NHPI催化分子氧选择性氧化木质素模型分子中的C—C键
发布时间：2019-02-17 18:18
【摘要】：以1,2-二苯乙烷为模型分子,考察了N-羟基邻苯二甲酰亚胺(NHPI)对分子氧氧化断裂木质素分子中C—C键的催化作用,比较了Cu、Co和Mn的多种可溶性盐对NHPI催化活性的促进作用,探究了工艺条件对1,2-二苯乙烷氧化的影响规律。结果表明:NHPI能够在温和条件下催化分子氧氧化1,2-二苯乙烷中的C—C键断裂生成苯甲醛和苯甲酸。可溶性的Cu、Co和Mn盐都具有助催化作用,其中乙酸锰的助催化作用最强。确定了二苯基乙酮为氧化的初级反应产物。发现提高反应温度、增加乙酸锰用量以及延长反应时间,有利于C—C键的氧化断裂和提高小分子产物的选择性。优化的反应条件为NHPI为底物物质的量的10%,乙酸锰和NHPI之比为1:10,反应温度90℃,氧气分压1.0 MPa,反应时间8 h,C—C键的氧化断裂产物苯甲醛和苯甲酸的总选择性可达76.5%。
[Abstract]:The catalytic effects of N-hydroxyphthalimide (NHPI) on C-C bond in oxygen oxidized lignin molecules were investigated by using 1-diphenylethane as model molecule, and Cu, was compared. Various soluble salts of Co and Mn promoted the catalytic activity of NHPI. The results show that NHPI can catalyze the oxidation of 1 ~ (2 +) -diphenyl ethane to benzaldehyde and benzoic acid under mild conditions. Soluble Cu,Co and Mn salts both had catalytic effects, among which manganese acetate had the strongest catalytic activity. Diphenyl ethyl ketone was determined as the primary product of oxidation. It was found that increasing the reaction temperature, increasing the amount of manganese acetate and prolonging the reaction time were beneficial to the oxidation fracture of C-C bond and the selectivity of small molecular products. The optimum reaction conditions were as follows: 10% of NHPI as substrate, the ratio of manganese acetate to NHPI was 1: 10, the reaction temperature was 90 鈩，
本文编号：2425452
[Abstract]:The catalytic effects of N-hydroxyphthalimide (NHPI) on C-C bond in oxygen oxidized lignin molecules were investigated by using 1-diphenylethane as model molecule, and Cu, was compared. Various soluble salts of Co and Mn promoted the catalytic activity of NHPI. The results show that NHPI can catalyze the oxidation of 1 ~ (2 +) -diphenyl ethane to benzaldehyde and benzoic acid under mild conditions. Soluble Cu,Co and Mn salts both had catalytic effects, among which manganese acetate had the strongest catalytic activity. Diphenyl ethyl ketone was determined as the primary product of oxidation. It was found that increasing the reaction temperature, increasing the amount of manganese acetate and prolonging the reaction time were beneficial to the oxidation fracture of C-C bond and the selectivity of small molecular products. The optimum reaction conditions were as follows: 10% of NHPI as substrate, the ratio of manganese acetate to NHPI was 1: 10, the reaction temperature was 90 鈩，
本文编号：2425452
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