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Adsorption and Diffusion pp 277–328Cite as

Positron Emission Profiling: a Study of Hydrocarbon Diffusivity in MFI Zeolites

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Part of the book series: Molecular Sieves ((SIEVES,volume 7))

Abstract

Zeolites are of prime importance to the petrochemical industry as catalysts for hydrocarbon conversion. In their molecule-sized micropores, hydrocarbon diffusion plays a pivotal role in the final catalytic performance. Here, we present the results of Positron Emission Profiling experiments with labeled hydrocarbons in zeolites with the MFI morphology. Single-component self-diffusion coefficients of hexanes in silicalite-1 and its acidic counterpart H-ZSM-5 are determined. For the first time, self-diffusion coefficients of n-pentane and n-hexane in mixtures are studied. This shows that Positron Emission Profiling is a powerful technique for in situ investigations of the adsorptive and diffusive properties of hydrocarbons in zeolites. The diffusion of hydrocarbons in medium-pore zeolites is determined by a complex interplay of factors such as the loading, the temperature, the preference for certain pore locations, the interactions with other hydrocarbon molecules of the same type or of other types and the presence of acid protons. In the diffusion of mixtures, pore blockage by one of the components might occur, thus strongly decreasing the diffusivity of the faster diffusing hydrocarbon.

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References

  1. Baerlocher C, Meier WM, Olson DH (2001) Atlas of zeolite framework types, 5th ed. Elsevier, Amsterdam, The Netherlands

    Google Scholar 

  2. Jost W (1960) Diffusion in solids, liquids and gases. Academic Press, New York

    Google Scholar 

  3. Kärger J, Ruthven DM (1992) Diffusion in zeolites and other microporous solids. John Wiley & Sons, Inc, New York

    Google Scholar 

  4. Chen NY, Degnan TF Jr, Smith CM (1994) Molecular transport and reaction in zeolites design and application of shape selective catalysis. VCH Publishers, New York

    Google Scholar 

  5. Benes NE, Verweij H (1999) Langmuir 15:8292

    Article  CAS  Google Scholar 

  6. Kauzmann W (1966) Kinetic theory of gases. Addison-Wesley, Reading

    Google Scholar 

  7. Post MFM (1991) In: Van Bekkum H, Flanigen EM, Jansen JC (eds) Introduction to zeolite science and practice. Elsevier, Amsterdam, pp 391–443

    Chapter  Google Scholar 

  8. Post MFM (1991) Stud Surf Sci Catal 58:391

    Article  CAS  Google Scholar 

  9. Wakao N, Kaguei S (1982) Heat and mass transfer in packed beds. Gordon and Breach Science, London

    Google Scholar 

  10. Weisz PB (1973) Chem Tech 3:498

    CAS  Google Scholar 

  11. Fick A (1855) Ann Phys 94:59

    Google Scholar 

  12. Barrer RM, Jost W (1949) Trans Faraday Soc 45:928

    Article  CAS  Google Scholar 

  13. Einstein A (1905) Ann Phys 17:549

    Article  CAS  Google Scholar 

  14. Paschek D, Krishna R (2001) Chem Phys Lett 333:278

    Article  CAS  Google Scholar 

  15. Skoulidas AI, Sholl DS (2001) J Phys Chem B 105:3151

    Article  CAS  Google Scholar 

  16. Barrer RM (1941) Trans Faraday Soc 37:590

    Article  CAS  Google Scholar 

  17. Theodorou DN, Wei J (1983) J Catal 83:205

    Article  CAS  Google Scholar 

  18. Tsikoyiannis J, Wei J (1991) Chem Eng Sci 46:233

    Article  CAS  Google Scholar 

  19. Coppens MO, Bell AT, Chakraborty AK (1998) Chem Eng Sci 53:2053

    Article  CAS  Google Scholar 

  20. Kärger J, Pfeifer H (1987) Zeolites 7:90

    Article  Google Scholar 

  21. Xiao J, Wei J (1992) Chem Eng Sci 47:1123

    Article  CAS  Google Scholar 

  22. Riekert L (1970) Adv Catal 21:281

    Article  CAS  Google Scholar 

  23. Koriabkina AO, De Jong AM, Schuring D, Van Santen RA (2002) J Phys Chem B 106:9559

    Article  CAS  Google Scholar 

  24. Haynes HW, Sarma PN (1973) AIChE J 19:1043

    Article  CAS  Google Scholar 

  25. Noordhoek NJ, Van Ijzendoorn NJ, Anderson BG, De Gauw FJ, Van Santen RA, De Voigt MJA (1998) Ind Eng Chem Res 37:825

    Article  CAS  Google Scholar 

  26. Mangnus AVG (2000) A detection system for Positron Emission Profiling, Ph.D. thesis. Eindhoven University of Technology, Eindhoven, The Netherlands

