Journal Home > Online First

The direct conversion of ethanol to 1,1-diethoxyethane (DEE) through one-pot dehydrogenation-acetalization has attracted broad interest from both academia and industry. Based on thermodynamics, the oxidative dehydrogenation of alcohol to acetaldehyde requires high temperature to activate oxygen to realize the C–H cleavage, while the acetalization of acetaldehyde with ethanol is exothermic reversible reaction favorable at low temperature. The mismatching of the reaction condition for the two consecutive steps makes it a great challenge to achieve both high ethanol conversion and high DEE selectivity. This work reports a highly efficient bi-functional catalysis by Bi/BiCeOx for one-pot oxidative dehydrogenation-acetalization route from ethanol to DEE under 150 °C and ambient pressure, affording a selectivity of 98.5% ± 0.5% to DEE at an ethanol conversion of 87.0% ± 1.0%. An efficient tandem catalysis has been achieved on the interfacial Biδ+-Ov-CeIII sites in Bi/BiCeOx established by strong metal–support interaction, in which Biδ+-Ov- sites contribute to the oxidative dehydrogenation of ethanol at mild temperature, and -Ov-CeIII sites to the subsequent acetalization between the generated acetaldehyde and ethanol.

File
4848_ESM.pdf (302.8 KB)
Publication history
Copyright
Acknowledgements
Rights and permissions

Publication history

Received: 26 May 2022
Revised: 14 July 2022
Accepted: 02 August 2022
Published: 13 September 2022

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

Financial support from the National Natural Science Foundation of China (Nos. 22138001 and 21521005) and the National Key R&D Program of China (No. 2017YFA0206804) is acknowledged. We thank the support of Beijing Engineering Center for Hierarchical Catalysts.

Rights and permissions

Reprints and Permission requests may be sought directly from editorial office.
Email: nanores@tup.tsinghua.edu.cn

Return