Electrocatalytic Water Oxidation by a Monomeric Amidate-Ligated Fe(III)–Aqua Complex
2014-04-16T00:00:00Z (GMT) by
The six-coordinate FeIII-aqua complex [FeIII(dpaq)(H2O)]2+ (1, dpaq is 2-[bis(pyridine-2-ylmethyl)]amino-N-quinolin-8-yl-acetamido) is an electrocatalyst for water oxidation in propylene carbonate–water mixtures. An electrochemical kinetics study has revealed that water oxidation occurs by oxidation to FeV(O)2+ followed by a reaction first order in catalyst and added water, respectively, with ko = 0.035(4) M–1 s–1 by the single-site mechanism found previously for Ru and Ir water oxidation catalysts. Sustained water oxidation catalysis occurs at a high surface area electrode to give O2 through at least 29 turnovers over an 15 h electrolysis period with a 45% Faradaic yield and no observable decomposition of the catalyst.
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