Co-reactant-on-Demand ECL: Electrogenerated Chemiluminescence by the in Situ Production of S2O82- at Boron-Doped Diamond Electrodes

Irkham; Takeshi Watanabe; Andrea Fiorani; Giovanni Valenti; Francesco Paolucci; Yasuaki Einaga

doi:10.1021/jacs.6b09020

Co-reactant-on-Demand ECL: Electrogenerated Chemiluminescence by the in Situ Production of S₂O₈^2- at Boron-Doped Diamond Electrodes

J Am Chem Soc. 2016 Dec 7;138(48):15636-15641. doi: 10.1021/jacs.6b09020. Epub 2016 Nov 22.

Authors

Irkham¹, Takeshi Watanabe¹, Andrea Fiorani², Giovanni Valenti², Francesco Paolucci², Yasuaki Einaga^{1

3}

Affiliations

¹ Department of Chemistry, Keio University , 3-14-1 Hiyoshi, Yokohama 223-8522, Japan.
² Department of Chemistry "G. Ciamician", University of Bologna , Via Selmi, 2, 40126 Bologna, Italy.
³ JST-ACCEL , 3-14-1 Hiyoshi, Yokohama 223-8522, Japan.

PMID: 27934028
DOI: 10.1021/jacs.6b09020

Abstract

A novel co-reactant-free electrogenerated chemiluminescence (ECL) system is developed where Ru(bpy)₃²⁺ emission is obtained on boron-doped diamond (BDD) electrodes. The method exploits the unique ability of BDD to operate at very high oxidation potential in aqueous solutions and to promote the conversion of inert SO₄^2- into the reactive co-reactant S₂O₈^2-. This novel procedure is rather straightforward, not requiring any particular electrode geometry, and since the co-reactant is only generated in situ, the interference with biological samples is minimized. The underlying mechanism is similar to that of the Ru(bpy)₃²⁺/S₂O₈^2- system; however, the intensity of the emitted signal increases linearly with [SO₄^2-] up to ∼0.6 M, with possible implications for analytical uses of the proposed procedure.

Publication types

Research Support, Non-U.S. Gov't