Deciphering an Abnormal Layered-Tunnel Heterostructure Induced by Chemical Substitution for the Sodium Oxide Cathode

Angew Chem Int Ed Engl. 2020 Jan 20;59(4):1491-1495. doi: 10.1002/anie.201912101. Epub 2019 Dec 5.

Abstract

Demands for large-scale energy storage systems have driven the development of layered transition-metal oxide cathodes for room-temperature rechargeable sodium ion batteries (SIBs). Now, an abnormal layered-tunnel heterostructure Na0.44 Co0.1 Mn0.9 O2 cathode material induced by chemical element substitution is reported. By virtue of beneficial synergistic effects, this layered-tunnel electrode shows outstanding electrochemical performance in sodium half-cell system and excellent compatibility with hard carbon anode in sodium full-cell system. The underlying formation process, charge compensation mechanism, phase transition, and sodium-ion storage electrochemistry are clearly articulated and confirmed through combined analyses of in situ high-energy X-ray diffraction and ex situ X-ray absorption spectroscopy as well as operando X-ray diffraction. This crystal structure engineering regulation strategy offers a future outlook into advanced cathode materials for SIBs.

Keywords: electrochemistry; layered-tunnel heterostructure; oxide cathodes; sodium-ion batteries; structural evolution.