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.

Tribo-electrochemistry induced artificial solid electrolyte interface by self-catalysis.

Potassium (K) metal is a promising alkali metal anode for its high abundance. However, dendrite on K anode is a serious problem which is even worse than Li. Artificial SEI (ASEI) is one of effective routes for suppressing dendrite. However, there are still some issues of the ASEI made by the traditional methods, e.g. weak adhesion, insufficient/uneven reaction, which deeply affects the ionic diffusion kinetics and the effect of inhibiting dendrites. Herein, through a unique self-catalysis tribo-electrochemistry reaction, a continuous and compact protective layer is successfully constructed on K metal anode in seconds. Such a continuous and compact protective layer can not only improve the K+ diffusion kinetics, but also strongly suppress K dendrite formation by its hard mechanical properties derived from rigid carbon system, as well as the improved K+ conductivity and lowered electronic conductivity from the amorphous KF. As a result, the potassium symmetric cells exhibit stable cycles last more than 1000 h, which is almost 500 times that of pristine K.

Synchronous Healing of Li Metal Anode via Asymmetrical Bidirectional Current.

The creation of Li metal anodes while minimizing dendrite growth is an important challenge for developing high-energy density batteries. Dendrites can originate from an inhomogeneous charge distribution or an irregular substrate, and often, the way to suppress dendrite growth is to avoid their formation altogether (ion-uniform mechanism over a shelf time). Herein, we propose a different route to eliminate dendrite formation, called an asymmetrical bidirectional current mode (ABCM) of charging, leading to a healable Li metal anode and resulting in a positive feedback cycle. This mode allows for a stable cyclic performance and suppresses dendrite formation effectively (while holding the polarization ∼27 mV for over 1,000 h), and provides a better result than suppressing Li dendrites via weakening of the Li dendrite (ion-uniform mechanism). These results indicate that ABCM may be a promising way to stabilize the Li anode of Li metal batteries, without any chemical/physical modification of the anode.