By Michele Aresta (auth.), M. Aresta, G. Forti (eds.)
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Through variation of pH, HC0 3 - and C0 3 2 - were ruled out as precursors tor CO formation; the reduction was thus shown proceed from CO 2 . v. , reduction of CO 2 takes place at the electrode surface. It was proposed that adsorption of Ni(cyclam)+ on Hg is followed Dy attack of CO 2 to give a Ni(III) species which is protonated and reduced to yield a Ni(II)-CO complex. Dissociation of CO then regenerates the starting Ni(cyclam)2+ catalyst. Once the concentration of CO increases, several of the species in the proposed cycle may form carbonyl adducts which could be reduced more easily than the original species, helping to explain the relatively high activity of V as an electrocatalyst.
Because of its stability, CO 2 serves along with H20 as the major end product of metabolism and fossil fuel combustion. These two species thus function as the principal repositories or "sinks" ot fixed oxygen in the biosphere. An analysis of CO 2 reduction must therefore begin with thermodynamics. ~Gfo Reduction by Hydrogen. For favorable reduction of CO 2 , either a high energy reductant or an external source of energy must be employed to drive the reaction. Of the possible chemical reductants, molecular hydrogen is clearly the most desirable since it is easily produced by 33 M.
However, there is little direct evidence at this point to support these proposals, and many of the questions regarding the intimate mechanism of CO 2 reduction remain unanswered. 40 C. O'CONNELL ET AL. Indirect Electrochemical Reduction of CO2 Efforts to circumvent the principal difficulties in direct electroreduction of CO 2 , namely the high overpotentials required and the low current efficiencies observed, have centered on the use of homogeneous transition metal complexes as catalysts to mediate the reduction.