Stabilizing lattice oxygen redox in layered sodium transition metal oxide through spin singlet state

Wang, Xuelong; Yin, Liang; Ronne, Arthur; Zhang, Yiman; Hu, Zilin; Tan, Sha; Wang, Qinchao; Song, Bohang; Li, Mengya; Rong, Xiaohui; Lapidus, Saul; Yang, Shize; Hu, Enyuan; Liu, Jue

doi:10.1038/s41467-023-43031-6

Title: Stabilizing lattice oxygen redox in layered sodium transition metal oxide through spin singlet state

Journal Article · 22 November 2023 · Nature Communications

DOI: https://doi.org/10.1038/s41467-023-43031-6 · OSTI ID:2217628

Wang, Xuelong; Yin, Liang; Ronne, Arthur; Zhang, Yiman; Hu, Zilin;

; Wang, Qinchao;

;

; Lapidus, Saul; Yang, Shize;

;

Abstract Reversible lattice oxygen redox reactions offer the potential to enhance energy density and lower battery cathode costs. However, their widespread adoption faces obstacles like substantial voltage hysteresis and poor stability. The current research addresses these challenges by achieving a non-hysteresis, long-term stable oxygen redox reaction in the P3-type Na _2/3 Cu _1/3 Mn _2/3 O ₂ . Here we show this is accomplished by forming spin singlet states during charge and discharge. Detailed analysis, including in-situ X-ray diffraction, shows highly reversible structural changes during cycling. In addition, local CuO ₆ Jahn-Teller distortions persist throughout, with dynamic Cu-O bond length variations. In-situ hard X-ray absorption and ex-situ soft X-ray absorption study, along with density function theory calculations, reveal two distinct charge compensation mechanisms at approximately 3.66 V and 3.99 V plateaus. Notably, we observe a Zhang-Rice-like singlet state during 3.99 V charging, offering an alternative charge compensation mechanism to stabilize the active oxygen redox reaction.

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Sponsoring Organization:: USDOE

OSTI ID:: 2217628

Alternate ID(s):: OSTI ID: 2246886; OSTI ID: 2267647

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 14; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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