon dioxide hydrogenation on potassium-promoted nickel catalysts , 1989 .

[6]  H. Schaper,et al.  Synthesis Of Methanation Catalysts By Deposition-Precipitation , 1983 .

[7]  R. Whittaker,et al.  Steam reforming catalysts , 1973 .

[8]  J. Dumesic,et al.  Migration of potassium on iron and alumina surfaces as studied by Auger electron spectroscopy , 1985 .

[9]  J. Dalmon,et al.  Exchange with deuterium of methane on nickel catalysts , 1984 .

[10]  Jens R. Rostrup-Nielsen,et al.  Catalytic Steam Reforming , 1984 .

[11]  J. G. Goodwin,et al.  Potassium dispersion on silica-supported ruthenium catalysts , 1991 .

[12]  F. Frusteri,et al.  Activity and Characterization of Alkali Doped Ni/MgO Catalysts , 1989 .

[13]  J. Ross,et al.  Mechanism of the steam reforming of methane over a coprecipitated nickel-alumina catalyst , 1973 .

[14]  G. G. Stokes "J." , 1890, The New Yale Book of Quotations.

[15]  R. W. Joyner The contribution made by surface science to understanding reactivity in heterogeneous catalysis , 1990 .

[16]  J. Ross,et al.  The effect of lanthanum additives on the catalytic activities of Ni-Al2O3 coprecipitated catalysts for the methanation of carbon monoxide , 1984 .

[17]  G. Ertl,et al.  XPS studies with ammonia synthesis catalysts , 1979 .

[18]  D. Blackmond,et al.  Adsorption and reaction of CO and H2 on K-promoted Rh/SiO2 catalysts , 1987 .

[19]  J. N. Wilson,et al.  Aging of Silica and Alumina Gels , 1965 .

[20]  I. Chorkendorff,et al.  Xps study of chemisorption of CH4 on Ni(100) , 1990 .

[21]  P. Schoubye Methanation of CO on some Ni catalysts , 1969 .

[22]  T. K. Campbell,et al.  Potassium promotion of Ni/Al2O3 catalysts , 1989 .

[23]  D. Goodman,et al.  Dissociative adsorption of alkanes on clean and sulfur-modified nickel surfaces , 1990 .

[24]  Patricio Reyes,et al.  React. Kinet. Catal. Lett. , 1974 .

[25]  Jens R. Rostrup-Nielsen,et al.  Activity of nickel catalysts for steam reforming of hydrocarbons , 1973 .

[26]  Sydney P. S. Andrew,et al.  Catalysts and Catalytic Processes in The Steam Reforming of Naphtha , 1969 .

[27]  A. Miyamoto,et al.  Effect of alkaline carbonate on the dissociation of the CO bond in the methanation over RuAl2O3 catalyst , 1986 .

[28]  H. Praliaud,et al.  Potassium addition to Fe/MgO, Ni/MgO and Ni/SiO2: Reducibility, dispersity and stabilization of the promoter by the support , 1987 .

[29]  M. Boudart Two‐step catalytic reactions , 1972 .

[30]  L. L. V. Reijen,et al.  Coprecipitated nickel–alumina catalysts for methanation at high temperature. Part 1.—Chemical composition and structure of the precipitates , 1981 .

[31]  R. Lathe Phd by thesis , 1988, Nature.

[32]  Coadsorption, promoters and poisons , 1993 .

[33]  Koji Kishida,et al.  The State of MCFC Technology Development , 1990 .

[34]  M. W. Roberts,et al.  Surface and defect properties of solids , 1974 .

[35]  G. Ertl,et al.  Scanning Auger Microscopy Studies on Industrial Ammonia Synthesis Catalysts , 1982 .

[36]  P. Gallezot,et al.  Study by Analytical Electron Microscopy of the Potassium Distribution on Silica-Supported Nickel and Palladium Catalysts , 1989 .

[37]  Keiske Kaji,et al.  X-Ray Diffraction Procedures , 1975 .

[38]  J. Szanyi,et al.  Methane activation on clean and oxidized Ni(100) , 1993 .

[39]  H. Praliaud,et al.  Alkali-induced sieving effect in Ni on silica catalysts , 1991 .

[40]  N. N. Bobrov,et al.  Studies of activity of Ni−MgO and Ni/LiAlO2 catalysts in methane steam reforming , 1989 .

[41]  H. Schaper,et al.  Synthesis of thermostable nickel-alumina catalysts by deposition-precipitation , 1985 .

[42]  W. Mross Alkali Doping in Heterogeneous Catalysis , 1983 .