Modeling Coordinatively Unsaturated Structures in Mixed Mg-Al Oxides as Active Sites for Dehydrogenation and Dehydration of Ethanol

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Abstract

Processes of dehydrogenation and dehydration of ethanol on a Lewis acid site (LAS) of mixed Mg–Al oxide have been studied by density-functional theory approach. The structure of the active site of the mixed oxide system has been proposed. Possible intermediates have been studied and the mechanisms of these processes occurring on LAS of mixed oxide containing aluminum or chromium have been suggested. Isomorphous substitution of aluminum for chromium in the structure of mixed oxide results in a decrease of the energetic barrier for the process of ethanol dehydrogenation.

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About the authors

М. N. Мikhailov

N.D. Zelinsky Institute of Organic Chemistry of the Russian Academy of Sciences

Email: lmk@ioc.ac.ru
Russian Federation, Moscow

L. М. Kustov

Lomonosov Moscow State University; N.D. Zelinsky Institute of Organic Chemistry of the Russian Academy of Sciences

Author for correspondence.
Email: lmk@ioc.ac.ru
Russian Federation, Moscow; Moscow

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Supplementary files

Supplementary Files
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2. Fig. 1. Selection of the mixed oxide cluster

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3. Scheme 1. Scheme of ethanol dehydrogenation process on LCC with aluminium

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4. Fig. 2. Mechanism of interaction of ethanol molecule with the active centre containing aluminium in the dehydrogenation reaction

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5. Scheme 2. Main steps of ethanol dehydration process on acid-base centres including aluminium atom

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6. Fig. 3. Mechanism of interaction of ethanol molecule with the active centre containing aluminium for the dehydration reaction

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7. Scheme 3. Main steps of the ethanol dehydrogenation process on the acid-base centre containing chromium

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8. Translation results Fig. 4. Mechanism of interaction of ethanol molecule with the active centre containing aluminium for the dehydrogenation reaction

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9. Scheme 4. Main steps of the ethanol dehydration process on the acid-base centre containing chromium

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10. Fig. 5. Mechanism of interaction of ethanol molecule with the active centre containing aluminium for the dehydration reaction

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11. Fig. 6. Total energy variation for the ethanol dehydrogenation process on a mixed oxide cluster with aluminium and chromium

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12. Fig. 7. Total energy variation for the ethanol dehydration process on a mixed oxide cluster with aluminium and chromium

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