High-voltage and stable co-free LiNiO2 positive electrode for sulfide-based all-solid-state batteries

The development of high-voltage LiNiO<sub>2</sub> is critical for achieving high-energy-density all-solid-state Lithium-ion batteries. However, their practical application is hindered by structural fatigue and interfacial incompatibility with solid electrolytes. Here, a universal heterophase reconstruction strategy is proposed to engineer a stable LiNiO<sub>2</sub>-based positive electrode (LiNi<sub>0.964</sub>Al<sub>0.03</sub>W<sub>0.006</sub>O<sub>2</sub>). In this architecture, high-valence W facilitates the formation of a robust surface spinel phase that exhibits good interfacial compatibility with sulfide electrolytes, while low-valence Al suppresses Li/Ni cation disorder through strong Al-O bonding, stabilizing the layered structure. The synergy of W and Al reinforces a stable layered-spinel framework with enhanced mechanical and chemical integrity, mitigates lattice strain and suppresses the detrimental rock-salt phase and microcracks. Operating up to 4.5 V, LiNi<sub>0.964</sub>Al<sub>0.03</sub>W<sub>0.006</sub>O<sub>2</sub> delivers a high capacity of 187.6 mAh g<sup>-1</sup> at 0.5 C and maintains 122.1 mAh g<sup>-1</sup> even after 720 cycles. This heterophase reconstruction strategy concept is further validated in LiNiO<sub>2</sub>-based systems (LiNi<sub>0.964</sub>Al<sub>0.03</sub>Mo<sub>0.006</sub>O<sub>2</sub>, LiNi<sub>0.964</sub>B<sub>0.03</sub>W<sub>0.006</sub>O<sub>2</sub>, and LiNi<sub>0.964</sub>B<sub>0.03</sub>Nb<sub>0.006</sub>O<sub>2</sub>), confirming a general, scalable design rule for advancing cobalt-free, high-energy and long-life all-solid-state Lithium-ion batteries.

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Journal
Nature Communications
Published
2026-03-08
DOI
https://doi.org/10.1038/s41467-026-70405-3
Primary Topic
Advancements in Battery Materials
Type
article
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article

High-voltage and stable co-free LiNiO2 positive electrode for sulfide-based all-solid-state batteries

Chao Chao Ye, Yue Wang, Shi-Zhang Qiao, Bernt Johannessen et al.
Nature Communications
Advancements in Battery Materials
article

High-voltage and stable co-free LiNiO2 positive electrode for sulfide-based all-solid-state batteries

Chao Chao Ye, Yue Wang, Shi-Zhang Qiao, Bernt Johannessen, Huan Li, Dixing Ni
article en

Abstract

The development of high-voltage LiNiO<sub>2</sub> is critical for achieving high-energy-density all-solid-state Lithium-ion batteries. However, their practical application is hindered by structural fatigue and interfacial incompatibility with solid electrolytes. Here, a universal heterophase reconstruction strategy is proposed to engineer a stable LiNiO<sub>2</sub>-based positive electrode (LiNi<sub>0.964</sub>Al<sub>0.03</sub>W<sub>0.006</sub>O<sub>2</sub>). In this architecture, high-valence W facilitates the formation of a robust surface spinel phase that exhibits good interfacial compatibility with sulfide electrolytes, while low-valence Al suppresses Li/Ni cation disorder through strong Al-O bonding, stabilizing the layered structure. The synergy of W and Al reinforces a stable layered-spinel framework with enhanced mechanical and chemical integrity, mitigates lattice strain and suppresses the detrimental rock-salt phase and microcracks. Operating up to 4.5 V, LiNi<sub>0.964</sub>Al<sub>0.03</sub>W<sub>0.006</sub>O<sub>2</sub> delivers a high capacity of 187.6 mAh g<sup>-1</sup> at 0.5 C and maintains 122.1 mAh g<sup>-1</sup> even after 720 cycles. This heterophase reconstruction strategy concept is further validated in LiNiO<sub>2</sub>-based systems (LiNi<sub>0.964</sub>Al<sub>0.03</sub>Mo<sub>0.006</sub>O<sub>2</sub>, LiNi<sub>0.964</sub>B<sub>0.03</sub>W<sub>0.006</sub>O<sub>2</sub>, and LiNi<sub>0.964</sub>B<sub>0.03</sub>Nb<sub>0.006</sub>O<sub>2</sub>), confirming a general, scalable design rule for advancing cobalt-free, high-energy and long-life all-solid-state Lithium-ion batteries.

Nature Communications
Australian Nuclear Science and Technology Organisation (AU), Australian Synchrotron (AU), National Supercomputing Center in Shenzhen (CN), The University of Adelaide (AU)
Openalex Percentile: Top 31%
Advancements in Battery Materials
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High-voltage and stable co-free LiNiO2 positive electrode for sulfide-based all-solid-state batteries — Chao Chao Ye, Yue Wang, et al. · Nature Communications (2026) | TGRS Research Map | TGRS