将一种新型Gemini表面活性剂，丙撑基双(十八烷基二甲基氯化铵)[C18H37(CH3)2-N+-(CH2)3-N+-(CH3)2C18H37]Cl2(C18-3-18)，作为介孔模板剂用于水热法合成介孔ZSM-5分子筛。结果表明，在130oC低温晶化即可高效合成介孔ZSM-5分子刷。 C18-3-18的加入量可影响到所合成介孔ZSM-5分子筛的相对结晶度和织构性质，它的形成遵从一个转晶过程。在合成初期，凝胶中介孔模板剂C18-3-18的使用导向了介孔材料的生成；随后在TPABr的模板作用下，介孔材料慢慢转晶生成具有MFI结构的介孔ZSM-5；然后所合成的介孔ZSM-5晶粒进一步长大并聚集形成块状颗粒，同时产生晶间介孔。 C18-3-18作为介孔导向剂不仅可用于合成介孔ZSM-5分子筛，也可用于其它介孔分子筛的合成中。
A new gemini surfactant, [C18H37(CH3)2-N+-(CH2)3-N+-(CH3)2C18H37]Cl2 (C18-3-18), has been success-fully used as the mesopore directing agent in the hydrothermal synthesis of mesoporous ZSM-5 (MZSM-5). The synthesis of MZSM-5 was realized with a low temperature crystallization process at 130 °C. The amount of C18-3-18 used in the synthesis affected the relative crystallinity and the textural properties of the obtained MZSM-5. Detailed investigation showed that the formation of MZSM-5 followed a crystallization transformation process. The use of C18-3-18 resulted in the formation of mesoporous material during the early stage of the synthesis, which was converted into MZSM-5 crystals templated by tetrapropylammonium bromide to form the MFI phase. As the synthesis pro-ceeded, the MZSM-5 crystals aggregated into particles by weak interactions. This work shows that C18-3-18 can be used as a mesopore directing agent, which could provide a route for the synthesis of other mesoporous zeolites.
参考文献
| [1] | Serrano D P;Aguado J;Escola J M;Rodríguez J M Peral á .[J].CHEMISTRY OF MATERIALS,2006,18:2462. |
| [2] | Chal R;Gérardin C;Bulut M;van Donk S .[J].ChemCatChem,2011,3:67. |
| [3] | Na K;Choi M;Ryoo R .[J].Microporous and Mesoporous Materials,2013,166:3. |
| [4] | 李小云,孙明慧,ROOKE Joanna Claire,陈丽华,苏宝连.多级孔催化剂的合成及应用[J].催化学报,2013(01):22-47. |
| [5] | Zhang C M;Liu Q;Xu Z;Wang K S .[J].Microporous and Mesoporous Materials,2003,62:157. |
| [6] | Beers AEW.;van Bokhoven JA.;de Lathouder KM.;Kapteijn F.;Moulijn JA. .Optimization of zeolite Beta by steaming and acid leaching for the acylation of anisole with octanoic acid: a structure-activity relation[J].Journal of Catalysis,2003(2):239-248. |
| [7] | Viswanadham, N;Kumar, M .Effect of dealumination severity on the pore size distribution of mordenite[J].Microporous and Mesoporous Materials,2006(1/3):31-37. |
| [8] | 宋燕梅,任楠,唐颐.HCl处理后局部有序Y沸石的二次晶化[J].催化学报,2012(01):192-198. |
| [9] | Groen JC;Peffer LAA;Moulijn JA;Perez-Ramirez J .Mechanism of hierarchical porosity development in MFI zeolites by desilication: The role of aluminium as a pore-directing agent[J].Chemistry: A European journal,2005(17):4983-4994. |
| [10] | 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. |
| [11] | Triantafillidis C S;Vlessidis A G;Evmiridis N P .[J].Industrial and Engineering Chemistry Research,2000,39:307. |
| [12] | Jacobsen C J H;Madsen C;Houzvicka J;Schmidt I Carlsson A .[J].Journal of the American Chemical Society,2000,122:7116. |
| [13] | Tao Y S;Kanoh H;Kaneko K .[J].Journal of the American Chemical Society,2003,125:6044. |
| [14] | Zhao J J;Zhou J;Chen Y;He Q J Ruan M L Guo L M Shi J L Chen H R .[J].Journal of Materials Chemistry,2009,19:7614. |
| [15] | Zhu H B;Liu Z C;Wang Y D;Kong D J Yuan X H Xie Z K .[J].Chem Ma-ter,2008,20:1134. |
| [16] | Holland B T;Abrams L;Stein A .[J].Journal of the American Chemical Society,1999,121:4308. |
| [17] | Zhu, Y.;Hua, Z.;Zhou, J.;Wang, L.;Zhao, J.;Gong, Y.;Wu, W.;Ruan, M.;Shi, J. .Hierarchical mesoporous zeolites: Direct self-assembly synthesis in a conventional surfactant solution by kinetic control over the zeolite seed formation[J].Chemistry: A European journal,2011(51):14618-14627. |
| [18] | Wang Q Y;Xu S T;Chen J R;Wei Y X Li J Z Fan D Yu Z X Qi Y He Y L Xu S L Yuan C Y Zhou Y Wang J B Zhang M Z Su B L Liu Z M .[J].RSC Adv,2014,4:21479. |
| [19] | Zhou J;Hua Z L;Liu Z C;Wu W Zhu Y Shi J L .[J].ACS Catal,2011,1:287. |
| [20] | Serrano, D.P.;García, R.A.;Vicente, G.;Linares, M.;Procházková, D.;?ejka, J. .Acidic and catalytic properties of hierarchical zeolites and hybrid ordered mesoporous materials assembled from MFI protozeolitic units[J].Journal of Catalysis,2011(2):366-380. |
| [21] | Song JW;Ren LM;Yin CY;Ji YY;Wu ZF;Li JX;Xiao FS .Stable, porous, and bulky particles with high external surface and large pore volume from self-assembly of zeolite nanocrystals with cationic polymer[J].The journal of physical chemistry, C. Nanomaterials and interfaces,2008(23):8609-8613. |
| [22] | Wang H;Pinnavaia T J .[J].ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2006,45:7603. |
| [23] | Jin J J;Zhang X D;Li Y S;Li H Wu W Cui Y L Chen Q Li L Gu J L Zhao W R Shi J L .[J].Chemistry-A European Journal,2012,18:16549. |
| [24] | Choi M;Na K;Kim J;Sakamoto Y Terasaki O Ryoo R .[J].NATURE,2009,461:246. |
| [25] | Na, K;Choi, M;Park, W;Sakamoto, Y;Terasaki, O;Ryoo, R .Pillared MFI Zeolite Nanosheets of a Single-Unit-Cell Thickness[J].Journal of the American Chemical Society,2010(12):4169-4177. |
| [26] | Na K;Jo C;Kim J;Cho K Jung J Seo Y Messinger R J Chmelka B F Ryoo R .[J].SCIENCE,2011,333:328. |
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