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Title: Post-Synthesis Strategies to Prepare Mesostructured and Hierarchical Silicates for Liquid Phase Catalytic Epoxidation
Author: Gomes, Diana M.
Neves, Patrícia
Antunes, Margarida M.
Fernandes, António J. S.
Pillinger, Martyn
Valente, Anabela A.
Keywords: Catalytic epoxidation
Porous materials
Hierarchical zeolite
Ordered mesoporous silica
Issue Date: Dec-2022
Publisher: MDPI
Abstract: Olefin epoxidation is an important transformation for the chemical valorization of olefins, which may derive from renewable sources or domestic/industrial waste. Different post-synthesis strategies were employed to introduce molybdenum species into mesostructured and hierarchical micro-mesoporous catalysts of the type TUD-1 and BEA, respectively, to confer epoxidation activity for the conversion of relatively bulky olefins (e.g., biobased methyl oleate, DL-limonene) to epoxide products, using tert-butyl hydroperoxide as an oxidant. The influences of (i) the type of metal precursor, (ii) type of post-synthesis impregnation method, (iii) type of support and (iv) top-down versus bottom-up synthesis methodologies were studied to achieve superior catalytic performances. Higher epoxidation activity was achieved for a material prepared via (post-synthesis) incipient wetness impregnation of MoO2(acac)2 (acac = acetylacetonate) on (pre-treated) siliceous TUD-1 and calcination; for example, methyl oleate was converted to the corresponding epoxide with 100% selectivity at 89% conversion (70 °C). Catalytic and solid-state characterization studies were conducted to shed light on material stability phenomena.
Peer review: yes
DOI: 10.3390/catal12121513
ISSN: 2073-4344
Appears in Collections:CICECO - Artigos
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