Mechanism of CO₂ and H+ Reduction by Ni(cyclam)+ in Aqueous Solution. A Pulse and Continuous Radiolysis Study

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Abstract

The reduction of CO2 and H+ by Ni(cyclam)+ in aqueous solution was found to proceed by the reduction of Ni(cyclam)(CO2)+ or Ni(cyclam)(H)2+ by Ni(cyclam)+. At ambient temperature the rate constants for the bimolecular reactions are 1.6 × 108 and 7.2 × 107 M-1 s-1, respectively. Continuous γ-radiolysis studies have demonstrated nearly quantitative formation of CO from two Ni(cyclam)+ at pH 5.2 under 1 atm of CO2 and in the presence of formate. Under the same conditions, but at low CO2 concentration, the reduction of protons was found to compete with CO2 reduction.

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