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  • 1 College of Chemistry and Chemical Engineering, Hunan University, Changsha, Hunan, 410082, China
  • 2 Department of Chemistry, Hong Kong Baptist University, Kowloon Tong, Hong Kong
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Abstract

Described in this paper are the synthesis, characterization and catalytic application of H-ZSM-5 zeolites for the conversion of CH3Br into aromatics. The H-ZSM-5 zeolites were fabricated by hydrothermal crystallization using n-butylamine (BTA) as a template and characterized by XRD, SEM and NH3-TPD techniques. The effects of batch SiO2/Al2O3 ratio, alkalinity, NaCl/Al2O3 ratio, seed crystals, and crystallization time on the yield, structure/texture and catalytic performance were systematically studied. Adopting the optimum sol (SiO2/Al2O3 = 70, BTA/SiO2 = 0.2847, Na2O/SiO2 = 0.1237, H2O/SiO2 = 37.4, NaCl/Al2O3 = 60, and seed/SiO2 = 5 wt%) and under the most preferable crystallization conditions of 100 °C/24 h–170 °C/24 h, H-ZSM-5 zeolites of high crystallinity and small size (300–700 nm) were obtained. Good catalytic performance was observed over the H-ZSM-5 zeolites (aromatic yield up to 44.2%). However, unlike the modification of large commercial HZSM-5, the use of MoO3 or PbO as modifying agents for the small-size H-ZSM-5 zeolites results in a decline of catalytic performance. The relationship between the structure and the catalytic efficiency of as-synthesized H-ZSM-5 samples were investigated. It was found that with crystallinity enhancement and/or decline in crystal size, there is improvement of catalytic performance.

  • 1.

    Arakawa, H, Aresta, M, Armor, JN, Barteau, MA, Beckman, EJ, Bell, AT, Bercaw, JE, Creutz, C, Dinjus, E, Dixon, DA, Domen, K, DuBois, DL, Eckert, J, Fujita, E, Gibson, DH, Goddard, WA, Goodman, DW, Keller, J, Kubas, GJ, Kung, HH, Lyons, JE, Manzer, LE, Marks, TJ, Morokuma, K, Nicholas, KM, Periana, R, Que, L, Rostrup-Nielson, J, Sachtler, WMH, Schmidt, LD, Sen, A, Somorjai, GA, Stair, PC, Stults, BR, Tumas, W (2001) Chem Rev. 101:953 .

    • Crossref
    • Search Google Scholar
    • Export Citation
  • 2.

    Wang, LS, Tao, LX, Xie, MS, Xu, GF (1993) Catal Let. 21:35 .

  • 3.

    Zhang, JZ, Long, MA, Howe, RF (1998) Catal Today. 44:293 .

  • 4.

    Echevsky, GV, Kodenev, EG, Kikhtyanin, OV, Parmon, VN (2004) Appl Catal A: Gen. 258:159 .

  • 5.

    Weckhuysen, B, Wang, D, Rosynek, MP, Lunsford, JH (1998) J Catal. 175:338 .

  • 6.

    Pour, AN, Zare, M, Shahri, SMK, Zamani, Y, Alaei, MR (2009) J Nat Gas Sci Eng. 1:183 .

  • 7.

    Liu, S, Gujar, AC, Thomas, P, Toghiani, H, White, MG (2009) Appl Catal A: Gen. 357:18 .

  • 8.

    Olah, GA, Gupta, B, Farina, M, Felberg, JD, Ip, WM, Husain, A, Karpeles, R, Lammertsma, K, Melhotra, AK, Trivedi, NJ (1985) J Am Chem Soc. 107:7097 .

    • Crossref
    • Search Google Scholar
    • Export Citation
  • 9.

    Wei, YX, Zhang, DZ, Liu, ZM, Su, BL (2006) J Catal. 238:46 .

  • 10.

    Leandro, A, Noronha, E, Falabella, SA, Claudio, JAM (2005) Catal Today. 101:9 .

  • 11.

    Zhang, DZ, Wei, YX, Xu, L, Du, AP, Chang, FX, Su, BL, Liu, ZM (2006) Catal Let. 109:1 .

  • 12.

    Svelle, S, Aravinthan, S, Bjørgen, M, Lillerud, KP, Kolboe, S, Dahl, IM, Olsbye, U (2006) J Catal. 241:243 .

  • 13.

    Osterwalder, N, Stark, WJ (2007) Chem Phys Chem. 8:297.

  • 14.

    Lorkovic, IM, Sun, S, Gadewar, S, Breed, A, Macala, GS, Sardar, A, Cross, SE, Sherman, JH, Stucky, GD, Ford, PC (2006) J Phys Chem A. 110:8695 .

  • 15.

    Yilmaz, A, Zhou, XP, Lorkovic, IM, Laverman, GAYL, Weiss, M, Sun, SL, Schaefer, D, Sherman, JH, McFarland, EW, Ford, PC, Stucky, GD (2005) Microporous Mesoporous Mater. 79:205 .

