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Influence of the operating conditions on the behavior and deactivation of a CuO-ZnO-ZrO2@SAPO-11 core-shell-like catalyst in the direct synthesis of DME

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  • Sánchez-Contador, M.
  • Ateka, A.
  • Ibáñez, M.
  • Bilbao, J.
  • Aguayo, A.T.

Abstract

The behavior of the CuO-ZnO-ZrO2@SAPO-11 core-shell catalyst in the direct synthesis of DME from H2 + CO + CO2 mixtures has been assessed. The effect of the reaction conditions (temperature, pressure, space-time) and feed composition (CO2 and H2 concentration) on the DME yield and selectivity, CO2 and COx (CO2+CO) conversions and stability of the catalyst have been studied. The experiments have been carried out in a fixed-bed reactor in the following condition ranges: 250–325 °C; 10–50 bar; space-time, 1.25–15 g h molC−1; CO2/COx molar ratio in the feed, 0–1; and H2/COx molar ratio in the feed, 2.5–4; time on stream, up to 48 h. Under mild conditions (275–300 °C range, 20–30 bar, space-time over 5 g h molC−1, CO2/COx molar ratio in the 0.5–0.75 range, and H2/COx molar ratio around 3) a good compromise is reached between the yield of DME and the conversion of CO2, with high catalyst stability. Coke deposition is the main cause of catalyst deactivation, formed by condensation of the hydrocarbon byproducts, blocking the metallic sites in the core. The formation rate of this fraction of coke is greater than that of the coke deposited in the SAPO-11 of the shell. Increasing reaction temperature favors the formation of coke, while co-feeding CO2 attenuates this formation, due to the increase of H2O concentration.

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  • Sánchez-Contador, M. & Ateka, A. & Ibáñez, M. & Bilbao, J. & Aguayo, A.T., 2019. "Influence of the operating conditions on the behavior and deactivation of a CuO-ZnO-ZrO2@SAPO-11 core-shell-like catalyst in the direct synthesis of DME," Renewable Energy, Elsevier, vol. 138(C), pages 585-597.
    • Handle: RePEc:eee:renene:v:138:y:2019:i:c:p:585-597
    DOI: 10.1016/j.renene.2019.01.093
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    References listed on IDEAS

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    1. Chen, Wei-Hsin & Hsu, Chih-Liang & Wang, Xiao-Dong, 2016. "Thermodynamic approach and comparison of two-step and single step DME (dimethyl ether) syntheses with carbon dioxide utilization," Energy, Elsevier, vol. 109(C), pages 326-340.
    2. Ateka, Ainara & Pérez-Uriarte, Paula & Gamero, Mónica & Ereña, Javier & Aguayo, Andrés T. & Bilbao, Javier, 2017. "A comparative thermodynamic study on the CO2 conversion in the synthesis of methanol and of DME," Energy, Elsevier, vol. 120(C), pages 796-804.
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    1. Ateka, Ainara & Portillo, Ander & Sánchez-Contador, Miguel & Bilbao, Javier & Aguayo, Andres T., 2021. "Macro-kinetic model for CuO–ZnO–ZrO2@SAPO-11 core-shell catalyst in the direct synthesis of DME from CO/CO2," Renewable Energy, Elsevier, vol. 169(C), pages 1242-1251.

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