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Electrochemical reduction of CO, catalysed by [RUL'(L~)(CO),]~+ [L',L2 = (bipy),, (bipy)(dmbipy), (dmbipy),, or (phen),], [Ru(phen),(CO)CI] + (phen = 1 ,lo-phenanthroline), and [RuL(CO),CI,] [ L = 2,2'-bipyridine (bipy) or 4,4'-dimethyl-2,2'-bipyridine (dmbipy)] were carried out by controlledpotential electrolysis at -1.30 V vs. saturated calomel electrode in acetonitrile-water (4: 1 , v/v), MeOH, or MeCN-MeOH (4: 1 , v/v). In acetonitrile-water (4: 1 , v/v) n o difference in activities between the catalysts was observed, however i n MeOH the amounts of carbon monoxide produced became larger than those of HC0,-upon introduction of the dmbipy ligand. This is attributed to the equilibrium constants among the reaction intermediates [RuL'(L2) (C0),l2+, [RuL1(L2)(CO)-{C(O)OH}] +, and [RuL1(L2)(CO)(C0,-)] + which become smaller o n substitution of bipy by dmbipy, because of the donor property of the CH, group.

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The one-electron reduced species of N-propyl-4,4′-bipyridinium cation (1+) which is generated under electrolysis at −1.1 V vs. SCE was found to be able to react with CO2 although it is even a neutral radical. The intermediate CO2 adduct was furthermore reduced by one-electron at the same electrolysis potential to form a stable CO2 adduct.