Electrochemiluminescence reaction pathways in nanofluidic devices
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RESEARCH PAPER
Electrochemiluminescence reaction pathways in nanofluidic devices Silvia Voci 1 & Hanan Al-Kutubi 2 & Liza Rassaei 3 & Klaus Mathwig 4 & Neso Sojic 1,5 Received: 27 February 2020 / Revised: 25 March 2020 / Accepted: 30 March 2020 # Springer-Verlag GmbH Germany, part of Springer Nature 2020
Abstract Nanofluidic electrochemical devices confine the volume of chemical reactions to femtoliters. When employed for light generation by electrochemiluminescence (ECL), nanofluidic confinement yields enhanced intensity and robust luminescence. Here, we investigate different ECL pathways, namely coreactant and annihilation ECL in a single nanochannel and compare light emission profiles. By high-resolution imaging of electrode areas, we show that different reaction schemes produce very different emission profiles in the unique confined geometry of a nanochannel. The confrontation of experimental results with finite element simulation gives further insight into the exact reaction ECL pathways. We find that emission strongly depends on depletion, geometric exclusion, and recycling of reactants in the nanofluidic device. Keywords Electrochemiluminescence . Electroanalytical methods . Nanofluidic device . Fluorescence/luminescence
Introduction Electrochemiluminescence (ECL) is a controllable form of chemiluminescence where light emission results from an initial electron-transfer reaction occurring at an electrode surface [1–5]. It is a powerful analytical method with remarkable performances
Silvia Voci and Hanan Al-Kutubi contributed equally to this work. Electronic supplementary material The online version of this article (https://doi.org/10.1007/s00216-020-02630-8) contains supplementary material, which is available to authorized users. * Klaus Mathwig [email protected] * Neso Sojic [email protected] Liza Rassaei [email protected] 1
Bordeaux INP, Univ. Bordeaux, CNRS, ISM, UMR 5255, Site ENSCBP, 16, Avenue Pey-Berland, 33607 Pessac, France
2
Department of Radiation Science and Technology, Delft University of Technology, Mekelweg 15, 2629 JB Delft, The Netherlands
3
Rotterdam, The Netherlands
4
Groningen Research Institute of Pharmacy, Pharmaceutical Analysis, University of Groningen, P.O. Box 196, 9700 AG Groningen, The Netherlands
5
Department of Chemistry, South Ural State University, Chelyabinsk, Russian Federation 454080
due to its dual intrinsic nature, which is based on the combination of electrochemistry and photophysics. ECL provides many advantages for analytical applications: time, duration, and position of the ECL-emitting region can be manipulated electrochemically [6–8]. In addition, it allows the simultaneous measurement of two experimental parameters (i.e., Faradaic current and light intensity) as a function of the applied potential, like fluorescence-based spectroelectrochemistry techniques [9–11]. Therefore, ECL offers a great selectivity and control over the light-emitting reactions. The most extensively investigated electrochemiluminophore is tris(2,2′-bipyridyl)ruthenium(II
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