Redox non-innocence permits catalytic nitrene carbonylation by (dadi)Ti 0000000000000000000000000000000000 0000000000000000000000000000000000 0000000000000000000000000000000000 0000000000000000000000000000000000 0000000000000000000000000000000000 0000000000000000000000000000000000 0000000000000000000000000000000000 0000000000000000000000000000000000 0000000000000000000000000000000000 0000000000000000000000000000000000 0000000000000000000000000000000000 0000000000000000000000000000000000 00000000000000000000

Chemical Science
Spencer P HeinsSamantha N MacMillan

Abstract

Application of the diamide, diimine {-CHN(1,2-C6H4)N(2,6-(i)Pr2-C6H3)}2(m) ((dadi) (m) ) ligand to titanium provided adducts (dadi)TiL x (1-L x ; L x = THF, PMe2Ph, (CNMe)2), which possess the redox formulation [(dadi)(4-)]Ti(iv)L x , and 22 πe(-) (4n + 2). Related complexes containing titanium-ligand multiple bonds, (dadi)TiX (2 X; X = O, NAd), exhibit a different dadi redox state, [(dadi)(2-)]Ti(iv)X, consistent with 20 πe(-) (4n). The Redox Non-Innocence (RNI) displayed by dadi (m) impedes binding by CO, and permits catalytic conversion of AdN3 + CO to AdNCO + N2. Kinetics measurements support carbonylation of 2 NAd as the rate determining step. Structural and computational evidence for the observed RNI is provided.

References

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Aug 11, 2017·Dalton Transactions : an International Journal of Inorganic Chemistry·Zachary W Davis-Gilbert, Ian A Tonks
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Dec 11, 2021·Inorganic Chemistry·Elena Álvarez-RuizCristina Santamaría
Dec 29, 2021·Journal of the American Chemical Society·Anders ReinholdtDaniel J Mindiola

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Methods Mentioned

BETA
X-ray
NMR

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