新型仿生催化剂催化氧化环己烷
Oxidation of Cyclohexane by Oxygen on Novel Biomimetic Catalyst
查看参考文献22篇
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文摘
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考察了仿生催化剂四苯基金属卟啉-金属Schiff碱-四苯基金属卟啉催化氧化环己烷的反应，探讨了反应温度、氧气压力、反应时间、催化剂用量、不同金属离子配合物催化剂对环己基过氧化氢产量、氧化产物产量、氧化产物酸值、己二酸酸值、氧化产物酯值的影响。研究结果表明，在此催化剂作用下，氧化结果与反应温度、氧气压力、反应时间、催化剂用量及配位的金属离子均有密切的关系。得到了适宜的反应条件：四苯基卟啉锰-Schiff碱锰-四苯基卟啉锰为催化剂，反应温度140℃，氧气压力2．00MPa，反应时间240min，m（催化剂）：m（环己烷）=8．5×10~(-5)；在此条件下，环己烷转化率36．32％，己二酸收率11．41％，氧化产物选择性达91．65％，催化剂每个活性中心上平均转化环己烷分子数达到17000。 |
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其他语种文摘
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Oxidation of cyclohexane to cyclohexyl hydroperoxide, adipic acid and KA oil（ mixture of cyclohexanol and cyclohexanone ） in presence of oxygen with MTPP - MSalen - MTPP （TPP： tetraphenylporphyrin; M： metallic ion）as catalyst was studied. Effects of reaction time, reaction temperature, oxygen pressure, catalyst dosage and coordination metallic ions on yield of cyclohexyl hydroperoxide, total yield of oxidation products, acid value of products, acid value of adipic acid and ester value of products were investigated. The apparent activation energy is significantly lowered by using the novel catalyst in the oxidation. Under same reaction conditions, 29. 5 g oxidation products can be obtained with FeTPP - FeSalen - FeTPP as catalyst but only 9. 0 g with FeTPP. Under appropriate conditions： MnTPP - MnSalen - MnTPP as catalyst, reaction temperature 140 ℃, oxygen pressure 2.00 MPa, reaction time 240 min and re（catalyst） ： m （cyclohexane） 8.5 × 10~(-5), the conversion of cyclohexane, yield of adipic acid, and selectivity to the oxidation products are 36. 32%, 11.41% and 91.65%, respectively. On each active center of catalyst, apporox. 17 000 molecules of cyclohexane convert. |
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来源
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石油化工
,2007,36(8):774-779 【核心库】
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关键词
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环己烷
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仿生催化剂
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氧化
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环己基过氧化氢
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地址
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中国科学院新疆理化技术研究所, 新疆, 乌鲁木齐, 830011
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语种
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中文 |
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文献类型
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研究性论文 |
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ISSN
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1000-8144 |
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学科
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化学工业 |
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文献收藏号
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CSCD:2955216
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参考文献 共
22
共2页
|
|
1.
Mansuy D. Biomimetic Catalysts for Selective Oxidation in Organic Chemistry.
Pure Appl Chem,1990,62(4):741-746
|
被引
6
次
|
|
|
|
|
2.
Yuan Ying. Oxidation of Cyclohexane to Adipic Acid Using Fe-Porphyrin as a Biomimetic Catalyst.
Org Process Res Dev,2004,8(3):418-420
|
被引
29
次
|
|
|
|
|
3.
Matilte H. Catalytic Activity of Anionic Iron(Ⅲ)Porphyrins Immobilized on Grafted Disordered Silica Obtained from Acidic Leached Chrysotile.
J Mol Catal A:Chem,2006,243(1):44-51
|
被引
1
次
|
|
|
|
|
4.
刘华锋. 环己基过氧化氢热分解过程中酸生成的研究.
精细化工中间体,2002,32(3):13-15
|
被引
1
次
|
|
|
|
|
5.
Hansen C B. Metalloporphyrins as Catalysts in the Decomposition of Cyclohexyl Hydroperoxide.
Catal Lett,1993,20:359-364
|
被引
1
次
|
|
|
|
|
6.
Ji Liangnian. Metalloporphyrin-Catalyzed Hydroxylation of Cyclohexane with Molecular Oxygen.
J Mol Catal,1991,70(2):247-257
|
被引
6
次
|
|
|
|
|
7.
Takahiro I. Direct Conversion of Cyclohexane into Adipic Acid with Molecular Oxygen Catalyzed by N-Hydroxyphthalimide Combined with Mn(acac)2 and Co(OAc)2.
Org Process Res Dev,1998,2(4):255-260
|
被引
2
次
|
|
|
|
|
8.
宋明纲. Cr沸石在环己烷氧化反应中的催化性能.
石油化工,2005,34(10):927-931
|
被引
7
次
|
|
|
|
|
9.
苏建玲. 新型Salen-卟啉金属配合物的合成.
表征与应用,2007,4(36):390-393
|
被引
1
次
|
|
|
|
|
10.
侯建敏. 镍（Ⅱ）与meso-四（4-N-甲基吡啶基）卟啉（TMPyP）络合物的伏安法研究.
高等学校化学学报,1994,15(8):1136-1139
|
被引
3
次
|
|
|
|
|
11.
Maldotti A. Oxidation of Cyclohexane by Molecular Oxygen Photo, assisted by Meso-Tetraarylporphyrin Iron(Ⅲ)-Hydroxo Complexes.
lnorg Chem,1996,35(5):1126-1131
|
被引
2
次
|
|
|
|
|
12.
Grinstaff M W. Mechanism of Catalyric Oxygenation of Alkanes by Halogenated Iron Porphyrins.
Science,1994,264(163):1311-1313
|
被引
19
次
|
|
|
|
|
13.
Meunier B. Metalloporphyrins as Versatile Catalysts for Oxidation Reactions and Oxidative DNA Cleavage.
Chem Rev,1992,92(6):1411-1456
|
被引
73
次
|
|
|
|
|
14.
Palakodaty S. Influence of the Thermodynamic State on Cyclohexane Oxidation Kinetics in Carbon Dioxide Medium.
Ind Eng Chem Res,1997,36(6):2066-2074
|
被引
1
次
|
|
|
|
|
15.
Adler A D. On the Preparation of Metalloporphyrins.
J Inorg Nucl Chem,1970,32(7):2443-2445
|
被引
44
次
|
|
|
|
|
16.
郭灿城. 金属卟啉催化环已烷羟基化反应中环己酮的形成机理研究.
化学学报,1998,56(5):2066-2074
|
被引
1
次
|
|
|
|
|
17.
赵仁殿.
芳烃工学.8,2001:344-347
|
被引
1
次
|
|
|
|
|
18.
庄乾坤. 钒-卟啉的电化学行为研究.
中国科学: B辑,1997,27(1):42-50
|
被引
4
次
|
|
|
|
|
19.
McMurry T J. Metalloporphyrin Models for Cytochrome P-450.
Cytochrome P-450, Structure, Mechanism and Biochemistry,1986:1-28
|
被引
1
次
|
|
|
|
|
20.
Lyons J E. Halogenated Metalloporphyrin Complexes as Catalysts for Selective Reactions of Acyclic Alkanes with Molecular Oxygen.
J Catal,1995,155(1):59-73
|
被引
40
次
|
|
|
|
|
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