Mesoporous Cubic Nanocages Assembled by Coupled Monolayers With 100% Theoretical Capacity and Robust Cycling

High capacity and long cycling often conflict with each other in electrode materials. Despite extensive efforts in structural design, it remains challenging to simultaneously achieve dual high electrochemical properties. In this study, we prepared brand-new completely uniform mesoporous cubic-cages assembled by large d-spacing Ni(OH)₂ coupled monolayers intercalated with VO₄^3– (NiCMCs) using a biomimetic approach. Such unique mesoporous structural configuration results in an almost full atomic exposure with an amazing specific surface area of 505 m²/g and atomic utilization efficiency close to the theoretical limit, which is the highest value and far surpasses all of the reported Ni(OH)₂. Thus, a breakthrough in simultaneously attaining high capacity approaching the 100% theoretical value and robust cycling of 10,000 cycles is achieved, setting a new precedent in achieving double-high attributes. When combined with high-performance Bi₂O₃ hexagonal nanotubes, the resulting aqueous battery exhibits an ultrahigh energy density of 115 Wh/kg and an outstanding power density of 9.5 kW/kg among the same kind. Characterizations and simulations reveal the important role of large interlayer spacing intercalation units and mesoporous cages for excellent electrochemical thermodynamics and kinetics. This work represents a milestone in developing “double-high” electrode materials, pointing in the direction for related research and paving the way for their practical application.

Mesoporous cubic nanocages, assembled from coupled monolayers with expanded interlayer spacing induced by intercalation, achieve nearly 100% theoretical capacity and robust cycling.