Abstract
In operando visualization of local electrochemical reactions provides mechanical insights into the dynamic transport of interfacial charge and reactant/product. Electrochemiluminescence is a crossover technique that quantitatively determines Faraday current and mass transport in a straightforward manner. However, the sensitivity is hindered by the low collision efficiency of radicals and side reactions at high voltage. Here, we report a site-selective heat boosting electrochemiluminescence microscopy. By generating a micron-scale heat point in situ at the electrode-solution interface, we achieved an enhancement of luminescence intensity up to 63 times, along with an advance of 0.2 V in applied voltage. Experimental results and finite element simulation demonstrate that the fundamental reasons are accelerated reaction rate and thermal convection via a photothermal effect. The concentrated electrochemiluminescence not only boosts the contrast of single cells by 20.54 times but also enables the site-selective cell-by-cell analysis of the heterogeneous membrane protein abundance. This electrochemical visualization method has great potential in the highly sensitive and selective analysis of local electron transfer events.
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