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.
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Acknowledgments
This work was supported by the Division of Chemical Sciences, Office of Basic Energy Sciences, U.S. Department of Energy (USDOE). It was performed at Ames Laboratory which is operated for the USDOE by Iowa State University under Contract No. DE-AC02-07CH11358.
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Wang, J., Ackerman, D.M., Kandel, K. et al. Conversion Reactions in Surface-Functionalized Mesoporous Materials: Effect of Restricted Transport and Catalytic Site Distribution. MRS Online Proceedings Library 1423, 19–24 (2012). https://doi.org/10.1557/opl.2012.229
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DOI: https://doi.org/10.1557/opl.2012.229