Treatment of [Mo(NAr)(2)Cl-2(DME)] (Ar = 2 6-diisopropylphenyl; DME =
1,2-dimethoxyethane) with LiOC(O-Bu-t)CMe2 at low temperature affords
the unexpected carbon-bound molybdenum(VI) enolate complex [Mo(NAr)(2)
Cl{eta 2-C(Me-2)CO2But}] 1; the novel alpha-aminoenolate derivative [M
o(NAr)(2)Cl{eta(2)-CH(NMe2)CO2Et}] 2 is obtained under analogous condi
tions using LiNPr2i/Me2NCH2CO2Et; the structures of 1 and 2 confirm th
e carbophilic nature of the [Mo(NAr)(2)] core.