    Google Scholar 

  27. Ferrieri RA, Wolf AP (1984) J Phys Chem 88:2256

    Article  CAS  Google Scholar 

  28. Ferrieri RA, Wolf AP (1984) J Phys Chem 88:5456

    Article  CAS  Google Scholar 

  29. Baltensperger U, Ammann M, Bochert UK, Eichler B, Gäggeler HW, Jost DT, Kovacs JA, Türler A, Sherer UW, Baiker A (1993) J Phys Chem 97:12325

    Article  CAS  Google Scholar 

  30. Hawkesworth MR, Parker DJ, Fowles P, Crilly JF, Jefferies NL, Jonkers G (1991) Nucl Instrum Methods A310:423

    CAS  Google Scholar 

  31. Hensel F (1996) Institut Sicherheitsforschung, Forschungszentrum Rossendorf, Dresden D-01314, Germany. FZR, FZR-152, p 12

    Google Scholar 

  32. Jonkers G, Vonkeman KA, Van der Wal SWA, Van Santen RA (1992) Nature 355:63

    Article  CAS  Google Scholar 

  33. Jonkers G, Vonkeman KA, Van der Waal SWA (1993) In: Weijnen MPC, Drinkenburg AAH (eds) Precision Process Technology. Kluwer Academic Publishers, The Netherlands, p 533

    Google Scholar 

  34. Mangnus AVG, Van Ijzendoorn LJ, De Goeij JJM, Cunningham RH, Van Santen RA, De Voigt MJA (1995) Nucl Instrum Methods B99:649

    Google Scholar 

  35. Schumacher RR, Anderson BG, Noordhoek NJ, De Gauw FJMM, De Jong AM, De Voigt MJA, Van Santen RA (2001) Microporous Mesoporous Mater 35–36:315

    Google Scholar 

  36. Noordhoek NJ, Schuring D, De Gauw FJMM, Anderson BG, De Jong AM, De Voigt MJA, Van Santen RA (2002) Ind Eng Chem Res 41:1973

    Article  CAS  Google Scholar 

  37. Cunningham RH, Mangnus AVG, Van Grondelle J, Van Santen RA (1996) J Mol Catal A 107:153

    Article  CAS  Google Scholar 

  38. Rosen JB (1952) J Chem Phys 20:387

    Article  CAS  Google Scholar 

  39. Nijhuis TA, Van den Broeke LJP, Linders MJG, Van de Graaf JM, Kapteijn F, Makkee M, Moulijn JA (1999) Chem Eng Sci 54:4423

    Article  CAS  Google Scholar 

  40. Hong U, Kärger J, Kramer R, Pfeifer H, Seiffert G, Müller U, Unger KK, Lück HB, Ito T (1991) Zeolites 11:816

    Article  CAS  Google Scholar 

  41. Schiesser WE (1991) The Numerical Method of Lines: Integration of Partial Differential Equations. Academic Press, San Diego

