Effect of Al2O3 addition on the catalytic performance of Co/SiC catalyst for Fischer-Tropsch synthesis
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摘要: 分别采用沉淀法、尿素水解法制备Al2O3/SiC复合载体,采用等体积浸渍法制备Co/Al2O3-SiC催化剂。结合N2吸附、XRD、H2-TPR、XPS等表征手段,研究Al2O3助剂对钴基催化剂物相结构、还原行为以及F-T合成性能等的影响。结果表明,氧化铝加入后增强了载体与钴物种之间的相互作用,提高了钴物种的分散度,降低了钴物种的还原度。尿素水解法引入Al2O3后,载体与钴物种具有适中的相互作用,表现出较高的反应活性。沉淀法制备的载体负载钴物种后由于较强的金属-载体相互作用,表现出较优的稳定性。Abstract: Two Al2O3-modified catalysts were prepared by urea hydrolysis method and precipitation disposition method respectively. Combined with N2 adsorption, XRD, XPS and H2-TPR, the effects of Al2O3 on the physico-chemical properties and catalytic properties for the Fischer-Tropsch synthesis were investigated. It was found that the metal-support interaction could be effectively strengthened for both catalysts. Consequently, the dispersion of the catalyst was enhanced and the Fischer-Tropsch synthesis activity was increased. The results also indicated that the modification of Co/SiC catalyst strongly depended on the preparation method. The highest CO conversion was observed on the catalyst prepared by urea hydrolysis method due to the superior dispersion and good reducibility. Besides, the catalytic stability was enhanced due to the stronger interaction between cobalt and Al2O3 prepared by precipitation disposition method.
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孙予罕, 陈建刚, 王俊刚, 贾丽涛, 侯博, 李德宝, 张娟. 费托合成钴基催化剂的研究进展[J]. Chinese Journal of Catalysis, 2010, 31(6): 919-927.
(SUN Yu-han, CHEN Jian-gang, WANG Jun-gang, JIA Li-tao, HOU Bo, LI De-bao, ZHANG Juan. The development of cobalt-based catalysts for Fischer-Tropsch synthesis[J]. Chinese Journal of Catalysis, 2010, 31(6): 919-927.)ZHU X, LU X, LIU X, HILDEBR D, GLASSER T D. Study of radial heat transfer in a tubular Fischer-Tropsch synthesis reactor[J]. Ind Eng Chem Res, 2010, 49(21): 10682-10688. LACROIX M, DREIBINE L, TYMOWSKI B D, VIGNERON F, EDOUARD D, BéGIN D, NGUYEN P, PHAM C, SAVIN-PONCET S, LUCK F. Silicon carbide foam composite containing cobalt as a highly selective and re-usable Fischer-Tropsch synthesis catalyst[J]. Appl Catal A: Gen, 2011, 397(1/2): 62-72. WANG Q, SUN W Z, JIN G Q, WANG Y Y, GUO X Y. Biomorphic SiC pellets as catalyst support for partial oxidation of methane to syngas[J]. Appl Catal B: Environ, 2008, 79(4): 307-312. MOENE R, TIJSEN E P A M, MAKKEE M, MOULIJN J A. Synthesis and thermal stability of Ni, Cu, Co, and Mo catalysts based on high surface area silicon carbide[J]. Appl Catal A: Gen, 1999, 184(1): 127-141. DE LA OSA A R, DE LUCAS A, ROMERO A, VALVERDE J L, SANCHEZ P. Infiuence of the catalytic support on the industrial Fischer-Tropsch synthetic diesel production[J]. Catal Today, 2011, 176(1): 298-302. WANG X, NING W, HU L, LI Y. Influences of Al2O3 on the structure and reactive performance of Co/ZnO catalyst[J]. Catal Commun, 2012, 24: 61-64. ARNOLDY P, MOULIJIN J. Temperature-programmed reduction of CoO/AI2O3 catalysts[J]. J Catal, 1985, 93(1): 38-54. VISWANATHAN B, GOPALAKRISHNAN R. Effect of support and promoter in Fischer-Tropsch cobalt catalysts[J]. J Catal, 1986, 99(2): 342-348. MARTINEZ A N, LOPEZ C, MARQUEZ F, DIAZ I. Fischer-Tropsch synthesis of hydrocarbons over mesoporous Co/SBA-15 catalysts: The influence of metal loading, cobalt precursor, and promoters[J]. J Catal, 2003, 220(2): 486-499. PRESSER V, NICKEL K G. Silica on silicon carbide[J]. Crit Rev Solid State, 2008, 33(1): 1-99. BINNER J, ZHANG Y. Characterization of silicon carbide and silicon powders by XPS and zeta potential measurement[J]. J Mater Sci Lett, 2001, 20(2): 123-126. TYMOWSKI D B, LIU Y, MENY C, LEFèVRE C, BEGIN D, NGUYEN P, PHAM C, EDOUARD D, LUCK F, PHAM-HUU C. Co-Ru/SiC impregnated with ethanol as an effective catalyst for the Fischer-Tropsch synthesis[J]. Appl Catal A: Gen, 2012, 419-420: 31-40. ZHANG Y, KOIKE M, TSUBAKI N. Preparation of alumina-silica bimodal pore catalysts for Fischer-Tropsch synthesis[J]. Catal Lett, 2005, 99(3): 193-198. DE LA OSA A R, DE LUCAS A, SANCHEZ-SILVA L, DIAZ-MAROTO J, VALVERDE J L, SANCHEZ P. Performing the best composition of supported Co/SiC catalyst for selective FTS diesel production[J]. Fuel, 2011, 95: 587-598. REUEL R C, BARTHOLOMEW C H. Effects of support and dispersion on the CO hydrogenation activity/selectivity properties of cobalt[J]. J Catal, 1984, 85(1): 78-88. 周玮, 陈建刚, 孙予罕. 钴基催化剂在固定床Fischer-Tropsch合成反应中的失活行为研究[D]. 太原: 中国科学院山西煤炭化学研究所, 2005.
(ZHOU Wei, CHEN Jian-gang, SUN Yu-han. Deactivation studies of Co-based catalysts for Fischer-Tropsch synthesis in fixed-bed reactor[D]. Taiyuan: The Institute of Coal Chemistry, Chinese Academy of Sciences, 2005.)MOODLEY D J, VAN DE LOOSDRECHT J, SAIB A M, OVERETT M J, DATYE A K, NIEMANTSVERDRIET J W. Carbon deposition as a deactivation mechanism of cobalt-based Fischer-Tropsch synthesis catalysts under realistic conditions[J]. Appl Catal A: Gen, 2009, 354(1/2): 102-110. TAVASOLI A, MALEK ABBASLOU R M, DALAI A K. Deactivation behavior of ruthenium promoted Co/γ-Al2O3 catalysts in Fischer-Tropsch synthesis[J]. Appl Catal A: Gen, 2008, 346(1/2): 58-64.
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