The reaction of the functional, zwitterionic quinonoid molecule (6E)-4-(butylamino)-6-(butyliminio)-3-oxo-2-(1,1,2,2-tetracyanoethyl)cyc lohexa-1,4-dien-1-olate, [C6H-2-{C(CN)(2)C(CN)(2)H}]-4,6-(center dot center dot center dot NH n-Bu)(2)-1,3(center dot center dot center dot O)(2) (2), which has been previously prepared by regioselective insertion of TCNE into the C-H bond adjacent to the C center dot center dot center dot O bonds of the zwitterionic benzoquinone monoimine (6E)-4- (butylamino)-6-(butyliminio)-3-oxocyclohexa-1,4-dien-l-olate, C6H2-4,6-(center dot center dot center dot NHn-Bu)(2)-1,3(center dot center dot center dot O)(2) (1), with 2 equiv of [Pt(C2H4)(PPh3)(2)], afforded the Pt(0) complex [Pt(PPh3)(2)(4)] (6) (4 = 2-HCN; (6E)-4-(butylamino)-6-(butyliminio)-3-oxo-2-(1,2,2-tricyanoethenyl)cyclo hexa-1,4-dien-1-olate), in which a tricyanoethenyl moiety is pi-bonded to the metal. A metal-induced HCN elimination reaction has thus taken place. The same complex was obtained directly by the reaction of 1 equiv of the Pt(0) complex [Pt(C2H4)(PPh3)(2)] with the olefinic ligand [C6H-2-{C(CN)=C(CN)(2)}]-4,6-(center dot center dot center dot NHn-Bu)(2)-1,3-(center dot center dot center dot O)(2)) (4), previously obtained by the reaction of 2 with NEt3 in THF. A similar reactivity pattern was observed between 2 and 2 equiv of the Pd(0) precursor [Pd(dba)(2)] in the presence of dppe, which led to [Pd(dppe) (4)] (7), which was also directly obtained from 4 and 1 equiv [Pd(dba)(2)]/dppe. In contrast to the behavior of the TCNE derivative 2, the reaction of the TCNQ derivative (6E)-4-(butylamino)-6-(butyliminio)-2-(dicyano(4-(dicyanomethyl)phenyl)methyl)-3-oxocyclohexa-1,4-dien-1-olate, [C6H-2-{C-(CN)(2)p-C6H4C(CN)(2)H}]-4,6-(center dot center dot center dot NHn-Bu)(2)-1,3-(center dot center dot center dot O)(2)) (3), with 2 equiv of [Pt(C2H4)(PPh3)(2)] led to formal oxidative-addition of the C-H bond of the C(CN)(2)H moiety to give the Pt(II) hydride complex trans-[PtH(PPh3)(2){N=C=C(CN)p-C6H4C(CN)(2)-2-[C6H-4,6-(center dot center dot center dot NHn-Bu)(2)-1,3-(center dot center dot center dot O)(2))}] (8). The molecular structures of 3, 4, 6.0.5(H2O), and 8.3(CH2Cl2) have been determined by single-crystal X-ray diffraction.