    Google Scholar 

  42. Marquardt D (1963) J Appl Math 11:431

    Google Scholar 

  43. Atkins PW, De Paula J (2002) Physical Chemistry, 7th ed. Oxford University Press, Oxford, United Kingdom, pp 822–824

    Google Scholar 

  44. Vlugt TJH, Krishna R, Smit B (1999) J Phys Chem B 103:1102

    Article  CAS  Google Scholar 

  45. Zhu W, Kapteijn F, Moulijn JA (2001) Microporous Mesoporous Mater 47:157

    Article  CAS  Google Scholar 

  46. June RL, Bell AT, Theodorou DN (1992) J Phys Chem B 96:1051

    Article  CAS  Google Scholar 

  47. June RL, Bell AT, Theodorou DN (1990) J Phys Chem B 94:1508

    Article  CAS  Google Scholar 

  48. Zhu W, Kapteijn F, Van der Linden B, Moulijn JA (2001) Phys Chem Chem Phys 3:1755

    Article  CAS  Google Scholar 

  49. Calero S, Smit B, Krishna R (2001) J Catal 202:395

    Article  CAS  Google Scholar 

  50. Schuring D, Koriabkina AO, De Jong AM, Smit B, Santen RA (2001) J Phys Chem B 105:7690

    Article  CAS  Google Scholar 

  51. Breck DW (1974) Zeolite Molecular Sieves. John Wiley, New York

    Google Scholar 

  52. Snurr RQ, Kärger J (1997) J Phys Chem B 101:64

    Article  Google Scholar 

  53. Schuring D, Jansen APJ, Van Santen RA (2000) J Phys Chem B 104:941

    Article  CAS  Google Scholar 

  54. Jost S, Bar NK, Fritzsche S, Haberlandt R, Kärger J (1998) J Phys Chem B 102:6375

    Article  CAS  Google Scholar 

  55. Masuda T, Fujikata Y, Ikeda H, Hashimoto K (2000) Microporous Mesoporous Mater 38:323

    Article  CAS  Google Scholar 

  56. Gergidis LN, Theodorou DN (1999) J Phys Chem B 103:3380

    Article  CAS  Google Scholar 

  57. Nivarthi SS, Davis HT, McCormick AV (1995) Chem Eng Sci 50:3217

    Article  CAS  Google Scholar 

  58. Förste C, Germanus A, Kärger J, Pfeifer H, Caro J, Pilz W, Zikánová A (1987) J Chem Soc Faraday Trans 83:2301

    Article  Google Scholar 

  59. Eder F (1996) Thermodynamics and siting of alkane sorption in molecular sieves, Ph.D.Thesis. University of Twente, The Netherlands

    Google Scholar 

  60. Wu P, Debebe A, Ma Y (1983) Zeolites 3:118

    Article  CAS  Google Scholar 

  61. Anderson J, Foger K, Mole T, Rajadhyaksha R, Sanders J (1979) J Catal 58:114

    Article  CAS  Google Scholar 

  62. Valyon J, Onyestyak G, Rees LVC (2000) In: Proc of 2nd Pac Basin Conf, p 482

    Google Scholar 

  63. Zikanova A, Bülow M, Schlodder H (1987) Zeolites 7:11

    Article  Google Scholar 

  64. Shen D, Rees LVC (1991) Zeolites 11:666

    Article  CAS  Google Scholar 

  65. Masuda T, Fujikata Y, Nishida T, Hashimoto K (1998) Microporous Mesoporous Mater 23:157

    Article  CAS  Google Scholar 

  66. Jost S, Bar NK, Fritzshe S, Haberlandt R, Kärger J (1999) In: Treacy MMC, Marcus BK, Bisher ME, Higgins JB (eds) Proc 12th Int Zeolite Conf, Baltimore, USA, July 5–10, 1998. Materials Research Society, Warrendale PA, USA, p 149

    Google Scholar 

  67. Bülow M, Schodder H, Rees LVC, Caro J, Richards R (1986) In: Murakami Y, Iijima A, Ward JW (eds) New developments in zeolite science and technology; Proc. 7th Int Zeolite Conf, Tokyo, Japan, 1986. Elsevier, Amsterdam, pp 579–586

    Google Scholar 

  68. Bülow M, Schodder H, Rees LVC, Caro J, Richards R (1986) Stud Surf Sci Catal 28:579

    Article  Google Scholar 

  69. Hashimoto K, Masuda T, Murakami N (1991) In: Jacobs PA, Jäger NI, Kubelkova L, Wichterlova B (eds) Zeolite Chemistry and Catalysis; Proc Int Symp, Prague, Czechoslovakia, September 8–13, 1991. Elsevier, Amsterdam, p 477

    Google Scholar 

  70. Hermann M, Niessen W, Karge HG (1996) In: LeVan MD (ed) Fundamentals of adsorption; Proc 5th Int Conf Fundamentals of adsorption, Asilomar Pacific Grove, California, USA, May 13–18, 1995. Kluwer Acad Publ Norwell, Mas, pp 377–384

    Google Scholar 

  71. Hermann M, Niessen W, Karge HG (1995) In: Beyer HK, Karge HG, Kiricsi I, Nagy JB (eds) Proc Int Symp Catalysis by Microporous Materials, Elsevier, Amsterdam, pp 131–138

