Synthesis of Micro-Mesoporous Ti-MOR/Silica Composite Spheres in Oil-in-water Microemulsion System

Abstract

The hierarchically structured micro-mesoporous spheres(MMS) composed of mesoporous silica and Ti-containing mordenite (Ti-MOR) zeolite were self-assembled in an oil-in-water microemulsion system containing tetrabutyl orthosilicate as silica source, cetyltrimethylammonium bromide as template and aluminum sulfate as additive. The composite materials possessed the connatural microporosity of zeolite together with the disordered mesopores(5.41 nm) in silica part. With a special focus on the importance of aluminum sulfate additive, a possible formation mechanism has been proposed, in which double electrostatic interactions played the crucial role of mediating the mesosilica species and zeolite crystals. The obtained MMS materials, with a tunable particle dimension(250–720 µm) and a changeable content of active component Ti-MOR(44%–70%), showed enhanced catalytic activity and lifetime in the liquid-phase ammoximation of cyclohexanone in comparison to the parent Ti-MOR powder.

Keywords

Micro-mesoporous composite sphere / Microemulsion / Mordenite / Aluminum sulfate / Double electrostatic interaction

References

[1] Le T T, Chawla A, Rimer J D. J. Catal., 2020, 391: 56.

[2] Xu H, Wu P. Chin. J. Chem., 2017, 35: 836.

[3] Liu L, Corma A. Nature Rev. Mater., 2021, 6: 244.

[4] Ding J, Wu P. Appl. Catal. A, 2014, 488: 86.

[5] Yang Y L, Ding J H, Wang B S, Wu J, Zhao C, Gao G H, Wu P. J. Catal., 2014, 320: 160.

[6] Xu H, Zhang Y T, Wu H H, Liu Y M, Li X H, Jiang J G, He M Y, Wu P. J. Catal., 2011, 281: 263.

[7] Serrano D P, Sanz R, Pizarro P, Moreno I, Blázquez S. Catal. Today, 2009, 143: 151.

[8] Shan Z C, Lu Z D, Wang L, Zhou C, Ren L M, Zhang L, Meng X J, Ma S J, Xiao F S. ChemCatChem, 2010, 2: 407.

[9] Itani L, Valtchev V, Patarin J, Rigolet S, Gao F F, Baudin G. Micropor. Mesopor. Mater., 2011, 138: 157.

[10] Choudhary V R, Devadas P, Kinage A K, Guisnet M. Appl. Catal. A, 1997, 162: 223.

[11] Canizares P, Duran A, Dorado F, Carmona M. Appl. Clay Sci., 2000, 16: 273.

[12] Dorado F, Romero R, Canizares P. Ind. Eng. Chem. Res., 2001, 40: 3428.

[13] Dorado F, Romero R, Canizares P. Appl. Catal. A: General., 2002, 236: 235.

[14] Choudhary V R, Kinage A K, Sivadinarayana C, Devadas P, Sansare S D, Guisnet M. J. Catal., 199, 158: 34.

[15] Choudhary V R, Devadas P, Kinage A K, Sivadinarayana C, Guisnet M. J. Catal., 199, 158: 537.

[16] Evilevitch A, Lobaskin V, Olsson U, Linsen P, Schurtenberger P. Langmuir, 2001, 17: 1043.

[17] Nagarajan R. Langmuir, 2000, 16: 6400.

[18] Paul K B, Moulik S P. J. Dispersion Sci. Technol., 1997, 18: 301.

[19] Dutta P K, Robins D. Langmuir, 1991, 7: 1048.

[20] Dutta P K, Jakupca M, Reddy K S N, Salvati L. Nature, 1995, 374: 44.

[21] Singh R, Doolittle J, George M A, Dutta P K. Langmuir, 2002, 18: 8193.

[22] Yates M Z, Ott K C, Birnbaum E R, McCleskey T M. Angew. Chem. Int. Ed., 2002, 41: 476.

[23] Lin J-C, Dipre J T, Yates M Z. Chem. Mater., 2003, 15: 2764.

[24] Lin J-C, Dipre J T, Yates M Z. Langmuir, 2004, 20: 1039.

[25] Lin J-C, Yates M Z. Langmuir, 2005, 21: 2117.

[26] Lee S, Shantz D F. Chem. Mater., 2005, 17: 409.

[27] Schacht S, Huo Q, Voigt-Martin I G, Stucky G D, Schüth F. Science, 199, 273: 768.

[28] Huo Q, Feng J, Schüth F, Stucky G D. Chem. Mater., 1997, 9: 14.

[29] Schmidt-Winkel P, Lukens W W Jr., Zhao D, Yang P, Chmelka B F, Stucky G D. J. Am. Chem. Soc., 1999, 121: 254.

[30] Schmidt-Winkel P, Glinka C J, Stucky G D. Langmuir, 2000, 16: 356.

[31] Sun B, Guo Y, Xu L, Huang Z H, Wu P, Che S A. Acta Chim. Sinica, 2012, 70: 2419.

[32] Wu P, Komatsu T, Yashima T. J. Catal., 1997, 168: 400.

[33] Ban S, Laak A N C, Landers J, Neimark A V, Jongh P E, Jong K P, Vlugt T J H. J. Phys. Chem. C, 2010, 114: 2056.