Enhancing reactant selectivity for Ni/Mg reforming catalysts using silicalite-1 shells: A modeling study

Gray, Brian; Kuhn, John N.; Joseph, Babu

doi:10.1016/j.cej.2022.135353

Title: Enhancing reactant selectivity for Ni/Mg reforming catalysts using silicalite-1 shells: A modeling study

Journal Article · 20 February 2022 · Chemical Engineering Journal

DOI: https://doi.org/10.1016/j.cej.2022.135353 · OSTI ID:1902717

Gray, Brian ^[1]; Kuhn, John N. ^[2]; Joseph, Babu ^[2]

Univ. of South Florida, Tampa, FL (United States); University of South Florida
Univ. of South Florida, Tampa, FL (United States)

The ability of a zeolite shell to enhance the selective conversion of hydrocarbons through diffusional limitations was investigated using a multi-scale model of a fixed-bed reactor. The impact of shell thickness and molecule/pore size on the catalytic performance of silicalite-1 zeolite encapsulated nickel catalyst pellets for steam reforming of C1-C7 hydrocarbons is reported. A reaction–diffusion model using kinetic expressions established in literature was employed. The model was verified through comparison with reported experimental results for steam reforming data over a temperature range of 748 – 1113 K and pressure of 1 – 10 bar. Comparisons are also made against experimental data for steam reforming in the presence of a zeolite shell. Evaluation of the Weisz-Prater criterion for both the core and encapsulated catalyst confirmed mass transfer limitation induced by the utilization of a zeolite shell. The model was used to suggest an optimal thickness that balances diffusional limitations imposed by the zeolite layer on methane versus that of the heavier hydrocarbons. The optimum thickness varied as a function of hydrocarbon size and shape which determined the diffusion rates. For toluene and heptane, a 50 nm thick shell was sufficient to wholly prevent reaction. Hydrocarbons like propane and butane required a shell 7.5 and 5 μm thick. Increasing the gas-hourly-space-velocity from 10,000 to 60,000 h^–1 caused a decrease in the optimum shell thickness. Furthermore, this approach can be modified for application to other mixed hydrocarbon systems to predict optimal catalyst design.

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Research Organization:: Univ. of South Florida, Tampa, FL (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: EE0008488

OSTI ID:: 1902717

Journal Information:: Chemical Engineering Journal, Journal Name: Chemical Engineering Journal Vol. 437; ISSN 1385-8947

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Enhancing reactant selectivity for Ni/Mg reforming catalysts using silicalite-1 shells: A modeling study

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