    Google Scholar 

  72. Hermann M, Niessen W, Karge HG (1995) Stud Surf Sci Catal 94:131

    Article  CAS  Google Scholar 

  73. Van-Den-Begin N, Rees LVC, Caro J, Bülow M (1989) Zeolites 9:287

    Article  CAS  Google Scholar 

  74. Eic M, Ruthven DM (1989) In: Jacobs PA, Van Santen RA (eds) Zeolites: Facts, figures, future; Proc. 8th Int Zeolite Conf, Amsterdam, The Netherlands, 1989. Elsevier, Amsterdam, p 897

    Google Scholar 

  75. Eic M, Ruthven DM (1989) Stud Surf Sci Catal 49:897

    Article  Google Scholar 

  76. Millot B, Methivier A, Jobic H, Moueddeb H, Dalmon JA (2000) Microporous Mesoporous Mater 38:85

    Article  CAS  Google Scholar 

  77. Cavalcante CL, Ruthven DM (1995) Ind Eng Chem Res 34:185

    Article  CAS  Google Scholar 

  78. Xiao J, Wei J (1992) Chem Eng Sci 47:1143

    Article  CAS  Google Scholar 

  79. Keipert OP, Baerns M (1998) Chem Eng Sci 53:3623

    Article  CAS  Google Scholar 

  80. Coppens MO, Bell AT, Chakraborty AK (1999) Chem Eng Sci 54:3455

    Article  CAS  Google Scholar 

  81. Koriabkina AO, De Jong AM, Hensen EJM, Van Santen RA (2004) Microporous Mesoporous Mat 77:119

    Article  CAS  Google Scholar 

  82. Paschek D, Krishna R (2001) Chem Phys Lett 342:148

    Article  CAS  Google Scholar 

  83. Trout BL, Chakraborty AK, Bell AT (1997) Chem Eng Sci 52:2265

    Article  CAS  Google Scholar 

  84. Krishna R, Paschek D (2002) Chem Eng J 85:715

    Article  Google Scholar 

  85. Smit B, Maesen T (1995) Nature 374:42

    CAS  Google Scholar 

  86. Heink W, Kärger J, Pfeifer H, Datema KP, Nowak AK (1992) J Chem Soc Faraday Trans 88:3505

    Article  CAS  Google Scholar 

  87. Datema KP, Den Ouden CJJ, Ylstra WD, Kuipers HPCE, Post MFM, Kärger J (1991) J Chem Soc Faraday Trans 87:1935

    Article  CAS  Google Scholar 

  88. Hayhurst DT, Paravar A (1988) Zeolites 8:27

    Article  CAS  Google Scholar 

  89. Song L, Rees LVC (1999) In: Treacy MMC, Marcus BK, Bisher ME, Higgins JB (eds) Proc 12th Int Zeolite Conf, Baltimore, USA, July 5–10, 1998. Materials Research Society, Warrendale PA, USA, p 67

    Google Scholar 

  90. Talu O, Sun MS, Shah DB (1998) AIChE J 44:681

    Article  CAS  Google Scholar 

  91. Van de Graaf JM, Kapteijn F, Moulijn JA (2000) Microporous Mesoporous Mater 35–36:267

    Article  Google Scholar 

  92. Nijhuis TA, Van den Broeke LJP, Van de Graaf JM, Kapteijn F, Makkee M, Moulijn JA (1997) Chem Eng Sci 52:3401

    Article  CAS  Google Scholar 

  93. Sun MS, Talu O, Shah DB (1996) J Phys Chem B 100:17276

    Article  CAS  Google Scholar 

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Authors and Affiliations

  1. Schuit Institute of Catalysis, Faculty of Chemical Engineering and Chemistry, Eindhoven University of Technology, PO Box 513, 5600MB, Eindhoven, The Netherlands

    E. J. M. Hensen & R. A. van Santen

  2. Accelerator Laboratory, Schuit Institute of Catalysis, Faculty of Technical Physics, Eindhoven University of Technology, PO Box 513, 5600MB, Eindhoven, The Netherlands

    A. M. de Jong

Authors
  1. E. J. M. Hensen
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  2. A. M. de Jong
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  3. R. A. van Santen
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Correspondence to E. J. M. Hensen .

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Hellmut G. Karge Jens Weitkamp

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Hensen, E.J.M., de Jong, A.M., van Santen, R.A. (2007). Positron Emission Profiling: a Study of Hydrocarbon Diffusivity in MFI Zeolites. In: Karge, H.G., Weitkamp, J. (eds) Adsorption and Diffusion. Molecular Sieves, vol 7. Springer, Berlin, Heidelberg. https://doi.org/10.1007/3829_2007_014

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