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Deactivation Kinetics of Solid Acid Catalyst with Laterally Interacting Protons.

Aditya Sengar1, Rutger A van Santen1,2, Erik Steur2,3

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Catalyst deactivation in solid acid catalysis is accelerated by proton interactions, leading to decreased selectivity over time. Simulations show that while these interactions initially boost selectivity, they ultimately reduce catalyst stability and speed up deactivation through carbenium ion formation.

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Area of Science:

  • Catalysis
  • Chemical Kinetics
  • Materials Science

Background:

  • Solid acid catalysts are crucial for alkylation reactions.
  • Catalyst deactivation limits efficiency and product selectivity.
  • Understanding proton behavior is key to improving catalyst performance.

Purpose of the Study:

  • To investigate the impact of lateral proton interactions on catalyst deactivation kinetics.
  • To model the inhomogeneity of proton reactivity over time.
  • To analyze the influence of these interactions on product selectivity and deactivation rates.

Main Methods:

  • Simulations of deactivation kinetics for the alkylation of propylene with isobutane.
  • Comparison of catalyst models with and without lateral proton interactions.
  • Utilizing mean field kinetic equations and stochastic simulations.
  • Development of a nonlinear dynamics model for proton dynamics.

Main Results:

  • Lateral proton interactions induce proton reactivity inhomogeneity, accelerating deactivation.
  • Initial catalyst deactivation is molecular, involving stable carbenium ion formation, not pore blocking.
  • The lateral interaction model shows higher initial selectivity but lower overall stability.
  • Two deactivation pathways identified: reactant oligomerization and carbenium ion deprotonation.
  • Stochastic simulations reveal island formation of intermediates, increasing deactivation rates at high selectivity.

Conclusions:

  • Lateral proton interactions significantly influence solid acid catalyst deactivation.
  • Proton reactivity inhomogeneity and carbenium ion formation are primary deactivation mechanisms.
  • Catalyst design must balance initial selectivity with long-term stability.
  • Discrepancies between mean field and stochastic simulations are attributed to frustrated proton state percolation.