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Deprotonation of the readily available organometallic aldehyde derivative [(η 4 -C 7 H 7 CHO)Fe(CO) 3 ] (2) with NaN(SiMe 3 ) 2 in benzene solution at ambient temperature afforded the anionic formylcycloheptatrienyl complex Na[(η 3 -C 7 H 6 CHO)Fe(CO) 3 ] (3). The anion is fluxional in solution and displays a unique ambident reactivity towards electrophiles (MeI, Me 3 SiCl). New substituted [(η 4 -RC 7 H 6 CHO)Fe(CO) 3 ] and [(η 4 -heptafulvene)Fe(CO) 3 ] complexes have been identified as the products. Treatment of 3 with 0.5 equivalents of dimeric [(COD)RhCl] 2 (COD ϭ 1,5-cyclooctadiene) afforded the functionalized Fe-Rh cycloheptatrienyl complex

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