Herein, we describe the formation of biologically relevant N-alpha,beta-unsaturated acyl sulfoximines via phosphine-catalyzed C-C bond activation of cyclopropenones with weakly nucleophilic sulfoximines. The new process does not require a transition metal or external oxidant and displays high regioselectivity and exclusive E-selectivity. Other salient features of the method are a broad substrate scope, high compatibility with various functional groups, and high atom economy.

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