采用晶种有机硅烷化法合成了纳米团簇ZSM-5沸石,考察了其在芳烃苄基化反应中的催化活性.X射线衍射、N2吸附和扫描电镜等结果表明,该沸石为由约20 nm的小晶粒聚集成的团簇体,并形成晶间中孔,其具有的外表面积是普通ZSM-5沸石的5倍之多.NH3-程序升温脱附和吡啶吸附的红外光谱结果显示,沸石的纳米化可使其表面酸中心,尤其是强酸中心的数目增多,大大提高了大分子的酸性位可接近性.在芳烃苄基化反应中,纳米ZSM-5沸石克服了反应分子空间位阻对催化活性的影响,表现出优异的催化活性,363 K时,甲苯苄基化反应的速率常数是普通ZSM-5沸石的约13倍.
参考文献
[1] | Díaz E;Ordó(n)ez S;Vega A;Auroux A Coca J .[J].Applied Catalysis A:General,2005,295:106. |
[2] | Commandeur R;Berger N;Jay P;Kervenal J .[P].EP 0 422986,1991. |
[3] | Iovel I;Mertins K;Kischel J;Zapf A,Beller M .[J].Angewandte Chemie International Edition,2005,44:3913. |
[4] | Coq B;Gourves V;Figueras F .[J].Applied Catalysis A:General,1993,100:69. |
[5] | Chaube V D .[J].Catalysis Communications,2004,5:321. |
[6] | 刘森,杜耘辰,肖霓,张永来,纪妍妍,肖丰收.一锅法合成介孔材料Fe-SBA-15及其对Friedel-Crafts苄基化反应的催化性能[J].催化学报,2008(05):468-472. |
[7] | Li Y;Zhang W H;Zhang L;Yang Q H Wei Zh B Feng Zh C Li C .[J].Journal of Physical Chemistry B,2004,108:9739. |
[8] | Okumura K;Nishigaki K;Niwa M .[J].Microporous and Mesoporous Materials,2001,44-45:509. |
[9] | Selvaraj M;Kawi S .An optimal direct synthesis of CrSBA-15 mesoporous materials with enhanced hydrothermal stability[J].Chemistry of Materials: A Publication of the American Chemistry Society,2007(3):509-519. |
[10] | 张泽凯,梁一微,任倩茹,刘华彦,陈银飞.高负载量LaMnOx/SBA-15的制备及其催化甲苯燃烧性能[J].催化学报,2011(02):250-257. |
[11] | Sun Y Y;Prins R .[J].Applied Catalysis A:General,2008,336:11. |
[12] | Christensen C H;Johannsen K;Schmidt I;Christensen C H .[J].Journal of the American Chemical Society,2003,125:13370. |
[13] | 祁晓岚,陈雪梅,孔德金,郑均林,袁晓红,杨德琴.介孔丝光沸石的制备及其对重芳烃转化反应的催化性能[J].催化学报,2009(12):1197-1202. |
[14] | Xiao F S;Wang L;Yin C;Lin K,Di Y,Li J,Xu R,Su D S,Schl(o)gl R,Yokoi T,Tatsumi T .[J].Angewandte Chemie International Edition,2006,45:3090. |
[15] | Song YQ;Zhu XX;Song Y;Wang QX;Xu LY .An effective method to enhance the stability on-stream of butene aromatization: Post-treatment of ZSM-5 by alkali solution of sodium hydroxide[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2006(1):69-77. |
[16] | Choi M;Cho H S;Srivastava R;Venkatesan C Choi D H Ryoo R .[J].Nature Materials,2006,5:718. |
[17] | 张志萍,赵岩,吴宏宇,谭伟,王祥生,郭新闻.改性纳米HZSM-5催化剂上甲苯与甲醇的烷基化反应[J].催化学报,2011(07):1280-1286. |
[18] | Covarrubias C;Gracia F;Palza H .[J].Applied Catalysis A:General,2010,384:186. |
[19] | Larsen S C .[J].Journal of Physical Chemistry C,2007,111:18464. |
[20] | Ivanova S;Louis B;Ledoux M J;Pham-Huu C .[J].Journal of the American Chemical Society,2007,129:3383. |
[21] | Serrano D P;Aguado J;Escola J M;Rodríguez J M Peral A .[J].Chemistry of Materials,2006,18:2462. |
[22] | Hibault-Starzyk F;Stan I;Abelló S;Bonilla A Thomas K Fernandez C Gilson J-P Pérez-Ramírez J .[J].Journal of Catalysis,2009,264:11. |
[23] | Selvaraj M;Lee T G .[J].J Mol CatalA,2005,243:176. |
[24] | Cui Sh H;Lu B;Cai Q H;Cai X J,Li X M,Xiao X,Hou L J,Han Y Y .[J].Industrial and Engineering Chemistry Research,2006,45:1571. |
[25] | Vinu A;Sawant D P;Ariga K;Hartmann M Halligudi S B .[J].Microporous and Mesoporous Materials,2005,80:195. |
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