Molecular-oriented single-site heterogeneous catalysis is a powerful approach to address the long-lasting challenge of the structure-activity relationship in catalysis, as it allows molecular level control of the catalytic centers and thus the elucidation of reaction mechanisms. In this dissertation, single-site molybdenum-dioxo species have been immobilized on carbon supports, i.e. activated carbon and carbon nanohorn. Several oxygenates transformations have been studied using the activated carbon-supported molybdenum dioxo catalyst, including reductive carbonyl coupling for functionalized symmetric ether synthesis; oxygen atom transfer for pharmaceutical relevant intermediates reduction; alcohol dehydration for biomass-derived platforms deoxygenation. Combined experimental and computational approaches have been applied for mechanistic study of the alcohol conversion and achieved great agreement. In-depth structural analysis has been applied using the carbon nanohorn matrix and isolated metal centers are observed. The content of this dissertation showcases several unique advantages of molecular-derived single-site heterogeneous catalysis in structural and mechanistic investigation.

Creator

• Li, Jiaqi

DOI

• https://doi.org/10.21985/n2-vm02-z480

Subject

• Chemistry

Language

• en

Alternate Identifier

• http://dissertations.umi.com/northwestern:15519
• etdadmin_upload_813943

Keyword

• Molybdenum-oxo
• Carbon support
• Single-site heterogeneous catalysis

Date created

• 2022-01-01

Resource type

• Dissertation

Rights statement

• In Copyright