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Thioiminium salts derived from these sulfur isologues of amides readily react with lithium acetylides to lead to several types of products, including α,β-unsaturated ketones, whereas sequential additions of lithium acetylides and Grignard reagents afford propargylamines. The direct addition of organolithium and Grignard reagents to thioformamides proceeds with high efficiency to give a range of tertiary 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