Abstract
The electrocatalytic reduction of CO 2 on mercury with Ni(II)-cyclam was studied in detail by cyclic voltammetry, polarography and electrocapillarity of aqueous solutions with and without the catalyst under N 2, CO and CO 2. It is concluded from these electrochemical measurements that (i) the adsorbed complex (Ni(I)-cyclam ad) on Hg, not the reduced complex in solution Ni(I)-cyclam, is the active catalyst for the CO 2 reduction; (ii) both Ni(II)- and Ni(I)-cyclam can adsorb on Hg, and the oxidation states of the adsorbed complexes depend on the electrode potentials; (iii) Ni(I)-cyclam adsorbs on Hg even at −2.0 V (vs. SCE) under N 2, but the surface concentration of Ni(I)-cyclam ad decreases gradually with a decrease in the potential and desorbs completely at potentials more negative than −1.7 V under CO or CO 2; and (iv) the desorption of Ni(I)-cyclam ad under CO or CO 2 is due to the formation of unadsorbable Ni(I)-cyclam-CO by the reaction of Ni(I)-cyclam in solution with dissolved CO or electrocatalytically generated CO from CO 2.
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