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A hierarchical zeolite-Y hampered metallo-ligand complexes for selective oxidation: A mechanistic point of view.

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Title: A hierarchical zeolite-Y hampered metallo-ligand complexes for selective oxidation: A mechanistic point of view.
Authors: Godhani, Dinesh R.1 drgodhani@yahoo.com, Nakum, Haresh D.1, Parmar, Digvijaysinh K.1, Mehta, Jignasu P.1, Desai, Nisheeth C.1
Source: Microporous & Mesoporous Materials. Nov2016, Vol. 235, p233-245. 13p.
Subjects: Zeolite Y, Ligands (Chemistry), Metal complexes, Oxidation, Nickel compounds, Condensation reactions
Abstract: A series of Ni 2+ and Mn 2+ complexes with ligands 1 and 2 derived from the condensation of 1-(2-hydroxyphenyl)ethan-1-one and/or 1-(5-chloro-2-hydroxyphenyl)ethan-1-one with ethane-1,2-diamine have been synthesized as neat and zeolite Y enslaved complexes. The structures of these complexes were established on the basis of various physicochemical (XRD, ICP-AES, elemental analysis, BET, SEM, magnetic measurements, and TGA) and spectroscopic studies (UV–vis and FTIR). The catalytic performance of these hybrid materials was scrutinized for the oxidation of cyclohexene, phenol, styrene, and benzene using 30% H 2 O 2 as an oxidant. Among all catalysts, 3Y ably catalyzed the cyclohexene (100%), phenol (39.2%), styrene (99.3%), and benzene (20.7%) with the higher selectivity of Cyclohex-2-en-1-one (55.6%), catechol (73.2%), benzaldehyde (87.5%), and phenol (80.7%), respectively. It has been revealed that the presence of electron-withdrawing substituents on the aromatic ring of catalyst degrades the catalytic activity and the selectivity of products. The results show that the heterogeneous systems are easily salvaged and reused without substantial fall in the activity and selectivity. Moreover, the involvement of metal hydroperoxide during the catalytic reaction is confirmed by the preparation, characterization, and utilization of metal hydroperoxide of complex 4 as catalyst over phenol oxidation without oxidant. [ABSTRACT FROM AUTHOR]
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Abstract:A series of Ni 2+ and Mn 2+ complexes with ligands 1 and 2 derived from the condensation of 1-(2-hydroxyphenyl)ethan-1-one and/or 1-(5-chloro-2-hydroxyphenyl)ethan-1-one with ethane-1,2-diamine have been synthesized as neat and zeolite Y enslaved complexes. The structures of these complexes were established on the basis of various physicochemical (XRD, ICP-AES, elemental analysis, BET, SEM, magnetic measurements, and TGA) and spectroscopic studies (UV–vis and FTIR). The catalytic performance of these hybrid materials was scrutinized for the oxidation of cyclohexene, phenol, styrene, and benzene using 30% H 2 O 2 as an oxidant. Among all catalysts, 3Y ably catalyzed the cyclohexene (100%), phenol (39.2%), styrene (99.3%), and benzene (20.7%) with the higher selectivity of Cyclohex-2-en-1-one (55.6%), catechol (73.2%), benzaldehyde (87.5%), and phenol (80.7%), respectively. It has been revealed that the presence of electron-withdrawing substituents on the aromatic ring of catalyst degrades the catalytic activity and the selectivity of products. The results show that the heterogeneous systems are easily salvaged and reused without substantial fall in the activity and selectivity. Moreover, the involvement of metal hydroperoxide during the catalytic reaction is confirmed by the preparation, characterization, and utilization of metal hydroperoxide of complex 4 as catalyst over phenol oxidation without oxidant. [ABSTRACT FROM AUTHOR]
ISSN:13871811
DOI:10.1016/j.micromeso.2016.08.016