Green oxidation of alkylaromatics using molecular oxygen over mesoporous manganese silicate catalysts

Selvaraj, Manickam and Bhaumik, Asim and Assiri, Mohammed A. and Ch, Subrahmanyam and Ha, Chang-Sik (2020) Green oxidation of alkylaromatics using molecular oxygen over mesoporous manganese silicate catalysts. Dalton Transactions, 49 (28). pp. 9710-9718. ISSN 1477-9226

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Abstract

A very green catalytic method has been introduced for the synthesis of alkylaromatic ketones by solvent-free benzylic oxidation of alkylaromatics with molecular oxygen (O2) over hexagonally mesostructured MnSBA-15 catalysts synthesized with a variety of manganese (Mn) contents using a pH-adjusting direct hydrothermal (pH-aDH) method. For example, the solvent-free oxidation of ethylbenzene (EB) over different mesoporous MnSBA-15 catalysts and uniform pore sized MnMCM-41(31) prepared by an alkaline hydrothermal method has been systematically evaluated. Washed MnSBA-15(4) (W-MnSBA-15(4)) or green mesoporous MnSBA-15(4) obtained after the removal of the non-framework octahedral Mn2O3 species deposited on the active surface of MnSBA-15(4) using a promising chemical treatment method is used for this reaction to evaluate its catalytic activity. Meanwhile the recyclability and hot-filtration experiments for this reaction have been also studied. The catalytic activities obtained from the above catalytic results prove that the W-MnSBA-15(4) has higher EB conversion and APO selectivity than the other mesoporous catalysts used in this reaction. Therefore, in order to find the optimal reaction parameters for this reaction, various reaction parameters with W-MnSBA-15(4) have been thoroughly evaluated. Using W-MnSBA-15(4), the catalytic results obtained with different oxidants used in this reaction have also been discussed clearly. The catalytic results of solvent-free benzylic oxidations with W-MnSBA-15(4) conducted with different alkylaromatic molecules have been obviously discussed. All the mesoporous catalysts used in this reaction have been characterized using several instrumental techniques to confirm them as the standard mesoporous catalysts. The plausible reaction mechanism for the solvent-free oxidation of EB has been successfully reported based on the characterization results of the catalyst and catalytic results. The ESR and UV-vis DRS results of the W-MnSBA-15 catalyst used in these reactions corroborate that the disordered octahedral divalent (Mn2+) and tetrahedral trivalent (Mn3+)-species have been successfully incorporated on the silica surface of the catalysts. Based on the catalytic results, it is noteworthy to observe that mesoporous W-MnSBA-15(4) is a highly active, green and promising heterogeneous catalyst for the selective synthesis of alkylaromatic ketones, since the catalyst produces the best catalytic activity among the other mesoporous Mn silicate catalysts.

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IITH Creators:

IITH Creators	ORCiD
Selvaraj, Manickam	UNSPECIFIED
Ch, Subrahmanyam	https://orcid.org/0000-0002-2643-3854

Item Type:

Article

Uncontrolled Keywords:

Alkalinity; Catalyst selectivity; Catalytic oxidation; Hydrothermal synthesis; Ketones; Manganese oxide; Mesoporous materials; Molecular oxygen; Oxidation; Silica; Silicates; Solvents; Chemical treatment method; Filtration experiments; Heterogeneous catalyst; Hydrothermal methods; Instrumental techniques; Mesoporous catalysts; Reaction parameters; Solvent-free oxidation

Subjects:

Chemistry
Chemistry > Techniques, procedures, apparatus, equipment, materials
Chemistry > Inorganic chemistry
Chemical Engineering

Divisions:

Department of Chemistry

Depositing User:

. LibTrainee 2021

Date Deposited:

19 Jun 2021 05:24

Last Modified:

19 Jun 2021 05:24

URI:

http://raiithold.iith.ac.in/id/eprint/7945