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Imidazolidine‐4‐thiones (ITOs) are cyclic, secondary amines that were considered as potential prebiotic organocatalysts for light‐driven α‐alkylations of aldehydes by bromoacetonitrile (BAN). Recent studies showed that the initially supplied ITOs represent the pre‐catalyst because they undergo S‐alkylation with BAN to give 4‐(alkylthio)‐3‐imidazolines (TIMs). Given that the same reagent mix that undergoes...