金属卟啉/MgAl水滑石催化醇选择性氧化制备羰基化合物

doi:10.11944/j.issn.1000-0518.2019.11.190073

摘要/Abstract

摘要：

将MgAl水滑石引入到金属四苯基卟啉(MTPPs,M=Co,Fe,Mn,Ni)催化氧化体系中,实现了醇的选择性氧化。结果表明,在分子氧/异丁醛体系中,CoTPP在苯甲醇氧化制苯甲醛反应中表现出优异的催化活性,MgAl水滑石添加剂可有效地提高醛的选择性。在苯甲醇1 mmol、乙腈2 mL、CoTPP 5 mg、MgAl水滑石18 mg、异丁醛5 mmol、反应温度60 ℃、氧气气氛下反应2 h,苯甲醇的转化率和苯甲醛的选择性分别达到94%和92%。另外,此催化体系在其它醇类化合物的氧化反应中也具有较好催化活性。

关键词: 钴卟啉, 类水滑石, 醇, 选择性氧化, 碱

Abstract:

The selective aerobic oxidation of alcohols to carbonyl compounds was achieved by introduction of MgAl hydrotalcite into the metallotetraphenylporphyrins(MTPPs, M=Co, Fe, Mn, Ni) catalytic oxidation system. The results indicated that CoTPP exhibited the highest catalytic activity in the oxidation of benzyl alcohol to benzaldehyde through molecular oxygen/isobutyraldehyde(IBA) system, and MgAl hydrotalcite additive could effectively improve the catalytic selectivity of aldehyde. Under the optimized conditions(benzyl alcohol 1 mmol, acetonitrile 2 mL, CoTPP 5 mg, MgAl hydrotalcite 18 mg, IBA 5 mmol, reaction temperature 60 ℃, oxygen atmosphere, reaction time 2 h), the conversion of benzyl alcohol and the selectivity of benzaldehyde reached 94% and 92%, respectively. The catalytic system also exhibited good catalytic performance in the oxidation of other benzylic alcohols.

Key words: cobalt porphyrin, hydrotalcite, alcohol, selective oxidation, base

陈川,徐迎迪,薛叙明,周鹏鹏. 金属卟啉/MgAl水滑石催化醇选择性氧化制备羰基化合物[J]. 应用化学, 2019, 36(11): 1286-1293.

CHEN Chuan,XU Yingdi,XUE Xuming,ZHOU Pengpeng. Selective Oxidation of Alcohols to Carbonyl Compounds over Metalloporphyrins with MgAl Hydrotalcite Additive[J]. Chinese Journal of Applied Chemistry, 2019, 36(11): 1286-1293.

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