| Autor: |
Massaro, Arianna, Lingua, Gabriele, Bozza, Francesco, Piovano, Alessandro, Prosini, Pier Paolo, Muñoz-García, Ana B., Pavone, Michele, Gerbaldi, Claudio |
| Zdroj: |
Chemistry of Materials; July 2024, Vol. 36 Issue: 14 p7046-7055, 10p |
| Abstrakt: |
Modern technologies that can replace state-of-the-art Li-ion batteries (LIBs), such as Na-ion batteries (NIBs), are currently driving new advancements in energy storage research. Developing functional active materials having sustainable features and enhanced performances able to assess their exploitation in the large-scale market represents a major challenge. Rationally designed P2-type layered transition metal (TM) oxides can enable high-energy NIB cathodes, where the tailored composition directly tunes the electrochemical and structural properties. Such positive electrodes need stable electrolytes, and exploration of unconventional room-temperature ionic liquid (RTIL)-based formulations paves the route toward safer options to flammable organic solvents. Notwithstanding the fact that Li+doping in these materials has been proposed as a viable strategy to improve structural issues, an in-depth understanding of structure–property relationship as well as electrochemical testing with innovative RTIL-based electrolytes is still missing. Herein, we propose the solid-state synthesis of P2-Na0.84Li0.1Ni0.27Mn0.63O2(NLNMO) cathode material, which exhibits promising structural reversibility and superior capacity retention upon cycling when tested in combination with RTIL-based electrolytes (EMI-, PYR14-, and N1114-FSI) compared to the standard NaClO4/PC. As unveiled from DFT calculations, lattice integrity is ensured by the reduced Jahn–Teller distortion upon Na removal exerted by Mn4+and Li+sublattices, while the good redox reversibility is mainly associated with the electrochemically active Ni2+/Ni3+/Ni4+series burdening the charge compensation upon desodiation. By declaring the electrochemical compatibility of the P2-NLNMO cathode with three RTIL-based electrolytes and dissecting the role of Li/Ni/Mn sublattices in determining the electrochemical behavior, our comprehensive study enlightens the potential application of this electrode/electrolyte setup for future high-energy NIB prototype cells. |
| Databáze: |
Supplemental Index |
| Externí odkaz: |
|
