Evidence for Silica Surface Three- and Five-Membered Metallacycle Intermediates in the Catalytic Cycle of Hydroaminoalkylation of Olefins Using Single-Ti-Metal Catalysts
AuthorsYaacoub, Layal F.
Aljuhani, Maha A.
Al-Harbi, Manal S.
El Eter, Mohamad
KAUST DepartmentChemical Science Program
Imaging and Characterization Core Lab
KAUST Catalysis Center (KCC)
Physical Science and Engineering (PSE) Division
Online Publication Date2020-06-30
Print Publication Date2020-07-13
Permanent link to this recordhttp://hdl.handle.net/10754/663954
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AbstractThe single-site silica-supported group IV metal amido complex [Ti(NMe2)4] gives the tris(amido)-supported fragment [(=Si−O−)Ti(−NMe2)3], which transforms into a three-membered metallacycle (called a metallaaziridine) by an αH transfer between two amido ligands. When the three-membered metallacycle reacts with 1-octene, it gives a five-membered metallacycle by insertion of the double bond into the M−C bond of the metallaziridine. These two metallacycles, key intermediates in the catalytic cycle of the hydroaminoalkylation of terminal olefins, were isolated and fully characterized following the surface organometallic chemistry (SOMC) concept and procedures. This paper shows that surface organometallic chemistry can be used to identify and fully characterize three- and five-membered metallacycles of Ti in the hydroaminoalkylation of olefins.
CitationYaacoub, L. F., Aljuhani, M. A., Jedidi, A., Al-Harbi, M. S., Al Maksoud, W., Wackerow, W., … Basset, J.-M. (2020). Evidence for Silica Surface Three- and Five-Membered Metallacycle Intermediates in the Catalytic Cycle of Hydroaminoalkylation of Olefins Using Single-Ti-Metal Catalysts. Organometallics. doi:10.1021/acs.organomet.0c00246
SponsorsThe King Abdullah University of Science and Technology (KAUST) supported the research. The authors acknowledge core lab at KAUST for their assistance. L.C. and A.J. are grateful to the KAUST Supercomputing Laboratory for the resources. A.J. thank High-Performance Computing Center (AZIZ supercomputer) for the support.
PublisherAmerican Chemical Society (ACS)