화학공학소재연구정보센터
홈 로그인 로그아웃 연락처 사이트맵
Journal of Industrial and Engineering Chemistry, Vol.40, 128-136, August, 2016
DOI10.1016/j.jiec.2016.06.016  Export Citation
Hierarchical K/LTL zeolites: Synthesis by alkali treatment, characterization and catalytic performance in Knoevenagel condensation reaction
Nilesh P. Tangale, Shilpa K. Sonar, Prashant S. Niphadkar, and Praphulla N. Joshi†
  • Catalysis & Inorganic Chemistry Division, CSIR-National Chemical Laboratory, Dr. Homi Bhabha Road, Pashan, Pune 411008, India
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The hierarchical K/LTL zeolites prepared by post-synthesis modification with aqueous 1.5 M KOH solution by varying alkali volume to K/LTL zeolite (10-70 ml/g) ratios, were examined in Knoevenagel condensation. The physico-chemical properties of the catalysts were thoroughly evaluated by PXRD, FTIR, ICP, CO2-TPD, XPS, N2 adsorption/desorption and 29Si and 27Al MAS-NMR. Among all the samples, hierarchical K/LTL prepared by treating K/LTL with 50 ml aqueous 1.5 M KOH solution per gram of K/LTL displayed about 1.5 fold higher catalytic activity as compared to parent K/LTL, presumably because of combined effect of enhanced basicity and molecular diffusion through pore channels.
Keywords:K/LTL;Hierarchical zeolite;Micro-mesoporous composite;Knoevenagel condensation;Basicity
  1. Pullabhotla VSSR, Rahman A, Jonnalagadda SB, Catal. Commun., 10, 365 (2009)
  2. Jain D, Khatri C, Rani A, Fuel, 90(6), 2083 (2011)
  3. Beutler U, Fuenfschilling PC, Steinkemper A, Org. Process Res. Dev., 11, 341 (2007)
  4. Tietze LF, Chem. Rev., 96(1), 115 (1996)
  5. Freeman F, Chem. Rev., 80, 329 (1980)
  6. Marciniak G, Delgado A, Leclerc G, Velly J, Decker N, Schwartz J, J. Med. Chem., 32, 1402 (1989)
  7. Angelescu E, Pavel OD, Birjega R, Zavoianu R, Costentin G, Che M, Appl. Catal. A: Gen., 308, 13 (2006)
  8. Al-Shihry SS, Molecules, 9, 658 (2004)
  9. Corma A, Iborra S, Primo J, Rey F, Appl. Catal. A: Gen., 114(2), 215 (1994)
  10. Sharma SK, Parikh PA, Jasra RV, J. Mol. Catal. A-Chem., 278(1-2), 135 (2007)
  11. Zhang Y, Xia CG, Appl. Catal. A: Gen., 366(1), 141 (2009)
  12. Corma A, Iborra S, Rodriguez I, Sanchez F, J. Catal., 211(1), 208 (2002)
  13. Almeida KA, Cardoso D, Catal. Today, 213, 122 (2013)
  14. Lai SM, Ng CP, Aranda RM, Yeung KL, Microporous Mesoporous Mater., 66, 239 (2003)
  15. Martins L, Holderich W, Cardoso D, J. Catal., 258(1), 14 (2008)
  16. Martins L, Vieira KM, Rios LM, Cardoso D, Catal. Today, 133-135, 706 (2008)
  17. Beers AEW, van Bokhoven JA, de Lathouder KM, Kapteijn F, Moulijn JA, J. Catal., 218(2), 239 (2003)
  18. Muller M, Harvey G, Prins R, Microporous Mesoporous Mater., 34, 135 (2000)
  19. Groen JC, Jansen JC, Moulijn JA, Perez-Ramirez J, J. Phys. Chem. B, 108(35), 13062 (2004)
  20. Verboekend D, Keller TC, Milina M, Hauert R, Pe´rez-Ramı´rez J, Chem. Mater., 25, 1947 (2013)
