Oxidation of phenol with H2O2 catalysed by Cu(II), Ni(II) and Zn(II) complexes of N,N′-bis-(salicylidene)diethylenetriamine (H2saldien) encapsulated in Y-zeolite

被引:62
作者
Maurya, MR [1 ]
Titinchi, SJJ
Chand, S
机构
[1] Indian Inst Technol, Dept Chem, Roorkee 247667, Uttar Pradesh, India
[2] Indian Inst Technol, Dept Chem Engn, Roorkee 247667, Uttar Pradesh, India
关键词
decomposition of H2O2; oxidation of phenol; encapsulation; zeolite-Y; catechol and hydroquinone formation;
D O I
10.1016/S1381-1169(03)00193-6
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
Interaction of excess of N,N'-bis(salicylidene)diethylenetriamine (H(2)saldien) with Cu(II), Ni(II) and Zn(H) exchanged zeolite-Y at ca. 90 degreesC leads to the encapsulation of ligand in the super cages of zeolite followed by complexation with metal ions. These encapsulated metal complexes have been characterised by IR and UV-Vis spectroscopic studies and thermal as well as X-ray diffraction (XRD) patterns. All encapsulated complexes serve as catalyst for the decomposition of H2O2 and for the oxidation of phenol to a mixture of catechol and hydroquinone using H2O2 as an oxidant. A suitable reaction condition has been optimised for [Zn(saldien)]-Y by considering the effect of various parameters such as different solvents, concentration of substrate, reaction time and amount of oxidant etc. for the maximum transformation of phenol. Thus, for a fixed amount of catalyst (0.025g), 5.67g of 30% H2O2 in 2 ml MeCN were sufficient enough to catalyse the oxidation of 4.70 g of phenol at 80 degreesC to give maximum transformation of phenol. Under the same reaction conditions the catalytic activity of these complexes follow the order: [Zn(saldien)]-Y (53%) > [Ni(saldien)]-Y (51%) > [Cu(saldien)]-Y (45%) after 24h of reaction time. These catalytic activities were always found better over their respective non-encapsulated complexes. (C) 2003 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:119 / 130
页数:12
相关论文
共 26 条
[1]  
BOWERS C, 1990, J CATAL, V122, P27
[2]   PENTADENTATE LIGANDS .1. NICKEL(II) COMPLEXES OF LINEAR SHIFF BASE LIGANDS DERIVED FROM SUBSTITUTED SALICYLALDEHYDES AND DIETHYLENETRIAMINE AND 2,2'-BIS(AMINOPROPYL)AMINE [J].
COLEMAN, WM ;
TAYLOR, LT .
INORGANIC CHEMISTRY, 1971, 10 (10) :2195-&
[3]   EPR and catalytic investigation of Cu(Salen) complexes encapsulated in zeolites [J].
Deshpande, S ;
Srinivas, D ;
Ratnasamy, P .
JOURNAL OF CATALYSIS, 1999, 188 (02) :261-269
[4]   STRUCTURES AND PROPERTIES OF COPPER(II) AND NICKEL(II) COMPLEXES OF NN'-BIS[(2-HYDROXY-5-METHYLPHENYL)PHENYLMETHYLENE]-4-AZAHEPTANE-1,7-DIAMINE AND RELATED COMPOUNDS - DIRECT COMPARISON OF D8 AND D9 ANALOGUES [J].
HEALY, PC ;
MOCKLER, GM ;
FREYBERG, DP ;
SINN, E .
JOURNAL OF THE CHEMICAL SOCIETY-DALTON TRANSACTIONS, 1975, (08) :691-698
[5]   Selective oxidation over copper and manganese salens encapsulated in zeolites [J].
Jacob, CR ;
Varkey, SP ;
Ratnasamy, P .
MICROPOROUS AND MESOPOROUS MATERIALS, 1998, 22 (1-3) :465-474
[6]   Zeolite-encapsulated copper (X2-salen) complexes [J].
Jacob, CR ;
Varkey, SP ;
Ratnasamy, P .
APPLIED CATALYSIS A-GENERAL, 1998, 168 (02) :353-364
[7]   Oxidation of para-xylene over zeolite-encapsulated copper and manganese complexes [J].
Jacob, CR ;
Varkey, SP ;
Ratnasamy, P .
APPLIED CATALYSIS A-GENERAL, 1999, 182 (01) :91-96
[8]   ZEOLITE-ENCAPSULATED MN(II) COMPLEXES AS CATALYSTS FOR SELECTIVE ALKENE OXIDATION [J].
KNOPSGERRITS, PP ;
DEVOS, D ;
THIBAULTSTARZYK, F ;
JACOBS, PA .
NATURE, 1994, 369 (6481) :543-546
[9]   Novel color isomerism and catalytic activities of Cu(salen) complex encapsulated in a zeolitic matrix [J].
Koner, S .
CHEMICAL COMMUNICATIONS, 1998, (05) :593-594
[10]   ZEOLITE ENCAPSULATED PD(SALEN), A SELECTIVE HYDROGENATION CATALYST [J].
KOWALAK, S ;
WEISS, RC ;
BALKUS, KJ .
JOURNAL OF THE CHEMICAL SOCIETY-CHEMICAL COMMUNICATIONS, 1991, (01) :57-58