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Structure and dynamics of catalytically competent but labile paramagnetic metal-hydrides: The Ti(iii)-H in homogeneous olefin polymerization

Articolo
Data di Pubblicazione:
2020
Abstract:
Metal hydride complexes find widespread application in catalysis and their properties are often understood on the basis of the available crystal structures. However, some catalytically relevant metal hydrides are only spontaneously formed in situ, cannot be isolated in large quantities or crystallised and their structure is therefore ill defined. One such example is the paramagnetic Ti(iii)-hydride involved in homogeneous Ziegler-Natta catalysis, formed upon activation of CpTi(iv)Cl3 with modified methylalumoxane (MMAO). In this contribution, through a combined use of electron paramagnetic resonance (EPR), electron-nuclear double resonance (ENDOR) and hyperfine sublevel correlation (HYSCORE) spectroscopies we identify the nature of the ligands, their bonding interaction and the extent of the spin distribution. From the data, an atomistic and electronic model is proposed, which supports the presence of a self-assembled ion pair between a cationic terminal Ti-hydride and an aluminate anion, with a hydrodynamic radius of ca. 16 Å.
Tipologia CRIS:
03A-Articolo su Rivista
Keywords:
EPR spectroscopy, ENDOR, HYSCORE, olefin polymerisation, metal-hydride
Elenco autori:
Salvadori E.; Chiesa M.; Buonerba A.; Grassi A.
Autori di Ateneo:
CHIESA Mario
SALVADORI Enrico
Link alla scheda completa:
https://iris.unito.it/handle/2318/1765153
Link al Full Text:
https://iris.unito.it/retrieve/handle/2318/1765153/688513/d0sc04967k.pdf
Pubblicato in:
CHEMICAL SCIENCE
Journal
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https://pubs.rsc.org/en/content/articlelanding/2020/sc/d0sc04967k#!divAbstract
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