Enabling Stable and Nonhysteretic Oxygen Redox Capacity in Li-Excess Na Layered Oxides

Geon Hee Yoon, Sojung Koo, Sung Joon Park, Jaewoon Lee, Chanwoo Koo, Seok Hyun Song, Tae Yeol Jeon, Hyungsub Kim, Jong Seong Bae, Won Jin Moon, Sung Pyo Cho, Duho Kim, Seung Ho Yu

Research output: Contribution to journalArticlepeer-review

4 Citations (Scopus)

Abstract

The demands for higher energy density of rechargeable batteries have been continuously increasing recently, and cationic redox based current cathodes have little scope to further increase energy density since they already exhibit near-theoretical specific capacities. In this regard, oxygen redox (OR) reactions have emerged as a promising breakthrough for sodium-ion battery (SIB) cathodes. Most OR-based layered oxides suffer from drastic hysteretic-oxygen capacities upon discharging after the first charging. In contrast, stable and nonhysteretic oxygen capacities are herein enabled via Al3+ incorporation into Li-excess Na layered oxide (NLMO). By combining experimental work and first-principles calculations, it is found that there is an additional stable phase during the oxygen redox for Al incorporated NLMO in comparison with bare NLMO, which is a critical factor in extending and stabilizing the discharge capacity in thermodynamics. In addition, the additional redox-inactive Al3+ leads to heterogeneous oxygen redox rather than homogeneous, which results in stabilization of the oxide framework with sensitively control of the oxygen participation upon cycling.

Original languageEnglish
Article number2103384
JournalAdvanced Energy Materials
Volume12
Issue number11
DOIs
Publication statusPublished - 2022 Mar 17

Keywords

  • Al substitution
  • first-principles calculations
  • layered oxides
  • oxygen redox
  • sodium-ion batteries

ASJC Scopus subject areas

  • Renewable Energy, Sustainability and the Environment
  • Materials Science(all)

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