New 1,3‐bis‐N‐acyliminium species generated easily with nontoxic Bi(OTf)3 catalyst at very low loadings (2 mol‐%) were trapped inter‐ and intramolecularly with various poly‐nucleophiles. This mild, efficient, practical and general tandem approach provides an array of substituted isoindolinones and cyclic N,O‐acetals.
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