Comparison of Co with Mn and Fe in LDH-hosted sulfonato-salen catalysts for olefin epoxidation

被引:45
作者
Bhattacharjee, Samiran [1 ]
Dines, Trevor. J. [2 ]
Anderson, James A. [1 ]
机构
[1] Univ Aberdeen, Dept Chem, Surface Chem & Catalysis Grp, Aberdeen AB24 3UE, Scotland
[2] Univ Dundee, Div Elect Engn & Phys, Dundee DD1 4HN, Scotland
关键词
D O I
10.1021/jp804339d
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Sulphonato-salen complexes containing Mn(III), Co(III), and Fe(III) metal centers intercalated into Zn/Al layered double-hydroxide (LDH) host have been synthesized and tested as catalysts for the epoxidation of cyclohexene and dicyclopentadiene Using pivaldehyde and Molecular oxygen at atmospheric pressure and room temperature. Oxidation of cyclohexene gave cyclohexene oxide and 2-cyclohexen-1-one as reaction products, whereas dicyclopentadiene was transformed to the cot-responding monoepoxide. Selectivity was found to depend on the central metal ion. Activity (TOF) increased according to LDH-[Fe(Cl)(salen)] < LDH-[Co(Cl)(salen)] < LDH-[Mn(Cl)(salen)] in both case of cyclohexene and dicyclopentadiene epoxidation. The structures of the metal(III) sulfonato-salen complexes were modeled by density functional theory calculations in order to compare differences in dimensions and geometries with differences in gallery height and catalytic behavior.
引用
收藏
页码:14124 / 14130
页数:7
相关论文
共 46 条
[1]  
ALI MA, 1977, J INORG NUCL CHEM, V39, P265
[2]   Chiral salen complexes: An overview to recoverable and reusable homogeneous and heterogeneous catalysts [J].
Baleizao, Carlos ;
Garcia, Hermenegildo .
CHEMICAL REVIEWS, 2006, 106 (09) :3987-4043
[3]   DENSITY-FUNCTIONAL THERMOCHEMISTRY .3. THE ROLE OF EXACT EXCHANGE [J].
BECKE, AD .
JOURNAL OF CHEMICAL PHYSICS, 1993, 98 (07) :5648-5652
[4]   Comparison of the epoxidation of cyclohexene, dicyclopentadiene and 1,5-cyclooctadiene over LDH hosted Fe and Mn sulfonato-salen complexes [J].
Bhattacharjee, S ;
Anderson, JA .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2006, 249 (1-2) :103-110
[5]   Synthesis and application of layered double hydroxide-hosted catalysts for stereoselective epoxidation using molecular oxygen or air [J].
Bhattacharjee, S ;
Dines, TJ ;
Anderson, JA .
JOURNAL OF CATALYSIS, 2004, 225 (02) :398-407
[6]   Synthesis and characterization of novel chiral sulfonato-salen-manganese(III) complex in a zinc-aluminium LDH host [J].
Bhattacharjee, S ;
Anderson, JA .
CHEMICAL COMMUNICATIONS, 2004, (05) :554-555
[7]   INTERCALATION OF [(MOO2)-O-VI(O2CC(S)PH(2))(2)](2-) IN A ZN(II)-AL(III) LAYERED DOUBLE HYDROXIDE HOST - A STRATEGY FOR THE HETEROGENEOUS CATALYSIS OF THE AIR OXIDATION OF THIOLS [J].
CERVILLA, A ;
CORMA, A ;
FORNES, V ;
LLOPIS, E ;
PALANCA, P ;
REY, F ;
RIBERA, A .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1994, 116 (04) :1595-1596
[8]   MODEL REACTIONS OF MOLYBDO-REDUCTASE - A NOVEL AND HIGHLY EFFICIENT REDUCTION OF NITROBENZENE TO ANILINE CATALYZED BY A MOLYBDENUM-MEDIATED OXYGEN-ATOM TRANSFER-REACTION [J].
CERVILLA, A ;
CORMA, A ;
FORNES, V ;
LLOPIS, E ;
PEREZ, F ;
REY, F ;
RIBERA, A .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1995, 117 (25) :6781-6782
[9]   THIO DERIVATIVES OF BETA-DIKETONES AND THEIR METAL CHELATES .7. VISIBLE-ULTRAVIOLET SPECTRA OF SOME MONOTHIO-BETA-DIKETONES AND THEIR METAL CHELATES [J].
CHASTON, SHH ;
LIVINGST.SE .
AUSTRALIAN JOURNAL OF CHEMISTRY, 1967, 20 (06) :1079-&
[10]   Catalytic asymmetric epoxidation of unfunctionalised olefins using silica, LDH and resin-supported sulfonato-Mn(salen) complex [J].
Choudary, BM ;
Ramani, T ;
Maheswaran, H ;
Prashant, L ;
Ranganath, KVS ;
Kumar, KV .
ADVANCED SYNTHESIS & CATALYSIS, 2006, 348 (4-5) :493-498