Evaluating catalytic (gas-solid) spectroscopic cells as intrinsic kinetic reactors: Methanol-to-hydrocarbon reaction as a case study
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2022-12Autor
Valecillos Díaz, José del Rosario
Cui, Mengmeng
Castaño Sánchez, Pedro
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Chemical Engineering Journal 450(Part 1) : (2022) // Article ID 137865
Resumen
Commercial spectroscopic gas-solid cell reactors are routinely used to analyze the dynamics of the catalyst (catalyst pelletized as a disc) structure and retained/adsorbed species using multiple operando techniques. These instruments have revolutionized the understanding of many catalytic reactions, including the methanol-to-hydrocarbon reactions. We propose a reaction engineering framework to evaluate spectroscopic cells based on (a) analyzing the fluid dynamic performance, (b) comparing their performance with a reference packed-bed reactor, and (c) the assessment of the external and internal mass transfer limitations. We have used a Specac HTHP and a Linkam THMS600 cell reactors coupled with the corresponding gas conditioning, spectroscopic, and mass spectrometry apparatuses. Our results reveal that these cells approach a perfect mixing only with several equivalent tanks in series and they are reliable at low catalyst loadings (thin disc) and high flowrates (low spacetimes). Under these conditions, we can avoid external-internal mass transfer limitations and fluid dynamic artifacts (e.g., bypassing or dead/stagnant volume zones), obtaining intrinsic kinetics with the corresponding operando spectroscopic signatures. The proposed methodology allows to understand the influence of process parameters and potential design modifications on the observed kinetic performance.