Ultrathin Cobalt-Based Prussian Blue Analogue Nanosheet-Assembled Nanoboxes Interpenetrated with Carbon Nanotubes as a Fast Electron/Potassium-Ion Conductor for Superior Potassium Storage.

Abstract

Rechargeable potassium-ion batteries (PIBs) are regarded as potential substitutes for industrial lithium-ion batteries in large scale energy storage systems due to the world's abundant potassium supplies. Althogh cobalt hexacyanocobaltate (CoHCC) exhibits broad potential as a PIB anode material, its performance is currently unsatisfactory. Herein, novel 5 nm scale ultrathin CoHCC nanosheet-assembled nanoboxes with interspersed carbon nanotubes (CNTs/CoHCC nanoboxes) are fabricated to realize a highly reactive PIB anode. The ultrathin CoHCC layers substantially accelerate electron conduction and provide numerous active sites, while the connected CNTs provide fast axial electron transport. Consequently, the optimized anode exhibits a remarkable discharge capacity of 580.9 mAh g-1 at 0.1 A g-1 and long-term stability with 71.3% retention over 1000 cycles. In situ and ex situ characterizations and density functional theory calculations are further employed to elucidate the K+ storage process and the reason for the enhanced performance of the CNTs/CoHCC nanoboxes.