Abstract
Nonhysteretic and reversible (nHR) oxygen redox is desirable for high-energy-density cathodes in lithium-ion batteries (LIBs); however, serious challenges remain. An interactive design concept that mimics the nHR anionic activity of Li-excess Na oxide for sodium-ion batteries is proposed herein to harness the full potential of the oxygen capacity of Li2MnO3 in LIBs. We investigated the reversible stacking sequence transition induced by layer gliding accompanied by oxygen redox during (de)sodiation in Na-layered oxides, with Li ions at the tetrahedral sites of the charged structure. Intriguingly, the stacking transition in F-doped Li2MnO3 was identified as a reversible reaction, and the delithiated phase exhibiting no O-O dimers included a consistent Li configuration of the Na cathode. Although in-plane Mn migration resulted in the formation of molecular O2 trapped in the bulk, the detailed electronic structures in the normal delithiation mode exhibited reversible lattice O(2p) activity.
Original language | English |
---|---|
Pages (from-to) | 4554-4560 |
Number of pages | 7 |
Journal | Energy and Environmental Science |
Volume | 15 |
Issue number | 11 |
DOIs | |
Publication status | Published - 30 Sept 2022 |
Bibliographical note
Publisher Copyright:© 2022 The Royal Society of Chemistry.