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Pnictogen-based vanadacyclobutadiene complexes
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DOI：10.1039/d4sc05884d.png)
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摘要
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The reactivity of the V 00000000000000000 00000000000000000 00000000000000000 01111111111111110 00000000000000000 01111111111111110 00000000000000000 01111111111111110 00000000000000000 00000000000000000 00000000000000000 CtBu multiple bonds in the complex (dBDI)VCtBu(OEt2) (C) (dBDI2- = ArNC(CH3)CHC(CH2)NAr, Ar = 2,6-iPr2C6H3) with unsaturated substrates such as NCR (R = Ad or Ph) and PCAd leads to the formation of rare 3d transition metal compounds featuring alpha-aza-vanadacyclobutadiene, (dBDI)V(kappa 2-C,N-tBuCC(R)N) (R = Ad, 1; R = Ph, 2) and beta-phospha-vanadacyclobutadiene moieties, (dBDI)V(kappa 2-C,C-tBuCPCAd) (3). Complexes 1-3 are characterized using multinuclear and multidimensional NMR spectroscopy, including the preparation of the 50% 15N-enriched isotopologue (dBDI)V(kappa 2-C,N-tBuCC(Ad)15N) (1-15N). Solid-state structural analysis is used to determine the dominant resonance structures of these unique pnictogen-based vanadacyclobutadienes. A systematic comparison with the known vanadacyclobutadiene (dBDI)V(kappa 2-C,C-tBuCC(H)CtBu) (4) is also presented. Theoretical investigations into the electronic structure of 2-4 highlight the crucial role of unique V-heteroatom interactions in stabilizing the vanadacyclobutadienes and identify the most dominant resonance structures.
Keyword:
RING-OPENING METATHESIS
METAL-CARBON BONDS
ALKYNE METATHESIS
ALKYLIDENE COMPLEXES
CRYSTAL-STRUCTURE
BIS(TRIMETHYLSILYL)ACETYLENE COMPLEXES
TUNGSTENACYCLOBUTADIENE COMPLEXES
TITANIUM ALKYLIDYNES
GROUP-4 METALLOCENES
CROSS-METATHESIS
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IF:
7.4
论文数:
1.7W
被引数:
9.3W
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