Mesoporous Silica-Supported Amidozirconium-Catalyzed Carbonyl Hydroboration

Autor: Zhuoran Wang, Aaron D. Sadow, Naresh Eedugurala, Umesh Chaudhary, Kapil Kandel, Nicholas C. Nelson, Marek Pruski, Igor I. Slowing, Takeshi Kobayashi
Rok vydání: 2015
Předmět:
Zdroj: ACS Catalysis. 5:7399-7414
ISSN: 2155-5435
Popis: The hydroboration of aldehydes and ketones using a silica-supported zirconium catalyst is reported. Reaction of Zr(NMe2)4 and mesoporous silica nanoparticles (MSN) provides the catalytic material Zr(NMe2)n@MSN. Exhaustive characterization of Zr(NMe2)n@MSN with solid-state (SS)NMR and infrared spectroscopy, as well as through reactivity studies, suggests its surface structure is primarily ≡SiOZr(NMe2)3. The presence of these nitrogen-containing zirconium sites is supported by 15N NMR spectroscopy, including natural abundance 15N NMR measurements using dynamic nuclear polarization (DNP) SSNMR. The Zr(NMe2)n@MSN material reacts with pinacolborane (HBpin) to provide Me2NBpin and the material ZrH/Bpin@MSN that is composed of interacting surface-bonded zirconium hydride and surface-bonded borane ≡SiOBpin moieties in an approximately 1:1 ratio, as well as zirconium sites coordinated by dimethylamine. The ZrH/Bpin@MSN is characterized by 1H/2H and 11B SSNMR and infrared spectroscopy and through its reactivity wit...
Databáze: OpenAIRE