Hydrogen‐Bonding Reinforced Flexible Composite Electrodes for Enhanced Energy Storage

Abstract The lack of advanced electrode materials is one of the main factors hindering the development of flexible rechargeable aqueous batteries (RABs) for high specific energy density and structural stability. It is also challenging to achieve high‐capacity performance for both the positive and negative electrodes simultaneously. Here, it is demonstrated that, by smartly designing the composite structures of positive and negative electrodes via one‐step electrodeposition strategy, the energy storage performance of the RAB is largely enhanced. For positive electrode material synthesis, Co‐Cu double hydroxides (Co‐Cu‐DH) nanosheets are skillfully rooted into electroreduced graphene oxide (eRG) via hydrogen bonding, in which graphene oxide reduction, Co‐Cu‐DH nucleation/growth, and formation of hydrogen bonding between Co‐Cu‐DH and eRG simultaneously occur. Moreover, when a RAB based on Co‐Cu‐DH@eRG//FeOOH@eRG using the same composite design strategy is established, a wide operating voltage window of ≈ 1.8 V, a high specific energy density of ≈ 142.8 Wh kg −1 at ≈ 890 W kg −1 , and long‐term cyclic stability (88.5% of capacity retention after 12 000 cycles) are obtained. This study presents a general compositing strategy for the development of advanced electrode materials, and it is expected to stimulate future material synthesis/design in RABs toward the goal of high energy density storage.