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“True” acyl anions would be desirable as synthetic reagents, but are inaccessible. Only some N,N-disubstituted carbamoyllithium compounds such as (1), which have presumably ionic, angular structures, are persistent in solution. Further carbonylation of (1) affords interesting secondary products, e.g. hydroxymalonamide (2), N-Monosubstituted lithium amides such as (3) rearrange to N-lithioformamides (4) on carbonylation.