TY - JOUR
T1 - Electrogenerated Chemiluminescence by in Situ Production of Coreactant Hydrogen Peroxide in Carbonate Aqueous Solution at a Boron-Doped Diamond Electrode
AU - Irkham,
AU - Fiorani, Andrea
AU - Valenti, Giovanni
AU - Kamoshida, Naoki
AU - Paolucci, Francesco
AU - Einaga, Yasuaki
N1 - Funding Information:
I. acknowledges a “Design the Future” International Student Award, Keio University. A.F. acknowledges the Japan Society for the Promotion of Science (Fellowship ID No. P19333) and Grant-in-Aid for JSPS Fellows (19F19333).
Publisher Copyright:
© 2019 American Chemical Society.
PY - 2020/1/22
Y1 - 2020/1/22
N2 - An electrogenerated chemiluminescence (ECL) system by in situ coreactant production, where Ru(bpy)3 2+ emission is generated at a boron-doped diamond (BDD) electrode, is presented. The system takes advantage of the unique properties of BDD to promote oxidation of carbonate (CO3 2-) into peroxydicarbonate (C2O6 2-), which further reacts with water to form hydrogen peroxide (H2O2), which acts as a coreactant for Ru(bpy)3 2+ ECL. Investigation of the mechanism reveals that ECL emission is triggered by the reduction of H2O2 to hydroxyl radicals (OH•), which later react with the reduced Ru(bpy)3 + molecules to form excited states, followed by light emission. The ECL signal was found to increase with the concentration of CO3 2- therefore, with the concentration of electrogenerated H2O2, although at the same time, higher concentrations of H2O2 can quench the ECL emission, resulting in a decrease in intensity. The carbonate concentration, pH, and oxidation parameters, such as potential and time, were optimized to find the best emission conditions.
AB - An electrogenerated chemiluminescence (ECL) system by in situ coreactant production, where Ru(bpy)3 2+ emission is generated at a boron-doped diamond (BDD) electrode, is presented. The system takes advantage of the unique properties of BDD to promote oxidation of carbonate (CO3 2-) into peroxydicarbonate (C2O6 2-), which further reacts with water to form hydrogen peroxide (H2O2), which acts as a coreactant for Ru(bpy)3 2+ ECL. Investigation of the mechanism reveals that ECL emission is triggered by the reduction of H2O2 to hydroxyl radicals (OH•), which later react with the reduced Ru(bpy)3 + molecules to form excited states, followed by light emission. The ECL signal was found to increase with the concentration of CO3 2- therefore, with the concentration of electrogenerated H2O2, although at the same time, higher concentrations of H2O2 can quench the ECL emission, resulting in a decrease in intensity. The carbonate concentration, pH, and oxidation parameters, such as potential and time, were optimized to find the best emission conditions.
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U2 - 10.1021/jacs.9b11842
DO - 10.1021/jacs.9b11842
M3 - Article
C2 - 31922404
AN - SCOPUS:85078328327
SN - 0002-7863
VL - 142
SP - 1518
EP - 1525
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 3
ER -