Bifunctional Noble-Metal-Free Catalyst for the Selective Aerobic Oxidation-Knoevenagel One-Pot Reaction: Encapsulation of Polyoxometalates into an Alkylamine-Modified MIL-101 Framework

Jiamin Sun; Sara Abednatanzi; Hui Chen; Ying-Ya Liu; Karen Leus; Pascal Van Der Voort

doi:10.1021/acsami.1c01621

Bifunctional Noble-Metal-Free Catalyst for the Selective Aerobic Oxidation-Knoevenagel One-Pot Reaction: Encapsulation of Polyoxometalates into an Alkylamine-Modified MIL-101 Framework

ACS Appl Mater Interfaces. 2021 May 26;13(20):23558-23566. doi: 10.1021/acsami.1c01621. Epub 2021 May 11.

Authors

Jiamin Sun¹, Sara Abednatanzi¹, Hui Chen¹, Ying-Ya Liu², Karen Leus¹, Pascal Van Der Voort¹

Affiliations

¹ COMOC-Center for Ordered Materials, Organometallics and Catalysis, Department of Chemistry, Ghent University, Krijgslaan 281, building S3, 9000 Ghent, Belgium.
² State Key Laboratory of Fine Chemicals, Dalian University of Technology, 116023 Dalian, PR China.

PMID: 33973759
DOI: 10.1021/acsami.1c01621

Abstract

One-pot reactions offer economic and environmental advantages. Therefore, the design and synthesis of multifunctional catalysts capable of catalyzing multistep organic transformations are highly important. Herein, an effective bifunctional heterogeneous catalyst is presented. For the first time, the encapsulation of H₅PMo₁₀V₂O₄₀ (PMoV₂) polyoxometalate into the cages of an alkylamine-modified MIL-101 using an optimized double-solvent method is reported. The obtained PMoV₂@DETA-MIL-101 material displays a great catalytic performance (99% conversion of alcohols) for the selective aerobic oxidation-Knoevenagel one-pot reaction. To the best of our knowledge, this is one of the first reports on the usage of noble-metal-free catalysts for the aerobic oxidation-Knoevenagel one-pot reaction without the addition of additives. The catalyst is very stable and can be used for at least five cycles with no leaching of the active sites.

Keywords: Knoevenagel reaction; bifunctional catalyst; double-solvent; metal−organic frameworks; one-pot reaction; polyoxometalate; ship in a bottle catalyst.