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Multi-functionalization of nanoporous catalytic materials to enhance reaction yield: Statistical mechanical modeling for conversion reactions with restricted diffusive transport

  • Jing Wang (a1) (a2), Andrés Garcia (a1) (a3), David M. Ackerman (a1), Mark S. Gordon (a1) (a4), Igor I. Slowing (a1) (a4), Takeshi Kobayashi (a1), Marek Pruski (a1) (a4) and James W. Evans (a1) (a2) (a3)...

Abstract

Multi-functionalization of catalytically-active nanomaterials provides a valuable tool for enhancing reaction yield by shifting reaction equilibrium, and potentially also by adjusting reaction-diffusion kinetics. For example, multi-functionalization of mesoporous silica to make the interior pore surface hydrophobic can enhance yield in dehydration reactions. Detailed molecular-level modeling to describe the pore environment, as well as the reaction and diffusion kinetics is challenging, although we briefly discuss current strategies. Our focus, however, is on coarse-grained stochastic modeling of the overall catalytic process for highly restricted transport within narrow pores (with single-file diffusion), while accounting for a tunable interaction of the pore interior with reaction products. We show that making the pore interior unfavorable to products can significantly enhance yield due to both thermodynamic and kinetics factors.

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