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Pyrrolidine‐derived functionalized chiral ionic liquids (FCILs) have been found to catalyze asymmetric SN1 α‐alkylations of ketones and aldehydes with up to 99 % yield, >99:1 dr and 87 % ee. The FCIL catalysts enable SN1 α‐alkylations of cyclic ketones, particularly of 3‐ and 4‐substituted cyclohexanones with excellent diastereoselectivity and good enantioselectivity, featuring unprecedented desymmetrization...
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