Lowering Sodium-Storage Lattice Strains of Layered Oxide Cathodes by Pushing Charge Transfer on Anions

Na Li; Wen Yin; Baotian Wang; Fangwei Wang; Xiaoling Xiao; Jinkui Zhao; Enyue Zhao

doi:10.1002/eem2.12671

Energy & Environmental Materials ›› 2024, Vol. 7 ›› Issue (4) : e12671 DOI: 10.1002/eem2.12671

RESEARCH ARTICLE

Lowering Sodium-Storage Lattice Strains of Layered Oxide Cathodes by Pushing Charge Transfer on Anions

Na Li ¹^,²
, Wen Yin ³^,⁴
, Baotian Wang ³^,⁴
, Fangwei Wang ¹^,²^,³
, Xiaoling Xiao ⁵
, Jinkui Zhao ¹^,²
, Enyue Zhao ¹^,^†

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Abstract

Due to a high energy density, layered transition-metal oxides have gained much attention as the promising sodium-ion batteries cathodes. However, they readily suffer from multiple phase transitions during the Na extraction process, resulting in large lattice strains which are the origin of cycled-structure degradations. Here, we demonstrate that the Na-storage lattice strains of layered oxides can be reduced by pushing charge transfer on anions (O^2-). Specifically, the designed O3-type Ru-based model compound, which shows an increased charge transfer on anions, displays retarded O3–P3–O1 multiple phase transitions and obviously reduced lattice strains upon cycling as directly revealed by a combination of ex situ X-ray absorption spectroscopy, in situ X-ray diffraction and geometric phase analysis. Meanwhile, the stable Na-storage lattice structure leads to a superior cycling stability with an excellent capacity retention of 84% and ultralow voltage decay of 0.2 mV/cycle after 300 cycles. More broadly, our work highlights an intrinsically structure-regulation strategy to enable a stable cycling structure of layered oxides meanwhile increasing the materials’ redox activity and Na-diffusion kinetics.

Keywords

anionic redox reaction / lattice strains / layered oxide cathodes / phase transitions / sodium-ion battery

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Na Li, Wen Yin, Baotian Wang, Fangwei Wang, Xiaoling Xiao, Jinkui Zhao, Enyue Zhao. Lowering Sodium-Storage Lattice Strains of Layered Oxide Cathodes by Pushing Charge Transfer on Anions. Energy & Environmental Materials, 2024, 7(4): e12671 DOI:10.1002/eem2.12671

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