Enhanced Ion Transport Through Mesopores Engineered with Additional Adsorption of Layered Double Hydroxides Array in Alkaline Flow Batteries

Abstract Efficient mass transfer in electrodes is essential for the electrochemical processes of battery charge and discharge, especially at high rates and capacities. This study introduces a 3D electrode design featuring layered double hydroxides (LDHs) nanosheets array grown in situ on a carbon felt surface for flow batteries. The mesoporous structure and surface characteristic of LDH nanosheets, especially, the hydroxyl groups forming a unique “H‐bonding‐like” geometry with ferrous cyanide ions, facilitate efficient adsorption and ion transport. Thus, the designed LDHs electrode enables the alkaline zinc‐iron flow battery to maintain a voltage efficiency of 81.6% at an ultra‐high current density of 320 mA cm −2 , surpassing the values reported in previous studies. The energy efficiency remains above 84% after 375 cycles at a current density of 240 mA cm −2 . Molecular dynamics simulations verify the enhanced adsorption effect of LDH materials on active ions, thus facilitating ion transport in the battery. This study provides a novel approach to improve mass transport in electrodes for alkaline flow batteries and other energy storage devices.