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摘要
以对苯二醛和乙二胺为原料合成线性席夫碱配体,并将其与Co配位制备席夫碱配合物Co-L(L=对苯二醛缩乙二胺席夫碱)。利用EA、ICP、FT-IR、UV-Vis、TGA和BET等对配体及配合物的结构与性能进行表征,在氧化环己烯制备环己烯酮的反应中测试其催化性能。结果表明,Co-L具有较高的催化活性和烯丙基氧化产物的选择性。在乙腈用量为5 mL、环己烯物质的量为6 mmol、氧压为0.3 MPa、催化剂质量为20 mg、反应温度为70℃条件下,环己烯的转化率为37.66%,烯丙基氧化产物的选择性高达83.59%。催化剂重复使用5次,环己烯的转化率和烯丙基氧化产物的选择性几乎不变。
Abstract
C-H oxidation for alkanes,olefins and other petroleum feedstocks can produce oxygen-containing compounds with higher added value.Linear Schiff base ligands are synthesized from p-phenylenedialdehyde and ethylenediamine,and coordinated with Co to prepare Schiff base Co complex Co-L (L=p-phenylenedialdehyde-ethylenediamine Schiff base).The ligands and complex samples are characterized by EA,ICP,FT-IR,UV-Vis,TGA,BET,etc.,the catalytic performance of Co-L is tested in the reaction of cyclohexene oxidation to cyclohexenone.Results show that Co-L exhibits high catalytic activity and high selectivity of allylic oxidation products.The conversion of cyclohexene can reach 37.66% and the selectivity of allylic oxidation products can reach 83.59% when the dosages of acetonitrile,cyclohexene and Co-L is 5 mL,6 mmol and 20 mg respectively,oxygen pressure stays at 0.3 MPa,and reaction temperature remains at 70℃.The conversion of cyclohexene and the selectivity of allylic oxidation products remains almost unchanged after the catalyst has been reused for 5 times.In addition,it is found that lower reaction temperature can reduce the selectivity of the by-product epoxy cyclohexane,which is beneficial to the selective oxidation of cyclohexene.
关键词
C-H氧化
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Co配合物
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席夫碱
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环己烯
Key words
C-H oxidation
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Co complex
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Schiff base
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cyclohexene
Author summay
王新国(1991-),男,硕士研究生,研究方向为过渡金属配合物的催化性能研究,925536941@qq.com
线性Co配合物催化环己烯烯丙基C-H氧化反应的研究[J].
现代化工, 2021, 41(1): 159-164 DOI:10.16606/j.cnki.issn0253-4320.2021.01.032