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Bipolar electrochemistry is based on the gradient distribution of free-electron density along an electrically isolated electrode, which causes a positive electrode potential at one end and a negative potential at the other, allowing for wide applications in analytical chemistry and materials science. To take full advantage of its wireless and high-throughput features, various types of optical probes, such as pH indicators and fluorescence and electrochemiluminescence reagents, have often been used to indirectly monitor the interfacial electron transfer through chromogenic or fluorogenic reactions. Herein, we report the first probe-free imaging approach that can directly visualize the distribution of the interfacial potential in bipolar electrodes, providing essential information for the validation and development of the theory and applications of bipolar electrochemistry. This approach is based on the sensitive dependence of surface plasmon resonance imaging on the local electron density in the electrode, which enables the direct mapping of potential with a spatial resolution close to the optical diffraction limit, a temporal resolution of 50 ms, and a sensitivity of 10 mV. In addition, in contrast to previous optical readouts that relied on faradaic reactions, the present work achieved the impedance-based measurements under non-faradaic conditions. It is anticipated that this technique will greatly expand the application of bipolar electrochemistry as a platform for chemical and biosensing. [ABSTRACT FROM AUTHOR]

Abstract: Here we report a novel approach for the detection of adenosine in cancer cells by electrochemiluminescence (ECL) on a wireless indium tin oxide bipolar electrode (BPE). In this approach, ferrocene (Fc) which is labeled on adenosine aptamer is enriched on one pole of the BPE by hybridization with its complementary DNA (ssDNA) and oxidized to Fc+ under an external voltage of 5.0V at the two ends of BPE. Then, a reversed external voltage was added on the BPE, making Fc+ enriched pole as cathode. The presence of Fc+ promotes the oxidation reaction on the anodic pole of the BPE, resulting in a significant increase of ECL intensity using Ru(bpy)3 2+/tripropylamine (TPA) system as test solution. The presence of target adenosine was reflected by the ECL signal decrease on the anodic pole caused by the target-induced removal of ferrocene-aptamer on the cathodic pole. The decrease of ECL signal was logarithmically linear with the concentration of ATP in a wide range from 1.0fM to 0.10μM. This ECL biosensing system could accurately detect the level of adenosine released from cancer cells. [Copyright &y& Elsevier]

Abstract: The cationic luminescence probe, tris(2,2′-bipyridyl)ruthenium(II) complex ([Ru(bpy)3]2+), was incorporated into laponite-modified glassy carbon electrode (GCE) via two strategies, namely, the adsorption and intercalation methods. These two incorporation methods resulted in different microenvironment for the immobilized [Ru(bpy)3]2+ within laponite as well as the different host–guest and guest–guest interactions. Herein, cyclic voltammetry and electrochemiluminescence (ECL) were innovatively performed to monitor the interactions. Tripropylamine (TPA) was used as coreactant in the electrochemical and ECL system. [Copyright &y& Elsevier]