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Highly stereoselective and rapid (<1 min) addition reactions to the imine double bond of 2-(methylimino)acetate complexes [L4Co(O2CCHNCH3)]2+ [L4 = (en)2 (7), (tren) (11)] were achieved in aqueous solution with nitromethane, ethyl 3-oxobutanoate or diethyl malonate. The molecular structures of two product complexes, rac-(Δ*-RC*-SN*)-[Co(en)2(O2CCH[CH2NO2]NHCH3)]ZnCl4 and rac-(Δ*-RC*-SN*)-[Co(en)2(O2CCH[CH2COCH3]NHCH3)]ZnCl4, were established by X-ray diffraction.
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