Gold modified cobalt-based Fischer-Tropsch catalysts for conversion of synthesis gas to liquid fuels
Alan J. McCue, Jura Aponaviciute, Richard P.K. Wells, James A. Anderson
Gold modified cobalt-based Fischer-Tropsch catalysts for conversion of synthesis gas to liquid fuels
The addition of Au as a promoter/modifier for alumina supported Co catalyst has been studied by combined in-situ high temperature, high pressure Fourier transform infrared (FTIR) and on-line gas chromatography. The combination of these tools permitted the state of the active catalyst surface to be monitored while following the elution of reaction products during the first 5–7 h on stream of the catalyst. The catalysts under study were a 10%Co/Al2O3 and a 2.5%Au/10%Co/Al2O3. Samples were characterised before use using Raman and temperature programmed reduction (TPR). During the initial stages of reaction, hydrocarbons were built up on the surface of the catalyst as monitored by FTIR and the nature and amount of these species were assessed in terms of CH2/CH3 ratio and the density of these alkyl fragments by employing absorption coefficients for the individual components. The nature and reducibility of the Co particles were modified by the presence of Au while the later also shifted the CO/H2 balance by acting as an effective water-gas shift catalyst during the early stages of reaction. This characteristic was lost during reaction as a consequence of redistribution of the two metallic phases.
gold modified catalyst / conversion of synthesis gas
[1] |
Fischer F, Tropsch H. Die erdölsynthese bei gewöhnlichem druck aus den vergangsprodukten der kohlen. Brennstoff Chemie, 1926, 7: 97–104
|
[2] |
Viswanathan B, Gopalakrishnan R. Effect of support and promoter in Fischer Tropsch cobalt catalysts. Journal of Catalysis, 1986, 99(2): 342–348
CrossRef
Google scholar
|
[3] |
Enger B C, Fossan A L, Borg Ø, Rytter E, Holmen A. Modified alumina as catalyst support for cobalt in the Fischer-Tropsch synthesis. Journal of Catalysis, 2011, 284(1): 9–22
CrossRef
Google scholar
|
[4] |
Morales F, Weckhuysen B M. Catalysis, Volume 19, RSC, 2006
|
[5] |
Anderson J A, McQuire M W, Rochester C H, Sweeney T. In-situ FTIR study of CO/H2 reactions over Rh/SiO2 catalysts at high pressure and temperature. Catalysis Today, 1991, 9(1-2): 23–30
CrossRef
Google scholar
|
[6] |
Anderson J A, Khader M M. A high pressure, high temperature infrared study of CO hydrogenation over Rh/ZrO2. Journal of Molecular Catalysis A Chemical, 1996, 105(3): 175–183
CrossRef
Google scholar
|
[7] |
Anderson J A, Khader M M. An in situ infrared study of hydrogenation of CO over Rh/ZrO2. Mikrochimica Acta, 1997, 14: 363–365
|
[8] |
McQuire M W, Rochester C H, Anderson J A. Syngas reactions over Rh/SiO2 at high-pressure and temperature studied by Fourier-transform infrared-spectroscopy. Journal of the Chemical Society, Faraday Transactions, 1992, 88(6): 879–886
CrossRef
Google scholar
|
[9] |
Anderson J A, Fernandez-Garcia M, Haller G L. Surface and bulk characterisation of metallic phases present during CO hydrogenation over Pd-Cu/KL zeolite catalysts. Journal of Catalysis, 1996, 164(2): 477–483
CrossRef
Google scholar
|
[10] |
Jiang M, Koizumi N, Ozaki T, Yamada M. Adsorption properties of cobalt and cobalt-managese catalysts studied by in-situ diffuse reflectance FTIR using CO and CO+H2 as probes. Applied Catalysis A, General, 2001, 209(1-2): 59–70
CrossRef
Google scholar
|
[11] |
Kobori Y, Yamasaki H, Naito S, Oniishi T, Tamuru K. Mechanistic study of carbon-monoxide hydrogenation over ruthenium catalysts. Journal of the Chemical Society, Faraday Transactions I, 1982, 78(5): 1473–1490
CrossRef
Google scholar
|
[12] |
Yamasaki H, Kobori Y, Naito S, Oniishi T, Tamuru K. Infrared study of the reaction of H2 + CO on a Ru-SiO2 catalysts. Journal of the Chemical Society, Faraday Transactions I, 1981, 77(12): 2913–2925
CrossRef
Google scholar
|
[13] |
Dalla Betta R A, Shelef M. Heterogeneous methanation—in-situ IR spectroscopic study of Ru/Al2O3 during hydrogenation of CO. Journal of Catalysis, 1977, 48(1-3): 111–119
CrossRef
Google scholar
|
[14] |
Ekerdt J G, Bell A T. Synthesis of hydrocarbons from CO and H2 over silica-supported Ru— reaction rate measurements and infrared-spectra of adsorbed species. Journal of Catalysis, 1979, 58(2): 170–187
