Exploring the Origin of Anionic Redox Activity in Super Li-Rich Iron Oxide-Based High-Energy-Density Cathode Materials

Yao, Zhenpeng; Chan, Maria Y.; Wolverton, Chris

doi:10.1021/acs.chemmater.2c00322

Exploring the Origin of Anionic Redox Activity in Super Li-Rich Iron Oxide-Based High-Energy-Density Cathode Materials

Journal Article · Wed May 04 00:00:00 EDT 2022 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.2c00322· OSTI ID:1960728

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Shanghai Jiao Tong Univ. (China); Northwestern Univ., Evanston, IL (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
Northwestern Univ., Evanston, IL (United States)

Super alkali-rich materials (alkali:transition metal ratio of ≥2:1), such as Li₅FeO₄, exhibit the potential to realize anionic redox upon deep delithiation. Li₅FeO₄ was shown to undergo reversible cycling between Li₄FeO_3.5 and Li₃FeO_3.5 with combined cation/anion redox, a remarkable capacity of 189 mAh/g, and no O₂ release. However, the impact of phase transformations on the reaction thermodynamics and the correlation between the structural changes and reaction reversibility remain unclear. In this study, we use first-principles calculations to examine the delithiation and (re)lithiation reactions of Li₅FeO₄. We show that the experimentally observed charge and discharge processes go through non-equilibrium pathways. Upon delithiation, the compound undergoes a phase transformation from Li₅FeO₄, with tetrahedrally coordinated (T_d) Fe ions, to a delithiated disordered rocksalt structure, with octahedral (O_h) Fe ions. Fe-ion migration has an asymmetric kinetic barrier that makes T_d → O_h migration facile, whereas the reverse process has a much larger barrier, explaining the difficulties in reaction reversibility. We further elucidate the transition metal and O redox sequences during the charge cycle and identify the complex electrochemistry associated with the dual participation of cationic redox (Fe³⁺/Fe⁴⁺) and anionic redox (O^2–/O^–/O^o). Armed with this knowledge, we conduct high-throughput screening of known alkali-rich transition metal oxides by evaluating their potential to enable reversible anionic redox, with multiple candidates proposed for further experimental trials. Furthermore, our work provides a useful guide for the further development of super alkali-rich anionic-redox-active electrodes for high-energy-density batteries.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Electrochemical Energy Science (CEES)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division

Grant/Contract Number:: AC02-05CH11231; AC02-06CH11357

OSTI ID:: 1960728

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 10 Vol. 34; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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