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Oleate Epoxidation in a Confined Matrix of Hydrotalcite.

ABSTRACT: Oleate ion was intercalated into a hydrotalcite obtained using a conventional precipitation method and an alternative, novel method involving microwave-assisted ion exchange. The latter method gave a more crystalline hydrotalcite with better textural properties than the former. The spacing between layers in the hydrotalcites was used to epoxidize the double bond in oleate ion. X-ray diffraction patterns revealed that the layered structure of the hydrotalcites was not altered by the reaction. The epoxidation of oleate ion with m-chloroperbenzoic acid (mCPBA) was monitored using Raman spectroscopy. The results of this work testify to the high potential of hydrotalcites as molecular reactors for reactions in confined spaces.

SUBMITTER: Cosano D

PROVIDER: S-EPMC6964289 | biostudies-literature | 2020 Jan

REPOSITORIES: biostudies-literature

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Oleate Epoxidation in a Confined Matrix of Hydrotalcite.

Cosano Daniel D Esquivel Dolores D Romero-Salguero Francisco J FJ Jiménez-Sanchidrián César C Ruiz José Rafael JR

ACS omega 20191227 1

Oleate ion was intercalated into a hydrotalcite obtained using a conventional precipitation method and an alternative, novel method involving microwave-assisted ion exchange. The latter method gave a more crystalline hydrotalcite with better textural properties than the former. The spacing between layers in the hydrotalcites was used to epoxidize the double bond in oleate ion. X-ray diffraction patterns revealed that the layered structure of the hydrotalcites was not altered by the reaction. The ...[more]

PMID: 31956810

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Project description:The catalytic performance with high conversion and high selectivity of Ti-based oxide catalysts have been widely investigated. Besides, stability, which is an essential parameter in the industrial process, lacked fundamental understanding. In this work, we combined computational and experimental techniques to provide insight into the deactivation of P25 and TS-1 Ti-based oxide catalysts during the methyl oleate (MO) epoxidation. The considered deactivation mechanisms are fouling and surface oxygen vacancy (OV). The fouling causes temporary catalyst deactivation through active site blockage but can be removed via calcination in air at high temperature. However, in this work, the OV formation plays an important role in the overall performance of the spent catalyst as the deactivated catalyst after regeneration, cannot be restored to the initial activity. Also, the effects of OV in spent catalysts caused (i) the formation of more Ti3+ species on the surface as evident by XPS and Bader charge analysis, (ii) the activity modification of the active region on the catalyst surface as the reduction in energy gap (Eg) occurred from the formation of the interstates observed in the density of states profiles of spent catalyst modeled by the O-vacant P25 and TS-1 models. This reduction in Eg affects directly the strength of Ti-OOH active site and MO bonding, in which high binding energy contributes to a low conversion because the MO needed an O atom from Ti-OOH site to form the methyl-9,10-epoxy stearate. Hence, the deactivation of the Ti-based oxide catalysts is caused not only by the insoluble by-products blocking the active region but also mainly from the OV. Note that the design of reactive and stable Ti-based oxide catalysts for MO epoxidation needed strategies to prevent OV formation that permanently deactivated the active region. Thus, the interrelation and magnitude between fouling and OV formation on catalyst deactivation will be investigated in future works.

Dataset Information

Oleate Epoxidation in a Confined Matrix of Hydrotalcite.

Publications

Oleate Epoxidation in a Confined Matrix of Hydrotalcite.

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