Multi‐Anion Intercalated Layered Double Hydroxide Nanosheet‐Assembled Hollow Nanoprisms with Improved Pseudocapacitive and Electrocatalytic Properties

Abstract Electrochemically active hollow nanostructured materials hold great promise in diverse energy conversion and storage applications, however, intricate synthesis steps and poor control over compositions and morphologies have limited the realization of delicate hollow structures with advanced functional properties. In this study, we demonstrate a one‐step wet‐chemical strategy for co‐engineering the hollow nanostructure and anion intercalation of nickel cobalt layered double hydroxide (NiCo‐LDH) to attain highly electrochemical active energy conversion and storage functionalities. Self‐templated pseudomorphic transformation of cobalt acetate hydroxide solid nanoprisms using nickel nitrate leads to the construction of well‐defined NiCo‐LDH hollow nanoprisms (HNPs) with multi‐anion intercalation. The unique hierarchical nanosheet‐assembled hollow structure and efficiently expanded interlayer spacing offer an increased surface area and exposure of active sites, reduced mass and charge transfer resistance, and enhanced stability of the materials. This leads to a significant improvement in the pseudocapacitive and electrocatalytic properties of NiCo‐LDH HNP with respect to specific capacitance, rate and cycling performance, and OER overpotential, outperforming most of the recently reported NiCo‐based materials. This work establishes the potential of manipulating sacrificial template transformation for the design and fabrication of novel classes of functional materials with well‐defined nanostructures for electrochemical applications and beyond.