Dataset Information

Kinetic Model for the Direct Conversion of CO₂/CO into Light Olefins over an In₂O₃-ZrO₂/SAPO-34 Tandem Catalyst.

ABSTRACT: An original kinetic model is proposed for the direct production of light olefins by hydrogenation of CO₂/CO (CO_x) mixtures over an In₂O₃-ZrO₂/SAPO-34 tandem catalyst, quantifying deactivation by coke. The reaction network comprises 12 individual reactions, and deactivation is quantified with expressions dependent on the concentration of methanol (as coke precursor) and H₂O and H₂ (as agents attenuating coke formation). The experimental results were obtained in a fixed-bed reactor under the following conditions: In₂O₃-ZrO₂/SAPO-34 mass ratio, 0/1-1/0; 350-425 °C; 20-50 bar; H₂/CO_x ratio, 1-3; CO₂/CO_x ratio, 0-1; space time, 0-10 g_In2O3-ZrO2 h mol_C^-1, 0-20 g_SAPO-34 h mol_C^-1; time, up to 500 h; H₂O and CH₃OH in the feed, up to 5% vol. The utility of the model for further scale-up studies is demonstrated by its application in optimizing the process variables (temperature, pressure, and CO₂/CO_x ratio). The model predicts an olefin yield higher than 7% (selectivity above 60%), a CO_x conversion of 12% and a CO₂ conversion of 16% at 415 °C and 50 bar, for a CO₂/CO_x = 0.5 in the feed. Additionally, an analysis of the effect of In₂O₃-ZrO₂ and SAPO-34 loading in the configuration of the tandem catalyst is conducted, yielding 17% olefins and complete conversion of CO₂ under full water removal conditions.

SUBMITTER: Portillo A

PROVIDER: S-EPMC10828986 | biostudies-literature | 2024 Jan

REPOSITORIES: biostudies-literature

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Publications

Kinetic Model for the Direct Conversion of CO2/CO into Light Olefins over an In2O3-ZrO2/SAPO-34 Tandem Catalyst.

Portillo Ander A Parra Onintze O Aguayo Andres T AT Ereña Javier J Bilbao Javier J Ateka Ainara A

ACS sustainable chemistry & engineering 20240118 4

An original kinetic model is proposed for the direct production of light olefins by hydrogenation of CO2/CO (COx) mixtures over an In2O3-ZrO2/SAPO-34 tandem catalyst, quantifying deactivation by coke. The reaction network comprises 12 individual reactions, and deactivation is quantified with expressions dependent on the concentration of methanol (as coke precursor) and H2O and H2 (as agents attenuating coke forma ...[more]

PMID: 38303907

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Project description:The selectivity toward lower olefins during the methanol-to-olefins conversion over H-SAPO-34 at reaction temperatures between 573 and 773 K has been studied with a combination of operando UV-vis diffuse reflectance spectroscopy and online gas chromatography. It was found that the selectivity toward propylene increases in the temperature range of 573-623 K, while it decreases in the temperature range of 623-773 K. The high degree of incorporation of olefins, mainly propylene, into the hydrocarbon pool affects the product selectivity at lower reaction temperatures. The nature and dynamics of the active and deactivating hydrocarbon species with increasing reaction temperature were revealed by a non-negative matrix factorization of the time-resolved operando UV-vis diffuse reflectance spectra. The active hydrocarbon pool species consist of mainly highly methylated benzene carbocations at temperatures between 573 and 598 K, of both highly methylated benzene carbocations and methylated naphthalene carbocations at 623 K, and of only methylated naphthalene carbocations at temperatures between 673 and 773 K. The operando spectroscopy results suggest that the nature of the active species also influences the olefin selectivity. In fact, monoenylic and highly methylated benzene carbocations are more selective to the formation of propylene, whereas the formation of the group of low methylated benzene carbocations and methylated naphthalene carbocations at higher reaction temperatures (i.e., 673 and 773 K) favors the formation of ethylene. At reaction temperatures between 573 and 623 K, catalyst deactivation is caused by the gradual filling of the micropores with methylated naphthalene carbocations, while between 623 and 773 K the formation of neutral poly aromatics and phenanthrene/anthracene carbocations are mainly responsible for catalyst deactivation, their respective contribution increasing with increasing reaction temperature. Methanol pulse experiments at different temperatures demonstrate the dynamics between methylated benzene and methylated naphthalene carbocations. It was found that methylated naphthalene carbocations species are deactivating and block the micropores at low reaction temperatures, while acting as the active species at higher reaction temperatures, although they give rise to the formation of extended hydrocarbon deposits.

Dataset Information

Kinetic Model for the Direct Conversion of CO₂/CO into Light Olefins over an In₂O₃-ZrO₂/SAPO-34 Tandem Catalyst.

Publications

Kinetic Model for the Direct Conversion of CO<sub>2</sub>/CO into Light Olefins over an In<sub>2</sub>O<sub>3</sub>-ZrO<sub>2</sub>/SAPO-34 Tandem Catalyst.

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