  21. Kulawong S, Prayoonpokarach S, Neramittagapong A, Wittayakun J, J. Ind. Eng. Chem., 17(2), 346 (2011)
  22. Hao K, Shen B, Wang Y, Ren J, J. Ind. Eng. Chem., 18(5), 1736 (2012)
  23. Saceda JJF, Rintramee K, Khabuanchalad S, Prayoonpokarach S, de Leon RL, Wittayakun J, J. Ind. Eng. Chem., 18(1), 420 (2012)
  24. Saxena SK, Viswanadham N, Garg MO, J. Ind. Eng. Chem., 20(5), 3875 (2014)
  25. Schmidt F, Lohe MR, Buchner B, Giordanino F, Bonino F, Kaskel S, Microporous Mesoporous Mater., 165, 148 (2013)
  26. Tsai ST, Chen CH, Tsai TC, Green Chem., 11, 1349 (2009)
  27. Groen JC, Abello A, Villaescusa LA, Perez-Ramirez J, Microporous Mesoporous Mater., 14, 93 (2008)
  28. Verboekend D, Keller TC, Mitchell S, Perez-Ramirez J, Adv. Funct. Mater., 23(15), 1923 (2013)
  29. Garces LJ, Makwana VD, Hincapie B, Sacco A, Suib SL, J. Catal., 217(1), 107 (2003)
  30. Barrer RM, Villiger H, Z. Krostallogr., 128, 352 (1969)
  31. Bhat SD, Niphadkar PS, Gaydhankar TS, Awate SV, Belhekar AA, Joshi PN, Microporous Mesoporous Mater., 76, 81 (2004)
  32. Weeks TJ, Bolton AP, J. Phys. Chem., 79, 1924 (1975)
  33. Bartl P, Holderich WF, Microporous Mesoporous Mater., 38, 279 (2000)
  34. Sadowska K, Gora-Marek K, Drozdek M, Kustrowski P, Datka J, Martinez-Triguero J, Rrey F, Microporous Mesoporous Mater., 168, 195 (2013)
  35. Groen JC, Peffer LAA, Moulijn JA, Perez-Ramirez J, Colloids Surf. A: Physicochem. Eng. Asp., 241, 53 (2004)
  36. Wei X, Smirniotis PG, Microporous Mesoporous Mater., 97, 97 (2006)
  37. Devi R, Borah R, Deka RC, Appl. Catal. A: Gen., 433-434, 122 (2012)
  38. Mao RLD, Ransaran A, Xiao S, Yao J, Semmer V, J. Mater. Chem., 5, 533 (1995)
  39. Joshi PN, Jacob NE, Shiralkar VP, J. Phys. Chem., 99(12), 4225 (1995)
  40. Oldfield E, Kirkpatrick RJ, Science, 227, 1537 (1985)
  41. Fyfe CA, Wasylislen RE, in: Cheetham AK, Day P (Eds.), Solid State Chemistry Techniques, Oxford Scientific, 1988, p. 190.
  42. Bonilla A, Baudouin D, Perez-Ramirez J, J. Catal., 265(2), 170 (2009)
  43. Barthomeuf D, Microporous Mesoporous Mater., 66, 1 (2003)
  44. Almeida KA, Landers R, Cardoso D, J. Catal., 294, 151 (2012)
  45. Kotwal MS, Niphadkar PS, Deshpande SS, Bokade VV, Joshi PN, Fuel, 88(9), 1773 (2009)
  46. Birla A, Singh B, Upadhyay SN, Sharma YC, Bioresour. Technol., 106, 95 (2012)
  47. Lai SM, Ng CP, Martin-Aranda R, Yeung KL, Microporous Mesoporous Mater., 66, 239 (2003)
  48. Reddy TI, Verma RS, Tetrahedron Lett., 38, 1721 (1997)
  49. Saravanamurugan S, Palanichamy M, Hartmann M, Murugesan V, Appl. Catal. A: Gen., 298, 8 (2006)
  50. Ernst S, Hartmann M, Sauerbeck S, Bongers T, Appl. Catal. A: Gen., 200(1-2), 117 (2000)
  51. Srasra M, Delsarte S, Gaigneaux EM, Top. Catal., 52, 1541 (2009)
  52. Verboekend D, Keller TC, Milina M, Hauert R, Pe´rez-Ramı´rez J, Chem. Mater., 25, 1947 (2013)
  53. Zhang CM, Xu Z, Wan K, Liu Q, Appl. Catal. A: Gen., 258(1), 55 (2004)