采用机械混合、机械混合后焙烧和机械混合后微波处理等方法制备Mo/HZSM-5催化剂,并对催化剂上甲烷芳构化反应性能进行了考察.结果表明,与浸渍法相比,用机械混合法、固相反应法和微波法制备的催化剂,在保持甲烷转化率不变的前提下,能明显提高芳烃选择性并减少积炭的生成;不同方法制备的Mo/HZSM-5催化剂上Mo物种的落位不同,机械混合法、固相反应法和微波法使Mo物种较多地落位于分子筛外表面.结合反应结果可以得出,落位于分子筛外表面的Mo物种对甲烷芳构化反应更为有利,而且明显减少积炭的生成.
Mo/HZSM-5 is a typical catalyst for methane dehydro-aromatizationin the abse nce of oxygen. The catalyst was prepared with impregnation method in previous st udies. In this paper, mechanical mixing, solid reaction and microwave methods we re used for Mo/HZSM-5 preparation. In addition, the catalytic performance of th e catalyst for methane dehydro-aromatization was investigated. Compared with im pregnated Mo/HZSM-5 sample, the catalyst samples prepared with mechanical mixin g, solid reaction and microwave methods show higher selectivity for aromatics an d lower selectivity for coke. BET, XRD and NH3-TPD experimental results exhib ited that the location of Mo species is heavily dependent on the preparation met hod. It is suggested that the Mo species located on the external surface of the zeolite is more efficient for methane dehydro-aromatization, and at the same ti me suppresses the coke formation.
参考文献
| [1] | Wang L Sh;Tao L X;Xie M S .[J].Catalysis Letters,1993,21(1-2):35. |
| [2] | Xu Y D;Liu Sh T;Wang L Sh .[J].Catalysis Letters,1995,30(1-4):135. |
| [3] | Chen LY.;Xu ZS.;Li XS.;Zhang T.;Lin LW. .DEHYDRO-OLIGOMERIZATION OF METHANE TO ETHYLENE AND AROMATICS OVER MOLYBDENUM/HZSM-5 CATALYST[J].Journal of Catalysis,1995(1):190-200. |
| [4] | Xu Y D;Shu Y Y;Liu Sh T .[J].Catalysis Letters,1995,35(3-4):233. |
| [5] | Solymosi F;Erdohelyi A;Szoke A .[J].Catalysis Letters,1995,32(1-2):43. |
| [6] | Wang D;Lunsford J H;Rosynek M P .[J].Topics in Catalysis,1996,3(3-4):289. |
| [7] | Shu YY.;Wong ST.;Wang LS.;Guo XX.;Xu YD. .PROMOTIONAL EFFECT OF RU ON THE DEHYDROGENATION AND AROMATIZATION OF METHANE IN THE ABSENCE OF OXYGEN OVER MO/HZSM-5 CATALYSTS[J].Journal of Catalysis,1997(1):11-19. |
| [8] | Liu Sh T;Dong Q;Ohnishi R.[J].Journal of the Chemical Society,Chemical Communications,1997(15):1457. |
| [9] | Zeng JL.;Zhang HB.;Lin GD.;Tsai KR.;Xiong ZT. .Nonoxidative dehydrogenation and aromatization of methane over W/HZSM-5-based catalysts[J].Catalysis Letters,1998(1/2):119-124. |
| [10] | Zhang Ch L;Li Sh;Yuan Y .[J].Catalysis Letters,1998,56(04):207. |
| [11] | Zhang W P;Ma D;Liu X Ch.[J].Journal of the Chemical Society,Chemical Communications,1999(12):1091. |
| [12] | Xu Y D;Lin L W .[J].Applied Catalysis A:General,1999,188(1-2):53. |
| [13] | 贾殿赠.微波技术在固相配位化学反应中的应用研究（Ⅰ）--Co（Ⅱ）、Ni（Ⅱ）、Cu（Ⅱ）配合物在微波条件下的固相合成[J].高等学校化学学报,1997(09):1432. |
| [14] | Yin D H;Yin D L .[J].Microporous and Mesoporous Materials,1998,24(4-6):123. |
- 下载量()
- 访问量()
- 您的评分：
-
10%
-
20%
-
30%
-
40%
-
50%