A self-healing electrocatalytic system via electrohydrodynamics induced evolution in liquid metal

Catalytic deterioration during electrocatalytic processes is inevitable for conventional composite electrodes, which are prepared by depositing catalysts onto a rigid current collector. In contrast, metals that are liquid at near room temperature, liquid metals (LMs), are potential electrodes that are uniquely flexible and maneuverable, and whose fluidity may allow them to be more adaptive than rigid substrates. Here we demonstrate a self-healing electrocatalytic system for CO2 electroreduction using bismuth-containing Ga-based LM electrodes. Bi2O3 dispersed in the LM matrix experiences a series of electrohydrodynamic-induced structural changes when exposed to a tunable potential and finally transforms into catalytic bismuth, whose morphology can be controlled by the applied potential. The electrohydrodynamically-induced evolved electrode shows considerable electrocatalytic activity for CO2 reduction to formate. After deterioration of the electrocatalytic performance, the catalyst can be healed via simple mechanical stirring followed by in situ regeneration by applying a reducing potential. With this procedure, the electrode's original structure and catalytic activity are both recovered.