以未硅烷化和硅烷化的SBA-15为载体,采用满孔浸渍法制备了钴基费-托合成催化剂,通过元素分析、N_2吸附-脱附、X射线衍射、H_2程序升温还原、H_2程序升温脱附以及氧滴定等手段对催化剂进行了表征.催化剂的费-托合成活性测试在固定床反应器上进行.研究表明,对于SBA-15硅烷化后制备的催化剂,金属钴与载体之间的相互作用降低,氧化钴的还原度增加.随着三甲基氯硅烷用量的增加,三甲基硅基的表面覆盖度增加,钴的晶粒直径增大.硅烷化后的催化剂的高活性归因于高的还原度.而C_(5+)选择性的增加则归因于钴晶粒直径的增大.
Cobalt catalysts supported on unsilylated and silylated SBA-1S were prepared by incipient wetness impregnation and characterized by elemental analysis, N_2 adsorption-desorption, X-ray diffraction, H_2 temperature-programmed reduction, H_2 temperature-programmed desorption, and oxygen titration. Their catalytic properties for Fischer-Tropsch synthesis were evaluated in a fixed-bed reactor. The results show that the interaction between cobalt and the support was decreased, and the reducibility of the cobalt oxide species was more facile on the silylated Co/SBA-15 catalyst. With increasing (CH_3)_3SiCl loading, the surface coverage of the trimethylsilyl group increased, and the cobalt cluster size was larger. The higher activity of the silylated 10%Co/SBA-15 catalysts was ascribed to its improved reducibility. The increase in selectivity for C_(5+) hydrocarbons was attributed to the increase in cobalt cluster size.
参考文献
| [1] | Schulz H .[J].Applied Catalysis,1999,186:3. |
| [2] | Dai X P;Yu Ch Ch .[J].Journal of Natural Gas Chemistry,2008,17:17. |
| [3] | Dry ME .[J].Catalysis Today,2002,71:227. |
| [4] | Panpranot J.;Goodwin JG.;Sayari A. .CO hydrogenation on Ru-promoted Co/MCM-41 catalysts[J].Journal of Catalysis,2002(2):530-539. |
| [5] | Iglesia E;Soled S L;Fiato KA .[J].Journal of Catalysis,1992,137:212. |
| [6] | Li J L;Zhan X D;Zhang Y Q;Jacobs G Das T Davis B H .[J].Applied Catalysis A:General,2002,228:203. |
| [7] | Rygh LES.;Nielsen CJ. .Infrared study of CO adsorbed on a Co/Re/gamma Al2O3-based Fischer-Tropsch catalyst[J].Journal of Catalysis,2000(2):401-409. |
| [8] | Kogelbauer A.;Oukaci R.;Goodwin JG. .RUTHENIUM PROMOTION OF CO/AL2O3 FISCHER-TROPSCH CATALYSTS[J].Journal of Catalysis,1996(1):125-133. |
| [9] | Feller A;Claeys M;van Steen E .[J].Journal of Catalysis,1999,185:120. |
| [10] | Kim DJ;Dunn BC;Cole P;Turpin G;Ernst RD;Pugmire RJ;Kang M;Kim JM;Eyring EM .Enhancement in the reducibility of cobalt oxides on a mesoporous silica supported cobalt catalyst[J].Chemical communications,2005(11):1462-1464. |
| [11] | Khodakov AY.;Griboval-Constant A.;Bechara R.;Zholobenko VL. .Pore size effects in Fischer Tropsch synthesis over cobalt-supported mesoporous silicas[J].Journal of Catalysis,2002(2):230-241. |
| [12] | Jacobs G;Das T K;Zhang Y Q;Li J L Racoillet G Davis B H .[J].Applied Catalysis A:General,2002,233:263. |
| [13] | 徐振刚;罗伟;五乃继;肖翠微 .[J].煤炭化,2008,31(03):92. |
| [14] | Ji Y G;Zhao Zh;Yu Ch Ch;Duan A J Jiang G Y .[J].Chem Ind Eng Progress,2007,26:927. |
| [15] | Zhao DY.;Feng JL.;Chmelka BF.;Stucky GD.;Huo QS. .Nonionic triblock and star diblock copolymer and oligomeric surfactant syntheses of highly ordered, hydrothermally stable, mesoporous silica structures[J].Journal of the American Chemical Society,1998(24):6024-6036. |
| [16] | Huang B Y;Li X J;Ji Sh F;Lang B Habimana F Li Ch Y .[J].Journal of Natural Gas Chemistry,2008,17:225. |
| [17] | Kubota Y;Ikeya H;Sugi Y;Yamada T Tatsumi T .[J].Journal of Molecular Catalysis A:Chemical,2006,249:181. |
| [18] | Zhang Y;Hanayama K;Tsubaki N .[J].Catalysis Communications,2006,7:251. |
| [19] | Martínez A;Prieto G .[J].Journal of Catalysis,2007,245:470. |
| [20] | Zhang L X;Shi J L;Yu J;Hua Z L Zhao X G Ruan M L .[J].Advanced Materials,2002,14:1510. |
| [21] | Corma A;Domine M;Gaona J A;Jord'a J L,Navarro M T,Rey F,Pérez-Pariente J,Tsuji J,McCulloch B,Nemeth L T.[J].Chemical Communications,1998:2211. |
| [22] | Reuel R C;Bartholomew CH .[J].Journal of Catalysis,1984,85:63. |
| [23] | Song D C;Li J L .[J].Journal of Molecular Catalysis A:Chemical,2006,247:206. |
| [24] | Xiong H F;Zhang Y H;Liew K Y;Li J L .[J].Journal of Molecular Catalysis A:Chemical,2008,295:68. |
| [25] | Martínez A;López C;Marquez F;Díaz I .[J].Journal of Catalysis,2003,220:486. |
| [26] | Belambe AR.;Goodwin JG.;Oukaci R. .EFFECT OF PRETREATMENT ON THE ACTIVITY OF A RU-PROMOTED CO/AL2O3 FISCHER-TROPSCH CATALYST[J].Journal of Catalysis,1997(1):8-15. |
| [27] | Borgφ;Eri S;Blekkan E A;Storsster S Wigum H Rytter E Holmen A .[J].Journal of Catalysis,2007,248:89. |
- 下载量()
- 访问量()
- 您的评分：
-
10%
-
20%
-
30%
-
40%
-
50%