用XRD,TPR和XPS技术对Co-Mo/AC(活性炭)和Co-Mo/γ-Al2O3催化剂进行了表征,并以二苯并噻吩HDS反应评价了催化剂的活性. 在不同温度下处理的催化剂,其活性组分高度分散在活性炭表面,未检测到明显的Mo和Co物种. 在Co-Mo/AC催化剂中,表面物种的还原温度低于Co-Mo/γ-Al2O3的还原温度. 在260 ℃下处理的Co-Mo/AC催化剂,其表面Mo是高价态的Mo(Ⅵ),在500 ℃下处理的Co-Mo/AC催化剂,其表面存在Mo(Ⅴ)和Mo(Ⅵ)两种价态. 硫化态CoMoS/AC催化剂中存在Mo(Ⅳ)和Mo(Ⅴ)两种低价态的Mo物种,而S主要以S2-2和S2-的形式存在于MoS2和MoO3S2-中,还有部分高价态的S6+. 在硫化态CoMoS/γ-Al2O3催化剂中,Mo主要以Mo(Ⅴ)和Mo(Ⅵ)两种状态存在,而S主要以S2-2或S2-的形式存在于MoO2S2-和MoO3S2- 中,还有部分高价态的S6+. 活性评价结果表明,n(Co)/n(Mo)=0.7的Co-Mo/AC的活性高于Co-Mo/γ-Al2O3的活性,而其他Co/Mo比的Co-Mo/AC的活性低于Co-Mo/γ-Al2O3的活性.
参考文献
[1] | 姚国欣,刘伯华.21世纪的炼油技术和炼油厂(1)[J].炼油设计,2001(01):1-6. |
[2] | 刘晨光,Flora T.T.Ng.二苯并噻吩在分散型钼催化剂和原位产生的氢存在下的加氢脱硫Ⅱ.原位氢和分子氢的比较[J].催化学报,1999(05):505-509. |
[3] | Geneste P;Amblard P;Bonnet M;Graffin P .[J].Journal of Catalysis,1980,61(01):115. |
[4] | 魏昭彬;辛勤;盛世善;陈恒荣, 刘敬利, 蒋建明 .[J].催化学报,1994,15(04):243. |
[5] | 魏昭彬;辛勤;盛世善;陈恒荣 .[J].催化学报,1995,16(05):359. |
[6] | Farag H.;Sakanishi K.;Mochida I. .Fundamental comparison studies on hydrodesulfurization of dibenzothiophenes over CoMo-based carbon and alumina catalysts[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2000(Special Issue SI):147-157. |
[7] | Farag H;Whitehurst D D;Sakanishi K;Mochida I .[J].Catalysis Today,1999,50(01):9. |
[8] | Wivel C;Candia R;Clausen B S;Mrup S, Topse H .[J].Journal of Catalysis,1981,68(02):453. |
[9] | Grange P .[J].Catalysis Review-Science and Engineering,1980,21(01):135. |
[10] | Ratnasamy P;Sivasanker S .[J].Catalysis Review-Science and Engineering,1980,22(03):401. |
[11] | Thomas R;De Beer V H J;Moulijn J A .[J].Bulletin des Societes Chimiques Belges,1981,90(12):1349. |
[12] | Arnoldy P;Moulijn J A .[J].Journal of Catalysis,1985,93(01):38. |
[13] | Duchet J C;van Oers E M;de Beer V H J;Prins R .[J].Journal of Catalysis,1983,80(02):386. |
[14] | Pan W-H;Leonowicz M E;Stiefel E I .[J].Inorganic Chemistry,1983,22(04):672. |
[15] | 张谊华;徐奕德;石映祯;倪月琴 .[J].催化学报,1987,8(01):27. |
[16] | Arnoldy P;Franken M C;Scheffer B;Moulijn J A .[J].Journal of Catalysis,1985,96(02):381. |
[17] | Feng L J;Li X G;Dadyburjor D B;Kugler E L .[J].Journal of Catalysis,2000,190(01):1. |
[18] | Calafat A.;Lopezagudo A.;Palacios JM.;Laine J. .EFFECT OF SURFACE OXIDATION OF THE SUPPORT ON THE THIOPHENE HYDRODESULFURIZATION ACTIVITY OF MO, NI, AND NIMO CATALYSTS SUPPORTED ON ACTIVATED CARBON[J].Journal of Catalysis,1996(1):20-30. |
[19] | Papadopoulou Ch;Vakros J;Matralis H K;Kordulis Ch, Lycourghiotis A .[J].Journal of Colloid and Interface Science,2003,261:146. |
[20] | Karakonstantis L;Matralis H;Kordulis Ch;Lycourghiotis A .[J].Journal of Catalysis,1996,162(02):305. |
[21] | Cordero R L;Llambias F J G;Agudo A L .[J].Applied Catalysis,1991,74(01):125. |
[22] | Brito J;Laine J .[J].Polyhedron,1986,5(1/2):179. |
[23] | Vakros J.;Kordulis C.;Lycourghiotis A. .Cobalt oxide supported gamma-alumina catalyst with very high active surface area prepared by equilibrium deposition filtration[J].Langmuir: The ACS Journal of Surfaces and Colloids,2002(2):417-422. |
[24] | Rajagopal S;Marini H J;Marzari J A;Miranda R .[J].Journal of Catalysis,1994,147(02):417. |
[25] | Yoshinaka S;Segawa K .[J].Catalysis Today,1998,45(1-4):293. |
[26] | Shimada H;Sato T;Yoshimura Y;Hiraishi J, Nishijima A .[J].Journal of Catalysis,1988,110(02):275. |
[27] | Patterson T A;Carver J C;Leyden D E;Hercules D M .[J].Journal of Physical Chemistry,1976,80(15):1700. |
[28] | Weber Th;Muijsers J C;Niemantsverdriet J W .[J].Journal of Physical Chemistry,1995,99(22):9194. |
[29] | Weber Th;Muijsers J C;van Wolput J H M C;Verhagen C P J, Niemantsverdriet J W .[J].Journal of Physical Chemistry,1996,100(33):14144. |
[30] | Muijsers J C;Weber Th;van Hardeveld R M;Zandbergen H W, Niemantsverdriet J W .[J].Journal of Catalysis,1995,157(02):698. |
[31] | Li C P;Hercules D M .[J].Journal of Physical Chemistry,1984,88(03):456. |
[32] | Sullivan DL.;Ekerdt JG. .EFFECT OF CATALYST OXIDATION STATE AND STRUCTURE ON THIOPHENE HYDRODESULFURIZATION OVER MODEL MOLYBDENUM CATALYSTS[J].Journal of Catalysis,1997(1):64-75. |
[33] | Bouwens S M A M;Prins R;de Beer V H J;Koning-sberger D C .[J].Journal of Physical Chemistry,1990,94(09):3711. |
[34] | Bouwens S M A M;van Veen J A R;Koningsberger D C;de Beer V H J, Prins R .[J].Journal of Physical Chemistry,1991,95(01):123. |
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