Bi‐Interlayer Strategy for Modulating NiCoP‐Based Heterostructure toward High‐Performance Aqueous Energy Storage Devices

Abstract Nickel‐cobalt (NiCo) phosphides (NCPs) possess high electrochemical activity, which makes them promising candidates for electrode materials in aqueous energy storage devices, such as supercapacitors and zinc (Zn) batteries. However, the actual specific capacitance and rate capability of NCPs require further improvement, which can be achieved through reasonable heterostructural design and loading conditions of active materials on substrates. Herein, novel hierarchical Bi‐NCP heterogeneous structures with built‐in electric fields consisting of bismuth (Bi) interlayers (electrodeposited on carbon cloth (CC)) are designed and fabricated to ensure the formation of uniform high‐load layered active materials for efficient charge and ion transport. The resulting CC/Bi‐NCP electrodes show a uniform, continuous, and high mass loading (>3.5 mg) with a superior capacitance reaching 1200 F g −1 at 1 A g −1 and 4129 mF cm −2 at 1 mA cm −2 combined with high‐rate capability and durable cyclic stability. Moreover, assembled hybrid supercapacitors (HSCs), supercapatteries, and alkaline Zn‐ion (AZBs) batteries constructed using these electrodes deliver high energy densities of 64.4, 81.8, and 319.1 Wh kg −1 , respectively. Overall, the constructed NCPs with excellent aqueous energy storage performance have the potential for the development of novel transition metal‐based heterostructure electrodes for advanced energy devices.