以甲酸为氢源在介孔 CuO 催化剂上制备 γ-戊内酯,Reaction Chemistry & Engineering

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以甲酸为氢源在介孔 CuO 催化剂上制备 γ-戊内酯
Reaction Chemistry & Engineering ( IF 3.4 ) Pub Date : 2022-08-02 , DOI: 10.1039/d2re00192f
Neda Ayashi ₁ , Alireza Najafi Chermahini ₁ , Nasim Amiri Ramsheh ₁ , Rafael Luque _{2,

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Affiliation

在本研究中，研究了乙酰丙酸 (LA)、乙酰丙酸丁酯 (BL) 和乙酰丙酸乙酯 (EL) 向有价值的生物质衍生化合物 γ-戊内酯 (GVL) 的转化。通过硬模板法制备的一系列介孔 CuO 催化剂与甲酸 (FA) 作为氢供体用于还原 LA 和乙酰丙酸酯。使用分析和物理方法对催化剂进行表征，例如 XRD、FESEM-EDX 和氮吸附 - 脱附、氢气程序升温还原和 TEM 技术。在这些样品中，在氢气气氛下还原的介孔CuO表现出更高的级联甲酸分解和氢转移至乙酰丙酸烷基酯的活性，随后闭环和形成γ-戊内酯。考察了催化剂用量、反应温度、乙酰丙酸和乙酰丙酸烷基酯用量与甲酸比、反应时间等影响因素对底物转化率和GVL产率的影响。根据所得结果，选择介孔CuO催化剂50 mg，反应温度180 ℃，反应时间5 h为最佳反应条件。

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Production of γ-valerolactone over mesoporous CuO catalysts using formic acid as the hydrogen source

In the present study, the conversion of levulinic acid (LA), butyl levulinate (BL), and ethyl levulinate (EL) to valuable biomass-derived compound γ-valerolactone (GVL) is studied. A series of mesoporous CuO catalysts prepared through the hard template method were used in combination with formic acid (FA) as the hydrogen donor for the reduction of LA and levulinate esters. The catalysts are characterized using analytical and physical methods such as XRD, FESEM-EDX, and nitrogen adsorption–desorption, hydrogen temperature-programmed reduction, and TEM techniques. Among the samples, mesoporous CuO which was reduced under a hydrogen atmosphere exhibited higher activity in the cascade formic acid decomposition and hydrogen transfer to alkyl levulinates, followed by the ring closure and formation of γ-valerolactone. The effect of influential factors including the amount of catalyst, reaction temperature, levulinic acid and alkyl levulinate amount to formic acid ratio, and reaction time on the conversion of substrates and GVL yield was also investigated. According to the obtained results, 50 mg of the mesoporous CuO catalyst, 180 °C as the reaction temperature, and 5 h as the reaction time were selected as the optimum reaction conditions.

更新日期：2022-08-02

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