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Multiscale yttrium-stabilized pillaring and fluorinated interphase engineering enable fast Mn redox toward 5C-level layered sodium oxide

  • Yuanyuan Liu
  • , Qiwen Ran
  • , Wanyue Sheng
  • , Hanxiao Chang
  • , Rui Cao
  • , Jintao Liu
  • , Mingqi Li
  • , Xingquan Liu
  • , Sridhar Komarneni

Research output: Contribution to journalArticlepeer-review

Abstract

P2-type layered oxide cathode possesses great potential for sodium (Na)-ion batteries due to its high capacity and cost effectiveness. However, its practical utilization has been impeded by structural degradation, sluggish reaction kinetics, and interfacial side reactions. Herein, a synergistic strategy is adopted, involving yttrium (Y) pillar doping and methyl (2,2,2-trifluoroethyl) carbonate‌ (FEMC) electrolyte additive, to realize 5C-level Na0.67MnO2 cathode (denoted as NMYO-FEMC) with highly exposed {010} active facets and high interfacial stability. It is found that atomic-scale Y doping not only expands the interlayer spacing by 0.12 Å, exposing more {010} active facets, but also activates reversible Mn redox reactions through localized electron redistribution. Moreover, FEMC additive, forming a hybrid structure with propylene carbonate solvent, induces a thin yet robust fluorinated interphase to inhibit Mn dissolution and structural collapse. As a result, the optimized NMYO-FEMC cathode shows a high capacity of 113.9 mAh g−1 with 82.8 % retention after 300 cycles at 5C, and also maintains an enhanced cycling stability even at high-temperature (55 °C). Most impressively, the fabricated NMYO-FEMC||hard carbon full cell realizes superior cycling stability with 84.7 % retention after 100 cycles and rate capability. This work elucidates the multi-scale influence mechanism of atomic doping on crystal structure and the crucial role of electrolyte additives in enhancing interfacial stability of layered oxide materials.

Original languageEnglish (US)
Article number167135
JournalChemical Engineering Journal
Volume521
DOIs
StatePublished - Oct 1 2025

All Science Journal Classification (ASJC) codes

  • Environmental Chemistry
  • General Chemistry
  • General Chemical Engineering
  • Industrial and Manufacturing Engineering

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