化学
芳构化
脱氢
催化作用
乙醇
乙醛
有机化学
锌
除氧
酒
组合化学
作者
Fan Tang,Wen‐Cui Li,Lei He,Dongqi Wang,An‐Hui Lu
出处
期刊:ACS Sustainable Chemistry & Engineering
[American Chemical Society]
日期:2023-11-01
卷期号:11 (45): 16300-16309
被引量:1
标识
DOI:10.1021/acssuschemeng.3c05085
摘要
The direct conversion of ethanol to aromatic alcohols has attracted much attention as increasingly available biomass ethanol fermented from renewable sources. Herein, we present a highly efficient zinc hydroxyapatite for direct synthesis of aromatic alcohols from ethanol with a specific rate of 1.95 × 10–7 molaromatics gcatal–1 s–1, which is up to now the best in the literature. The γ-C of 2-butenal after deprotonation undergoes the nucleophilic attack to the carbonyl-C of another 2-butenal to form 2,4,6-octatrienal, which is subsequently cyclized to give ortho-aromatics, as the main pathway for the aromatization. Dynamic and theoretical studies reveal that the Zn site plays a role in hydrogen transfer for dehydrogenation and hydrogenation. The substitution of the Zn atom for the Ca atom was identified at the strong basic [Ca–O–P] site, and the Zn site lowers the energy barrier to ethanol dehydrogenation. The rate-determining step of this reaction is the coupling of two acetaldehyde molecules to form 2-butenal. This work provides a strategy to catalyze the efficient conversion of ethanol to high value-added aromatic alcohols and contributes to the development of protocols for sustainable synthesis of aromatic alcohols from biomass through heterogeneous catalysts.
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