Abstract

Bimetallic MnCo catalyst, supported on the mesoporous hierarchical MCM-41/halloysite nanotube composite, was synthesized for the first time and proved its efficacy in the selective oxidation of p-xylene to terephthalic acid under conditions of the AMOCO process. Quantitative yields of terephthalic acid were achieved within 3 h at 200–250 °C, 20 atm. of O2 and at a substrate to the Mn + Co ratio of 4–4.5 times higher than for traditional homogeneous system. The influence of temperature, oxygen, pressure and KBr addition on the catalyst activity was investigated, and the mechanism for the oxidation of p-toluic acid to terephthalic acid, excluding undesirable 4-carboxybenzaldehyde, was proposed.

Highlights

  • Terephthalic acid (TPA) and its dimethyl ester are important monomers in thermoresistant and mechanically stable polymer production, such as polyethylene terephthalate (PET) and poly-paraphenylene terephthalamide (Kevlar) [1,2]

  • We present for the first-time synthesis of new heterogeneous bimetallic MnCo catalyst, based on mesoporous hierarchical MCM-41/HNT composite that can be successfully applied for quantitative oxidation of p-xylene to terephthalic acid in the AMOCO process, proving its efficiency, that was 4–4.5 times higher, as compared with a traditional homogeneous system

  • Bimetallic MnCo catalyst, based on MCM-41/HNT composite was synthesized by the wetness impregnation method

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Summary

Introduction

Terephthalic acid (TPA) and its dimethyl ester are important monomers in thermoresistant and mechanically stable polymer production, such as polyethylene terephthalate (PET) and poly-paraphenylene terephthalamide (Kevlar) [1,2]. Catalyst heterogenization is considered as one of the possible ways for improving the AMOCO process It was earlier demonstrated, that the use of CoO and Co3 O4 as catalysts together in the presence of MnO, NiO or CeO co-catalysts and p-toluic acid as a promotor allowed for oxidation without KBr [14]. We present for the first-time synthesis of new heterogeneous bimetallic MnCo catalyst, based on mesoporous hierarchical MCM-41/HNT composite that can be successfully applied for quantitative oxidation of p-xylene to terephthalic acid in the AMOCO process, proving its efficiency, that was 4–4.5 times higher, as compared with a traditional homogeneous system

Results and Discussion
Chemicals
Analyses and Instrumentations
Protocol for the Catalytic Experiments
Conclusions
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