3D space-confined Co0.85Se architecture with effective interfacial stress relaxation as anode material reveals robust and highly loading potassium-ion batteries

Abstract

Conversion-type transition metal chalcogenide anodes could bring relatively high specific capacity in potassium ion storage due to multiple electron transport reactions, but often accompanying huge volume changes and resulting in low cycle life and rapid capacity fading.While electrode materials are closely packed, the contact at the interface during potassiation/depotassiation is similar to point-to-point contact, generating strong stress to make self-aggregation occur. In this work, we constructed a 3D carbon framework to confine Co0.85Se nanocrystals in three-dimensional space, both fulfilling the requirements of the material's size in the nano-scale and providing the largest contact area for releasing stress. With this optimization, nitrogen-doped carbon confined Co0.85Se nanocrystals (Co0.85Se@NC) reach an ultra-stable cycle life over 4000 times with a specific capacity of 190.9 mA h g−1 at 500 mA g−1 and provide 155.6 mA h g−1 at 10 A g−1 in the rate capability test. It also renders the areal capacity up to 1.03 mA h cm−2 at 500 mA g−1 in the high-mass loading test. Furthermore, based on the finite element analysis, the 3D confinement strategy has the lowest interfacial stress, ensuring Co0.85Se nanocrystals with high structural integrity. This strategy can relieve the stress issue in the conversion-type anode and demonstrate superior electrochemical performance even at high-loading mass electrodes.