采用同体多核~(13)C,~(27)Al及~(29)Si MAS NMR结合吸附气体xe后的~(129)Xe NMR,详细研究了乙烯和2-丁烯歧化生成丙烯反应过程中6%Mo/Hβ-Al_2O_3催化剂上积炭的类型和落位.结果表明,积炭以饱和烷烃为主,并随着反应的进行生成更多的支链烷烃,积炭主要分布在Hβ分子筛上,并主要落位在分子筛的交叉孔道处.
Multinuclear solid-state ~(13)C, ~(27)Al, and ~(29)Si MAS NMR and ~(129)Xe NMR were used to study the carbon deposition on the 6%Mo/Hβ-Al_2O_3 catalyst in metathesis of ethene and 2-butene to propene. The results showed that the coke composition was aliphatic hy-drocarbons, and the most of them was present in Hβ zeolite instead of in Al_2O_3. The ~(129)Xe NMR experiments clearly revealed that the depos-ited carbon was located at the positions of channel intersections in HI3 zeolite, which caused the deactivation of the catalyst.
参考文献
| [1] | 邹颈松.[J].化工时刊,1998(12):30. |
| [2] | 陈乐怡.世界丙烯工业进展与展望[J].中外能源,2009(03):66-70. |
| [3] | 吴铭.丙烯需求持续增长增产工艺色彩纷呈[J].中国石油和化工,2004(10):38-44. |
| [4] | 黄声骏,辛文杰,白杰,谢素娟,刘盛林,徐龙伢.钼负载型催化剂上乙烯与2-丁烯歧化制丙烯[J].石油化工,2003(03):191-194. |
| [5] | Liu Sh L;Huang Sh J;Xin W J;Bai J Xie S J Xu L Y .[J].Catalysis Today,2004,93:471. |
| [6] | Li X J;Zhang W P;Liu Sh L;Han X W Xu L Y Bao X H .[J].Journal of Catalysis,2007,250:55. |
| [7] | Mol J C .[J].Catalysis Today,1999,51:289. |
| [8] | 许峥,张鎏,张继炎.Ni/γ-Al2O3催化剂上CH4-CO2重整体系中积碳-消碳的研究[J].催化学报,2001(01):18-22. |
| [9] | 石雷,周晓霜,蔡天锡,王新平.一步法合成吲哚用Ag/SiO2催化剂的失活及其抑制[J].催化学报,2003(06):471-474. |
| [10] | 刘红梅,申文杰,包信和,徐奕德.Co助剂对甲烷脱氢芳构化反应中Mo/MCM-22催化剂积碳行为的影响[J].催化学报,2004(06):495-500. |
| [11] | Li X J;Zhang W P;Li X;Liu Sh L Huang H J Han X W Xu L Y Bao X H .[J].Journal of Physical Chemistry C,2009,113:8228. |
| [12] | Jameson A K;Jameson C J;Gutowsky H S .[J].Journal of Chemical Physics,1970,53:2310. |
| [13] | Zhang W P;Han X W;Liu X C;Lei H Liu X M Bao X H .[J].Microporous and Mesoporous Materials,2002,53:145. |
| [14] | Gutsze A;Lange J P;Karge H G;Allgeier J .[J].Journal of Catalysis,1988,113:525. |
| [15] | Bonardet J L;Barrage M C;Fraissard J .[J].Journal of Molecular Catalysis A:Chemical,1995,96:123. |
| [16] | Datema K P;Nowak A K;Houckgeest J V;Wielers A F H .[J].Catalysis Letters,1991,11:267. |
| [17] | van Bokhoven JA.;Kunkeler P.;van Bekkum H.;Kentgens APM.;Koningsberger DC. .Stepwise dealumination of zeolite beta at specific T-sites observed with Al-27 MAS and Al-27 MQ MAS NMR[J].Journal of the American Chemical Society,2000(51):12842-12847. |
| [18] | Kraus H;Muller M;Prins R;Kentgens A P M .[J].Journal of Physical Chemistry B,1998,102:3862. |
| [19] | Zhang W;Ma D;Han X W;Liu X M Bao X H Guo X W Wang X S .[J].Journal of Catalysis,1999,188:393. |
| [20] | Liu W;Xu Y;Wong S T;Wang L Qiu J Yang N .[J].Journal of Molecular Catalysis A:Chemical,1997,120:257. |
| [21] | Perez-Pariente J;Sanz J;Fornes V;Corma A .[J].Journal of Catalysis,1990,124:217. |
| [22] | Meinhold R H;Bibby D M .[J].Zeolites,1990,10:146. |
| [23] | Meinhold R H;Bibby D M .[J].Zeolites,1990,10:74. |
| [24] | Demarquay J;Fraissard J .[J].Chemical Physics Letters,1987,136:314. |
| [25] | Cheung T T P;Fu C M .[J].Journal of Physical Chemistry,1989,93:3740. |
| [26] | Ito T;Bonardet J L;Fraissard J P;Nagy J B Andre C Gabelica Z Derouane E G .[J].Applied Catalysis,1988,43:L5. |
| [27] | Pradhan A R;Wu J F;Jong S J;Chen W H,Tsai T C.Liu S B .[J].Applied Catalysis A:General,1997,159:187. |
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%