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A Carbon Electrode Functionalized by a Tricopper Cluster Complex: Overcoming Overpotential and Production of Hydrogen Peroxide in the Oxygen Reduction Reaction
Author(s) -
Thiyagarajan Natarajan,
Janmanchi Damodar,
Tsai YiFang,
Wanna Wondemagegn Hailemichael,
Ramu Ravirala,
Chan Sunney I.,
Zen JyhMyng,
Yu Steve S.F.
Publication year - 2018
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.201712226
Subject(s) - overpotential , chemistry , catalysis , copper , hydrogen peroxide , ligand (biochemistry) , carbon fibers , inorganic chemistry , oxygen , reversible hydrogen electrode , electrode , electrocatalyst , redox , electrochemistry , working electrode , materials science , organic chemistry , biochemistry , composite number , receptor , composite material
A study of the oxygen reduction reaction (ORR) on a screen printed carbon electrode surface mediated by the tricopper cluster complex Cu 3 (7‐ N ‐Etppz(CH 2 OH)) dispersed on electrochemically reduced carbon black, where 7‐ N ‐Etppz(CH 2 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 ( E 1/2 ), 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 O 2 efficiently and the ORR is accompanied by the production of only small amounts of H 2 O 2 . The involvement of the copper triad in the O 2 activation process is also verified.