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蔗渣纤维素基季铵过氧磷钨酸盐的合成与表征及其在无溶剂条件下催化环己烯氧化的性能。

Synthesis and characterization of bagasse cellulose-based quaternary ammonium peroxyphosphotungstate and their catalytic properties for cyclohexene oxidation in the absence of any solvent.

机构信息

College of chemical and environmental Engineering, Hanshan Normal University, Guangdong Province, Chaozhou 521041, China; Key laboratory of Resources Environmental and Green Low Carbon Processes in East Guangdong, Guangdong Province, Chaozhou 521041, China.

College of chemical and environmental Engineering, Hanshan Normal University, Guangdong Province, Chaozhou 521041, China; Key laboratory of Resources Environmental and Green Low Carbon Processes in East Guangdong, Guangdong Province, Chaozhou 521041, China.

出版信息

Int J Biol Macromol. 2024 Aug;274(Pt 2):133549. doi: 10.1016/j.ijbiomac.2024.133549. Epub 2024 Jul 8.

Abstract

Bagasse cellulose, an industrial waste byproduct of sugar production, was demonstrated to be a viable solid support for a solid-phase ionic oxidation catalyst enabling organic solvent-free aqueous reaction conditions and facile catalyst recovery. Bagasse cellulose-supported quaternary ammonium peroxyphosphotungstate was synthesized from bagasse cellulose-supported quaternary ammonium chloride, phosphotungstic acid, and hydrogen peroxide. The chemical structure of this material was characterized by SEM, XRD, FT-IR, XPS, and C NMR, revealing stability of the cellulose matrix to the catalyst loading conditions and effective dispersion of the acicular catalyst crystals throughout the matrix. High catalytic activity of this synthetic complex was demonstrated in the oxidation of cyclohexene to 1,2-cyclohexanediol with hydrogen peroxide in the absence of solvent. Optimized conditions providing trans-1,2-cyclohexanediol with 86.2 % selectivity were 12 wt% catalyst and 4 mL/g 30 % HO (vs. cyclohexene) at 50 °C for 10 h.

摘要

蔗渣纤维素是糖生产的工业废物副产物,已被证明是一种可行的固相离子氧化催化剂的固体载体,能够实现有机溶剂免费的水相反应条件和易于催化剂回收。从蔗渣纤维素负载的季铵氯化物、磷钨酸和过氧化氢合成了蔗渣纤维素负载的过氧磷酸钨季铵盐。通过 SEM、XRD、FT-IR、XPS 和 C NMR 对该材料的化学结构进行了表征,结果表明纤维素基质对催化剂负载条件具有稳定性,并且针状催化剂晶体有效地分散在整个基质中。该合成复合物在无溶剂条件下用过氧化氢氧化环己烯制备 1,2-环己二醇时表现出很高的催化活性。在优化条件下,以 30%的 HO(相对于环己烯)为 4 mL/g,在 50°C 下反应 10 h,可获得 86.2%选择性的反式-1,2-环己二醇。

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