Skip to main content Accessibility help
×
Home

Conversion Reactions in Surface-Functionalized Mesoporous Materials: Effect of Restricted Transport and Catalytic Site Distribution

  • Jing Wang (a1) (a2), David M. Ackerman (a1) (a3), Kapil Kandel (a1) (a3), Igor I. Slowing (a1), Marek Pruski (a1) (a3) and James W. Evans (a1) (a2) (a4)...

Abstract

We analyze the interplay between anomalous transport and conversion reaction kinetics in mesoporous materials functionalized with catalytic groups. Of primary interest is functionalized mesoporous silica containing an array of linear pores with diameters tunable from 2-10 nm, although functionalization can produce smaller effective diameters, d. For d < 2 nm, transport and specifically passing of reactant and product species within the pores can be strongly inhibited (single-file diffusion). The distribution of catalytic groups can also vary depending on the synthesis approach. We apply statistical mechanical modeling (utilizing spatially discrete stochastic lattice-gas models) to explore the dependence of reactivity on the extent of inhibition of passing of species within the pore, as well as on the distribution of catalytic sites.

Copyright

References

Hide All
1. Catalysis and Adsorption by Zeolites; Ohlmann, G., Pfeifer, H., Fricke, G., Eds.; Elsevier, Amsterdam, 1991.
2. Tajima, K. and Aida, T., Nanostructured Catalysts, Plenum, New York, 2003.
3. Beck, J.S., Vartulli, J.C., Roth, W.J., Leonowicz, M.E., Kresge, C.T., Schmitt, K.D., Chu, C.T.W., Olson, D.H., and Sheppard, E.W., J. Am. Chem. Soc. 114, 1083410843 (1992).
4. Huh, S., Wiench, J.W., Woo, J.-C., Pruski, M., and Lin, V.S.-Y., Chem. Mater. 15, 4247 (2003).
5. Tsai, C.-H., Chen, H.-T., Althaus, S.M., Mao, K., Kobayashi, T., Pruski, M., and Lin, V.S.-Y., ACS Cat. 1, 729 (2011).
6. Harris, T.E., J. Appl. Prob. 2, 323 (1965).
7. Kärger, J. and Freude, D., Chem. Eng. Technol. 25, 769 (2002).
8. Tsikoyiannis, J.G. and Wei, J.E., Chem. Eng. Sci, 46, 233 (1991).
9. Kärger, J., Petzold, M., Pfieffer, H.S., Ernst, S., and Weitkamp, J., J. Catal. 136, 283 (1992).
10. Rodenbeck, C., Kärger, J., and Hahn, K., Phys. Rev. E 55, 5697 (1997).
11. Okino, M.S., Snurr, R.Q., Kung, H.H., Ochs, J.E., and Mavrovouniotis, M.L., J. Chem. Phys. 111, 2210 (1999).
12. Nedea, S.V., Jansen, A.P.J., Lukkien, J.J, and Hilbers, P.A.J., Phys. Rev. E 65, 066701 (2002).
13. Ackerman, D.M., Wang, J., Wendel, J.H., Liu, D.-J., Pruski, M., and Evans, J.W., J. Chem. Phys. 134, 114107 (2011).
14. Liu, D.-J., Wang, J., Ackerman, D.M., Slowing, I.I., Pruski, M., Chen, H.-T., Lin, V.S.-Y., and Evans, J.W., ACS Catalysis 1, 751 (2011).
15. Ackerman, D.M., Wang, J., and Evans, J.W., Phys. Rev. Lett., submitted (2012).
16. Kutner, R., Phys. Lett. 81A, 239 (1981).

Keywords

Conversion Reactions in Surface-Functionalized Mesoporous Materials: Effect of Restricted Transport and Catalytic Site Distribution

  • Jing Wang (a1) (a2), David M. Ackerman (a1) (a3), Kapil Kandel (a1) (a3), Igor I. Slowing (a1), Marek Pruski (a1) (a3) and James W. Evans (a1) (a2) (a4)...

Metrics

Full text views

Total number of HTML views: 0
Total number of PDF views: 0 *
Loading metrics...

Abstract views

Total abstract views: 0 *
Loading metrics...

* Views captured on Cambridge Core between <date>. This data will be updated every 24 hours.

Usage data cannot currently be displayed