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Kinetics of the direct DME synthesis from CO₂ rich syngas under variation of the CZA-to-γ-Al₂O₃ ratio of a mixed catalyst bed.

ABSTRACT: The one-step synthesis of dimethyl ether over mechanical mixtures of Cu/ZnO/Al₂O₃ (CZA) and γ-Al₂O₃ was studied in a wide range of process conditions. Experiments were performed at an industrially relevant pressure of 50 bar varying the carbon oxide ratio in the feed (CO₂ in CO _x from 20 to 80%), temperature (503-533 K), space-time (240-400 kg_cat s m_gas ^-3), and the CZA-to-γ-Al₂O₃ weight ratio (from 1 to 5). Factors favoring the DME production in the investigated range of conditions are an elevated temperature, a low CO₂ content in the feed, and a CZA-to-γ-Al₂O₃ weight ratio of 2. A lumped kinetic model was parameterized to fit the experimental data, resulting in one of the predictive models with the broadest range of validity in the open literature for the CZA/γ-Al₂O₃ system.

SUBMITTER: Delgado Otalvaro N

PROVIDER: S-EPMC9036900 | biostudies-literature | 2021 Jul

REPOSITORIES: biostudies-literature

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Kinetics of the direct DME synthesis from CO2 rich syngas under variation of the CZA-to-γ-Al2O3 ratio of a mixed catalyst bed.

Delgado Otalvaro Nirvana N Sogne Gerardo G Herrera Delgado Karla K Wild Stefan S Pitter Stephan S Sauer Jörg J

RSC advances 20210713 40

The one-step synthesis of dimethyl ether over mechanical mixtures of Cu/ZnO/Al2O3 (CZA) and γ-Al2O3 was studied in a wide range of process conditions. Experiments were performed at an industrially relevant pressure of 50 bar varying the carbon oxide ratio in the feed (CO2 in CO x from 20 to 80%), temperature (503-533 K), space-time (240-400 kgcat s mgas -3), and the CZA-to-γ-Al2O< ...[more]

PMID: 35481015

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Project description:The direct synthesis of dimethyl ether (DME) via CO2 hydrogenation in a single step was studied using an improved class of bifunctional catalysts in a fixed bed reactor (T R: 210-270 °C; 40 bar; gas hourly space velocity (GHSV) 19,800 NL kgcat -1 h-1; ratio CO2/H2/N2 3:9:2). The competitive bifunctional catalysts tested in here consist of a surface-basic copper/zinc oxide/zirconia (CZZ) methanol-producing part and a variable surface-acidic methanol dehydration part and were tested in overall 45 combinations. As dehydration catalysts, zeolites (ferrierite and β-zeolite), alumina, or zirconia were tested alone as well as with a coating of Keggin-type heteropoly acids (HPAs), i.e., silicotungstic or phosphotungstic acid. Two different mixing methods to generate bifunctional catalysts were tested: (i) a single-grain method with intensive intra-particular contact between CZZ and the dehydration catalyst generated by mixing in an agate mortar and (ii) a dual-grain approach relying on physical mixing with low contact. The influence of the catalyst mixing method and HPA loading on catalyst activity and stability was investigated. From these results, a selection of best-performing bifunctional catalysts was investigated in extended measurements (time on stream: 160 h/7 days, T R: 250 and 270 °C; 40 bar; GHSV 19,800 NL kgcat -1 h-1; ratio CO2/H2/N2 3:9:2). Silicotungstic acid-coated bifunctional catalysts showed the highest resilience toward deactivation caused by single-grain preparation and during catalysis. Overall, HPA-coated catalysts showed higher activity and resilience toward deactivation than uncoated counterparts. Dual-grain preparation showed superior performance over single grain. Furthermore, silicotungstic acid coatings with 1 KU nm-2 (Keggin unit per surface area of carrier) on Al2O3 and ZrO2 as carrier materials showed competitive high activity and stability in extended 7-day measurements compared to pure CZZ. Therefore, HPA coating is found to be a well-suited addition to the CO2-to-DME catalyst toolbox.

Dataset Information

Kinetics of the direct DME synthesis from CO₂ rich syngas under variation of the CZA-to-γ-Al₂O₃ ratio of a mixed catalyst bed.

Publications

Kinetics of the direct DME synthesis from CO<sub>2</sub> rich syngas under variation of the CZA-to-γ-Al<sub>2</sub>O<sub>3</sub> ratio of a mixed catalyst bed.

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