The potential of ZrO2 catalysts for the dehydration of 2,3-butanediol into 3-buten-2-ol: Impact of synthesis method and operating conditions

[Display omitted] •Hydrothermal ZrO2 calcined at high temperature gives high 3-buten-2-ol selectivity.•Highest 3-buten-2-ol selectivity at low temperature and high space time.•Mild acid-base properties are crucial for selective first dehydration step.•Incompatible acid-base properties for one-step o...

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Vydáno v:Journal of catalysis Ročník 411; s. 200 - 211
Hlavní autoři: Bekele, Beruk A., Poissonnier, Jeroen, Thybaut, Joris W.
Médium: Journal Article
Jazyk:angličtina
Vydáno: Elsevier Inc 01.07.2022
Témata:
2,3-butanediol dehydration
adsorption
Biomass conversion
catalysts
catalytic activity
crystal structure
Hydrothermal ZrO₂ synthesis
Kinetics
partial pressure
Kinetics
Biomass conversion
2,3-butanediol dehydration
Hydrothermal ZrO₂ synthesis
ISSN:0021-9517, 1090-2694
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Shrnutí:[Display omitted] •Hydrothermal ZrO2 calcined at high temperature gives high 3-buten-2-ol selectivity.•Highest 3-buten-2-ol selectivity at low temperature and high space time.•Mild acid-base properties are crucial for selective first dehydration step.•Incompatible acid-base properties for one-step optimization of both dehydrations. 2,3-Butanediol (2,3-BDO) dehydration towards 1,3-butadiene was investigated over commercial and in-house synthesized ZrO2 catalysts in a Berty reactor at intrinsic kinetics conditions. The commercial and ZrO2 catalysts prepared via precipitation (ZrO2-PP) exhibited a higher selectivity towards the undesired methyl ethyl ketone which was attributed to a lack of sufficient acid-base concerted active sites. For ZrO2-PP, this was attributed to its tetragonal crystal structure with weaker adsorption sites. Hydrothermal synthesis allowed producing ZrO2 with a monoclinic crystal structure, with correspondingly more pronounced acidic and basic properties which could be further tuned via calcination. A maximal 3-buten-2-ol, i.e., the desired intermediate for further conversion into 1,3-butadiene, yield amounting to 38% (mol mol−1) could be obtained under a N2 flow at 300 °C, a space time of 1130 kg s mol−1 and 2,3-BDO partial pressure of 0.16 bar over the hydrothermally synthesized catalyst.
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ISSN:0021-9517
1090-2694
DOI:10.1016/j.jcat.2022.05.011