Hydrogenative Ring-Rearrangement of Furfural to Cyclopentanone over Pd/UiO-66-NO<sub>2</sub> with Tunable Missing-Linker Defects

Chunhua Wang; Zhiquan Yu; Yuhao Yang; Zhichao Sun; Yao Wang; Chuan Shi; Ying-Ya Liu; Anjie Wang; Karen Leus; Pascal Van Der Voort

doi:10.3390/molecules26195736

Molecules (Sep 2021)

Hydrogenative Ring-Rearrangement of Furfural to Cyclopentanone over Pd/UiO-66-NO<sub>2</sub> with Tunable Missing-Linker Defects

Chunhua Wang,
Zhiquan Yu,
Yuhao Yang,
Zhichao Sun,
Yao Wang,
Chuan Shi,
Ying-Ya Liu,
Anjie Wang,
Karen Leus,
Pascal Van Der Voort

Affiliations

Chunhua Wang: State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China
Zhiquan Yu: State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China
Yuhao Yang: State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China
Zhichao Sun: State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China
Yao Wang: State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China
Chuan Shi: State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China
Ying-Ya Liu: State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China
Anjie Wang: State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China
Karen Leus: Department of Chemistry, Ghent University, Krijgslaan 281-S3, 9000 Ghent, Belgium
Pascal Van Der Voort: Department of Chemistry, Ghent University, Krijgslaan 281-S3, 9000 Ghent, Belgium

DOI: https://doi.org/10.3390/molecules26195736
Journal volume & issue: Vol. 26, no. 19
p. 5736

Abstract

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Upgrading furfural (FAL) to cyclopentanone (CPO) is of great importance for the synthesis of high-value chemicals and biomass utilization. The hydrogenative ring-rearrangement of FAL is catalyzed by metal-acid bifunctional catalysts. The Lewis acidity is a key factor in promoting the rearrangement of furan rings and achieving a high selectivity to CPO. In this work, highly dispersed Pd nanoparticles were successfully encapsulated into the cavities of a Zr based MOF, UiO-66-NO2, by impregnation using a double-solvent method (DSM) followed by H2 reduction. The obtained Pd/UiO-66-NO2 catalyst showed a significantly better catalytic performance in the aforementioned reaction than the Pd/UiO-66 catalyst due to the higher Lewis acidity of the support. Moreover, by using a thermal treatment. The Lewis acidity can be further increased through the creating of missing-linker defects. The resulting defective Pd/UiO-66-NO2 exhibited the highest CPO selectivity and FAL conversion of 96.6% and 98.9%, respectively. In addition, the catalyst was able to maintain a high activity and stability after four consecutive runs. The current study not only provides an efficient catalytic reaction system for the hydrogenative ring-rearrangement of furfural to cyclopentanone but also emphasizes the importance of defect sites.

Published in Molecules

ISSN: 1420-3049 (Online)
Publisher: MDPI AG
Country of publisher: Switzerland
LCC subjects: Science: Chemistry: Organic chemistry
Website: http://www.mdpi.com/journal/molecules

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