Zeolite encapsulated host-guest Cu(II) Schiff base complexes: Superior activity towards oxidation reactions over homogenous catalytic systems

被引:37
|
作者
Kundu, Bidyut Kumar [1 ]
Chhabra, Vaishali [1 ]
Malviya, Novina [1 ]
Ganguly, Rakesh [2 ]
Mishra, Gopal S. [3 ]
Mukhopadhyay, Suman [1 ,4 ]
机构
[1] Indian Inst Technol Indore, Sch Basic Sci, Dept Chem, Khandwa Rd, Indore 453552, Madhya Pradesh, India
[2] Nanyang Technol Univ, Div Chem & Biol Chem, Singapore, Singapore
[3] Univ Tras Os Montes & Alto Douro, Ctr Qim, Lab Mat, P-5001801 Vila Real, Portugal
[4] Indian Inst Technol Indore, Sch Basic Sci, Ctr Biosci & Biomed Engn, Khandwa Rd, Indore 453552, Madhya Pradesh, India
关键词
Cu(II) Schiff base complexes; Single crystal XRD; Homogenous and heterogeneous catalysis; Phenol oxidation mechanism; Metal hydroperoxide species; EFFICIENT HETEROGENEOUS CATALYST; TRANSITION-METAL-COMPLEXES; SELECTIVE OXIDATION; HYDROGEN-PEROXIDE; HYDROXYLATION REACTIONS; METHANE MONOOXYGENASE; COPPER-COMPLEXES; AQUEOUS-SOLUTION; PHENOL; LIGAND;
D O I
10.1016/j.micromeso.2018.05.046
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
Crystalline copper Schiff base complexes of general formula [(CuLNO3)-N-1](n) (1) and [(CuLCl)-Cl-2] (2) (where HL1 = 1-[(3-dimethylaminopropylimino)-methyl] -naphthalen-2-ol and HL2 = 3- [(3-dimethylamino-2,2-dimethyl-propylimino)-methyl]-naphthalen-2-ol) were prepared and well characterized. The guest, metal complexes were entrapped in the supercages of NaY zeolite (host) in the solvent phase through two stage process (i) ion exchange of the selected transition metal (Cu(II)-salt) in the porous structure and (ii) encapsulation of Schiff-base ligands (HL1/HL2) in Cu(II) exchanged zeolite. The novel Cu(II) complexes as well as host-guest catalysts were characterized using various physicochemical [Single crystal XRD, elemental analysis, EDX, scanning electron microscopy (FE-SEM), the Brunauer-Emmet-Teller (BET) adsorption technique (N-2 gas), Inductively coupled plasma (ICP-MS), powder X-ray diffraction (PXRD), thermal analysis (TGA), cyclic voltametry] and spectroscopic techniques [H-1 and C-13 NMR, FT-IR, ESI-MS, electro spin resonance (ESR), diffuse reflectance spectroscopy (DRS), FT-Raman and GC-MS]. Herein, this study reveals the advantage of heterogeneous catalytic methods for the stability of metal complexes into the supercages of zeolite-Y and the selective oxidation of phenol, styrene and cyclohexene in presence of H2O2 at mild reaction conditions. The catalytic activities of the zeolite entrapped Cu(II) complexes were tested with their homogeneous analogous as well. The heterogeneous catalyst can be re-used after recovering for several cycles without decay of activity which was confirmed by PXRD, cyclic voltammetry, SEM and FTIR studies.
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页码:100 / 117
页数:18
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