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A Carbon Electrode Functionalized by a Tricopper Cluster Complex: Overcoming Overpotential and Production of Hydrogen
Natarajan Thiyagarajan1, Damodar Janmanchi1, Yi-Fang Tsai1
1Institute of Chemistry, Academia Sinica, Nankang, Taipei, 11529, Taiwan) (R.O.C.
Abstract:
A study of the oxygen reduction reaction (ORR) on a screen printed carbon electrode surface mediated by the tricopper cluster complex Cu3 (7-N-Etppz(CH2 OH)) dispersed on electrochemically reduced carbon black, where 7-N-Etppz(CH2 OH) is the ligand 3,3'-(6-(hydroxymethyl)-1,4-diazepane-1,4-diyl)bis(1-(4-ethyl piperazin-1-yl)propan-2-ol), is described. Onset oxygen reduction potentials of about 0.92 V and about 0.77 V are observed at pH 13 and pH 7 vs. the reversible hydrogen electrode, which are comparable to the best values reported for any synthetic copper complex. Based on half-wave potentials (E1/2 ), the corresponding overpotentials are about 0.42 V and about 0.68 V, respectively. Kinetic studies indicate that the trinuclear copper catalyst can accomplish the 4 e- reduction of O2 efficiently and the ORR is accompanied by the production of only small amounts of H2 O2 . The involvement of the copper triad in the O2 activation process is also verified.
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