CrossRef
Google scholar
|
[15] |
King D L. In-situ infrared study of CO hydrogenation over slica and alumina supported ruthenium and silica supported iron. Journal of Catalysis, 1980, 61(1): 77–86
CrossRef
Google scholar
|
[16] |
Jalama K, Coville N J, Hildebrandt D, Glasser D, Jewell L L, Anderson J A, Taylor S, Enache D, Hutchings G J. Effect of the addition of Au on Co/TiO2 catalyst for the Fischer-Tropsch reaction. Topics in Catalysis, 2007, 44(1-2): 129–136
CrossRef
Google scholar
|
[17] |
Jalama K, Coville N J, Xiong H, Hildebrandt D, Glasser D, Taylor S, Carley A, Anderson J A, Hutchings G J. A comparison of Au/Co/Al2O3 and Au/Co/SiO2 catalysts in the Fischer-Tropsch reaction. Applied Catalysis A, General, 2011, 395(1-2): 1–9
CrossRef
Google scholar
|
[18] |
Andreeva D, Idaklev V, Tabakova T, Giovanoli R. Low temperature water gas shift reactions on Au/TiO2, Au/α-Fe2O3 and Au/Co3O4. Bulgarian Chemical Communications, 1998, 30: 59–68
|
[19] |
Tang C W, Wang C B, Chen S H. Characteristion of cobalt oxides studied by FT-IR, Raman, TPR and TG-MS. Thermochimica Acta, 2008, 473(1-2): 68–73
CrossRef
Google scholar
|
[20] |
Jacobs G, Ji Y, Davis B H, Cronauer D, Kropf A J, Marshall C L. Fischer-Tropsch synthesis: Temperature programmed EXAFS/XANES investiation of the influence of support type, cobalt loading and noble metal promoter addition to the reduction behaviour of cobalt oxide particles. Applied Catalysis A, General, 2007, 333(2): 177–191
CrossRef
Google scholar
|
[21] |
Li J, Zhan X, Zhang Y, Jacobs G, Das T, Davis B H. Fischer-Tropsch synthesis: effect of water on the deactivation of Pt promoted Co/Al2O3 catalysts. Applied Catalysis A, General, 2002, 228(1-2): 203–212
CrossRef
Google scholar
|
[22] |
Jacobs G, Ribeiro M C, Ma W, Ji Y, Khalid S, Sumodjo P T A, Davis B H, 0. (Cu, Ag, Au) promotion of 15%Co/Al2O3 Fischer-Tropsch synthesis catalysts. Applied Catalysis A, General, 2009, 361(1-2): 137–151
CrossRef
Google scholar
|
[23] |
Couble J, Bianchi D. Heats of adsorption of linearly adsorbed CO species on Co2+ and Co sites of reduced Co/Al2O3 catalysts in relashionship with the CO/H2 reaction. Applied Catalysis A, General, 2012, 445: 1–13
CrossRef
Google scholar
|
[24] |
Khodakov A Y, Lynch J, Bazin D, Rebours B, Zanier N, Moisan B, Chaumette P. Reducibility of cobalt species in silica-supported Fischer-Tropsch catalysts. Journal of Catalysis, 1997, 168(1): 16–25
CrossRef
Google scholar
|
[25] |
Busca G, Guidetti P, Lorenzelli V. Fourier-Transform infrared study of the surface properties of cobalt oxides. Journal of the Chemical Society, Faraday Transactions I, 1990, 86(6): 989–994
CrossRef
Google scholar
|
[26] |
Rao K M, Spoto G, Zecchina A. IR investigation of CO adsorbed on Co particles obtained via Co2(CO)8 on MgO and SiO2. Journal of Catalysis, 1988, 113(2): 466–474
CrossRef
Google scholar
|
[27] |
Galhenage R P, Ammal S C, Yan H, Duke A S, Tenney S A, Heyden A, Chen D A. Nucleation, growth and adsorbate-induced changes in composition for Co-Au bimetallic clusters on TiO2. Journal of Physical Chemistry C, 2012, 116(46): 24616–24629
CrossRef
Google scholar
|
[28] |
Wexler A S. Infrared determination of structural units in organic compounds by integrated intensity measurements: Alkanes, alkenes and monosubstituted alkyl benzenes. Spectrochimica Acta. Part A: Molecular Spectroscopy, 1965, 21: 1725–1742
|
[29a] |
McCue A J, McNab A, Anderson J A. unpublished data
|
[29] |
Stefanowicz-Pieta I A, Ishaq M, Wells R, Anderson J A. Quantitative determination of acid sites on silica-alumina. Applied Catalysis A, General, 2010, 390(1-2): 127–134
CrossRef
Google scholar
|
[30] |
McQuire M W, Rochester C H, Anderson J A. Fourier-transform infrared study of Rh/SiO2 catalysts exposed to CO H2 mixtures at high-pressure and temperature. Journal of the Chemical Society, Faraday Transactions, 1991, 87(12): 1921–1928
CrossRef
Google scholar
|
[31] |
Jacobs G, Chaney J A, Patterson P M, Das T K, Davis B H. Fischer-Tropsch synthesis: study of the promotion of Re on the reduction property of Co/Al2O3 catalysts bu in-situ EXAFS/XANES of CoK and Re L-III edges and XPS. Applied Catalysis A, General, 2004, 264(2): 203–212
CrossRef
Google scholar
|
/
〈 | 〉 |