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A palladium catalytic method has been developed for the coupling of amides and cyclopropanols to γ-diketones, through simultaneous C–N and C–C activation. Heteroatom ligand exchange and heteroatom-to-carbon ligation mode switching enable the achievement of molecular cross-coupling in an amide N-atom structural context-dependent manner, avoiding any stoichiometric organometallic reagent or base. [ABSTRACT FROM AUTHOR]

A Rh(III)-catalyzed hydrazine-directed C-H olefination approach was developed for synthesizing amino-side-chained poly(phenylene vinylene) (PPV). The creation of such a divergent portfolio of PPV candidates enabled the discovery of a mega Stokes shift, high fluorescence quantum yield, and solid-state fluorescence, highlighting the great prospects of our synthetic protocol as an innovative tool.