By Michele Aresta (auth.), M. Aresta, G. Forti (eds.)
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Additional info for Carbon Dioxide as a Source of Carbon: Biochemical and Chemical Uses
In contrast to these results, Lewis and Lieber have recently studied the cobalt phthalocyanine (CoPc) system on carbon electrodes and have found that the only C-containing product is CO. 2 v vs SCE of CoPc deposited on pyrolytic graphite or carbon cloth in aqueous solution at pH 5 under 1 atm of CO 2 yielded CO and H2 (2:1) with an overal I current etficiency for more than 105 turnovers ot 90-95 I.. Only trace amounts of oxalate and formate were detected by spot tests. The pH dependence of the CoPc reduction waves and the lack of current enhancement under CO 2 relative to Ar led the authors to propose that reduction occurs by protonation of CoPc- followed by a second reduction and subsequent reaction with CO 2 , Use of CoPc dissolved in aqueous THF solution rather than adsorbed onto the C electrode resulted in poor stability and low catalytic efficiency for CO 2 reduction.
34 ° electrolysis of H2 0, and it serves as an effective atom acceptor via the formation of H2 0. However, the simple reductions of CO 2 by H2 as shown in eqns (1)-(4) reveal themselves to be thermodynamically unfavorable with small, positive aGo,s, although the reactions can be driven when H2 0 is removed from the reaction system as it is formed. It is only when the reduction of CO 2 reaches methanol as the carbon product that H2 reduction, eqn (4), becomes favorable. This analysis, however, does not take into account the intermediate oxidation states which the carbon atom of CO 2 must pass through before reaching the CH 30H product.
The photolysis is done in triethanolamine-DMF with the system showing very high selectivity to CO formation. 15 at 436 nm. There is agreement that the initial reaction of the excited state of ReX(CO)3(bpy) involves reductive quenChing, eqn (16), and that the reduced species then rapidly reacts with CO 2 while the cation TEOA+ undergoes oxidative decomposition. ReCI(CO)3(bDY)* + TEOA ~ ReCI (CO)3(bpyl (16 ) Subsequent electrocatalytic studies by Meyer using ReCI(CO)3(bpy) support the intermediacy of the 19 e- species ReCI(CO)3(bpy)- and its rapid reaction with CO 2 .