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Alkylation of lignin-derived aromatic oxygenates with cyclic alcohols on acidic zeolites
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2020-08-13 , DOI: 10.1016/j.apcatb.2020.119424
Yuanshuai Liu , Guanhua Cheng , Eszter Baráth , Hui Shi , Johannes A. Lercher

Moderately strong BAS and spacious microporous environments (i.e., large-pore acidic zeolites HBEA and HY) are important criteria for efficient alkylation of phenols with cyclic alcohols and alkenes, while very strong BAS appear to be responsible for catalyst deactivation. BAS confined in HBEA and HY pores show substantially higher turnover frequencies compared to solids without molecularly sized pore constraints. HBEA favors the formation of mono-alkylates, while enhanced formation of di-alkylates is observed on HY. Dehydration of alcohols always dominates over the alkylation at the onset of the reaction. Carbenium ions, the direct electrophile for aromatic oxygenates, are produced mainly from the adsorption and protonation of olefins. The present study shows that for the alkylation of phenols and cyclic alcohols in apolar liquids, the alcohol concentration should be kept low to avoid the formation of unreactive surface dimers and mitigate their inhibitory effects on olefin adsorption and protonation.



中文翻译:

木质素衍生的芳香族含氧化合物与环状醇在酸性沸石上的烷基化

中等强度的BAS和宽敞的微孔环境(即大孔酸性沸石HBEA和HY)是酚与环醇和烯烃有效烷基化的重要标准,而非常强的BAS似乎是造成催化剂失活的原因。与没有分子大小的孔隙限制的固体相比,封闭在HBEA和HY孔隙中的BAS显示出更高的周转频率。HBEA有利于单烷基化物的形成,而在HY上观察到二烷基化物的形成增加。在反应开始时,醇的脱水总是比烷基化更重要。碳原子离子,是芳香族含氧化合物的直接亲电体,主要是由烯烃的吸附和质子化产生的。目前的研究表明,对于非极性液体中酚和环状醇的烷基化,

更新日期:2020-09-07
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