    • Crossref
    • Search Google Scholar
    • Export Citation
  • 16.

    Xu, HF, Wang, KX, Li, WS, Zhou, XP (2005) Catal Lett. 100:53 .

  • 17.

    Wang, KX, Xu, HF, Li, WS, Zhou, XP (2005) J Mol Catal A. 225:65 .

  • 18.

    Wang, KX, Xu, HF, Li, WS, Au, CT, Zhou, XP (2006) Appl Catal A: Gen. 304:168 .

  • 19.

    Liu, Z, Huang, L, Li, WS, Yang, F, Au, CT, Zhou, XP (2007) J Mol Catal A. 273:14 .

  • 20.

    Tao, L, Chen, L, Yin, SF, Luo, SL, Ren, YQ, Li, WS, Zhou, XP, Au, CT (2009) Appl Catal A: Gen. 367:99 .

  • 21.

    Long, HY, Wang, XS, Sun, WF (2009) Microporous Mesoporous Mater. 119:18 .

  • 22.

    Zhang, WP, Han, XW, Liu, XC, Lei, H, Bao, XH (2001) Chem Commun. 1:293 .

  • 23.

    Zhang, WP, Han, XW, Liu, XC, Lei, H, Liu, XM, Bao, XH (2002) Microporous Mesoporous Mater. 53:145 .

  • 24.

    Sano, T, Ikeya, H, Kasuno, T (1997) Zeolites. 19:80 .

  • 25.

    Camblor, MA, Corma, A, Martinez, A, Mocholi, FA, Pariente, JP (1989) Appl Catal. 55:65 .

  • 26.

    R Van Grieken Sotelo, JL, Menendez, JM, Melero, JA (2000) Microporous Mesoporous Mater. 39:135 .

  • 27.

    Yamamura, M, Chaki, K, Wakatsuki, T, Okado, H, Fujimoto, K (1994) Zeolites. 14:643 .

  • 28.

    Song, YQ, Zhu, XX, Xie, SJ, Wang, QX, Xu, LY (2004) Catal Lett. 97:31 .

  • 29.

    Hayburst, DT, Evanina, G, Hunag, F (1990) J Chem. 64:295.

  • 30.

    Persson, AE, Schoeman, BJ, Sterte, J, Otterstedt, JE (1995) Zeolites. 15:611 .

  • 31.

    Lowe, BM, Nee, JRD, Casci, JL (1994) Zeolites. 14:610 .

  • 32.

    Padovan, M, Leofanti, G, Solari, M, Moretti, E (1984) Zeolites. 4:295 .

  • 33.

    Wang, Y, Tuel, A (2008) Microporous Mesoporous Mater. 113:286 .

  • 34.

    Narita, E, Sato, K, Yatabe, N, Okabe, T (1985) Ind Eng Chem Prod Res Dev. 24:507 .

  • 35.

    Szostak, R, Sieves, Molecular. 1989 Principles of synthesis and identification Van Nostrand Reinhold New York.

  • 36.

    Suzuki, K, Kiyozumi, Y, Matsuzaki, K, Shin, S (1988) Appl Catal. 42:35 .

  • 37.

    Kumara, N, Nieminen, V, Demirkan, K, Salmi, T, Murzin, D, Laine, E (2002) Appl Catal A: Gen. l235:113 .

  • 38.

    Mohamed, RM, Fouad, OA, Ismail, AA, Ibrahim, IA (2005) Mat Let. 59:344.

  • 39.

    Lechert, H, Staelin, P, Kuntz, C (1996) Zeolites. 16:149 .

  • 40.

    Yang, Z, Lin, YS (2000) Ind Eng Chem Res. 39:4944 .

  • 41.

    Narayanana, S, Sultanaa, A, Leb, QT, Aurouxb, A (1998) Appl Catal A: Gen. 168:373 .

  • 42.

    Shiralkar, VP, Joshi, PN, Eapen, MJ (1991) Zeolites. 11:511 .

  • 43.

    Wang, ZN, Yin, XZ, Xue, YF (1983) Chin Petrochem Technol. 12:744.

  • 44.

    Rollmann, LD, Schlenker, JL, Lawton, SL, Kennedy, CL, Kennedy, GJ, Doren, DJ (1999) J Phys Chem B. 103:7175 .

  • 45.

    Zhang, DZ, Wei, YX, Xu, L (2006) Natural Gas Cheml Ind. 31:42.

  • 46.

    Corma, A, González-Alfaro, V, Orchillés, AV (1999) Appl Catal A: Gen. 187:245 .

  • 47.

    Lobree, LJ, Hwang, IC, Reimer, JA, Bell, AT (1999) J Catal. 186:242 .

  • 48.

    Marschmeyer, S, Papp, H (1997) Surf Interface Anal. 25:660 .

  • 49.

    Dahl, IM, Kolboe, S (1994) J Catal. 149:458 .