制备了两种器外预硫化型MoNiP/γ-Al2O3催化剂,并以二苯并噻吩为模型化合物考察了其加氢脱硫(HDS)活性,选择了传统的器内预硫化催化剂作为参比.采用X射线衍射(XRD)、高分辨透射电镜(HRTEM)和X射线光电子能谱(XPS)等手段对二者在加氢活性相方面的差别进行了研究.结果表明,器外预硫化催化剂的HDS活性(最高达到99%)与器内预硫化催化剂相当,但是其加氢能力相对较弱.XRD与HRTEM等研究表明,器外预硫化催化剂所形成的MoS2片晶的堆垛层数相对较低,而Mo与S元素的XPS分析结果则说明相对器内预硫化催化剂,器外预硫化催化剂中不但Mo的硫化度较低,而且MoS2活性相的含量亦较少,而二者活性相之间的这种差异应是导致两类催化剂加氢活性不同的主要原因.
参考文献
[1] | 曹光伟,罗锡辉,刘振华,何金海.加氢处理催化剂的制备和表征Ⅰ. MoNiP/Al2O3催化剂的制备及助剂的作用[J].催化学报,2001(02):143-147. |
[2] | 徐友明,李文库,何金海,罗锡辉.加氢处理催化剂的制备和表征Ⅱ. 制备方法对MoNiP/Al2O3催化剂性质的影响[J].催化学报,2001(06):575-578. |
[3] | Bataille F.;Michaud P.;Perot G.;Vrinat M.;Lemaire M. Schulz E.;Breysse M.;Kasztelan S.;Lemberton JL. .Alkyldibenzothiophenes hydrodesulfurization-promoter effect, reactivity, and reaction mechanism[J].Journal of Catalysis,2000(2):409-422. |
[4] | 王月霞.加氢催化剂的器外预硫化[J].炼油设计,2000(07):57-58. |
[5] | Berrebi G .[P].US 4530917,1985. |
[6] | Berrebi G;Le Gall B .[P].US 5139983,1992. |
[7] | Roumieu R;Boitiaux J P .[P].US 5153163,1992. |
[8] | Blashka S;Bond G;Ward D .[J].Oil & Gas Journal,1998,96(01):36. |
[9] | 贺胜如,袁赞根,刘建平.加氢催化剂器外预硫化技术的工业应用[J].石油炼制与化工,2004(08):34-36. |
[10] | Dufresne P;Le Gall B;Berrebi G .[P].US 5397756,1995. |
[11] | Dufresne P;Brahma N;Murff S R .[P].US 5985787,1994. |
[12] | Dufresne P;Brahma N;Labruyere F;Lacroix M Breysse M .[J].Catalysis Today,1996,29(1-4):251. |
[13] | Labruyere F;Dufresne P;Lacroix M;Breysse M .[J].Catalysis Today,1998,43(1-2):111. |
[14] | 王倩,聂红,龙湘云.H2S对NiW/Al2O3和CoMo/Al2O3上二苯并噻吩和4,6-二甲基二苯并噻吩加氢脱硫反应的影响[J].催化学报,2005(05):399-402. |
[15] | Hoffer B W;Devred F;Kooyman P J;van Langeveld A D Bonne R L C Griffiths C Lok C M Moulijn J A .[J].Journal of Catalysis,2002,209(01):245. |
[16] | Calais C.;Geantet C.;Yoshimura Y.;Shimada H. Nishijima A.;Lacroix M.;Breysse M.;Matsubayashi N. .Crystallite size determination of highly dispersed unsupported MoS2 catalysts[J].Journal of Catalysis,1998(2):130-141. |
[17] | Hensen E J M;Kooyman P J;van der Meer Y;van der Kraan A M de Beer V H J van Veen J A R van Santen R A .[J].Journal of Catalysis,2001,199(02):224. |
[18] | Topsф'e H;Clausen B S;Topsф'e N Y;Pedersen E .[J].Industrial and Engineering Chemistry Research,1986,25(01):25. |
[19] | Chung P L;Hercules D M .[J].Journal of Physical Chemistry,1984,88(03):456. |
[20] | Zhang LP.;Ozkan US.;Karakas G. .NiMoS/gamma-Al2O3 catalysts: The nature and the aging behavior of active sites in HDN reactions[J].Journal of Catalysis,1998(2):457-465. |
[21] | Damyanova S;Petrov L;Grange P .[J].Applied Catalysis A:General,2003,239(1-2):241. |
[22] | Portela L.;Delmon B.;Grange P. .XPS AND NO ADSORPTION STUDIES ON ALUMINA-SUPPORTED CO-MO CATALYSTS SULFIDED BY DIFFERENT PROCEDURES[J].Journal of Catalysis,1995(2):243-254. |
[23] | Quincy R B;Houalla M;Proctor A;Hercules D M .[J].Journal of Physical Chemistry,1990,94(04):1520. |
[24] | Yamada M;Yasumaru J;Houalla M;Hercules D M .[J].Journal of Physical Chemistry,1991,95(18):7037. |
[25] | 朱崇业;牛国兴;陈海鹰;李全芝,陆秋韵,王家寰,方维平 .[J].复旦学报(自然科学版),1995,34(05):490. |
[26] | 刘世宏;王当憨;潘承璜.X射线光电子能谱分析[M].北京:科学出版社,1988:15. |
[27] | 冯丽娟.超细Mo/AⅠ2O3催化剂(Ⅱ)--加氢脱硫表面结构性质研究[J].高等学校化学学报,1995(01):103. |
[28] | Arnoldy P;Van Den Heijkant J A;de Bok G D;Moulijn J A .[J].Journal of Catalysis,1985,92(01):35. |
[29] | Weber T;Muijsers J C;van Wolput H J M C;Verhagen C P J Niemantsverdriet J W .[J].Journal of Physical Chemistry,1996,100(33):14144. |
上一张
下一张
上一张
下一张
计量
- 下载量()
- 访问量()
文章评分
- 您的评分:
-
10%
-
20%
-
30%
-
40%
-
50%