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Heteroleptic chlorosilylene (PhC(NtBu)2SiCl) (1) reacts with unsaturated organic compounds under oxidative addition. Reactions of 1 with cyclooctatetraene (COT) and a diimine afford [1+4]‐cycloaddition products 3 and 6, respectively. In the case of COT, one SiN bond of the amidinato ligand is cleaved, resulting in tetracoordinate silicon, whereas with a diimine a pentacoordinate silicon is formed...
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