Regulating Phase Transition and Oxygen Redox to Achieve Stable High-Voltage O3-Type Cathode Materials for Sodium-Ion Batteries,Advanced Energy Materials

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Regulating Phase Transition and Oxygen Redox to Achieve Stable High-Voltage O3-Type Cathode Materials for Sodium-Ion Batteries
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2023-10-17 , DOI: 10.1002/aenm.202302793
Kai Zhang ₁ , Zhenming Xu ₂ , Guodong Li ₁ , Rui‐Jie Luo ₃ , Cui Ma ₃ , Yonggang Wang ₁ , Yong‐Ning Zhou ₃ , Yongyao Xia ₄

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O3-type layered oxides are promising cathode materials for sodium-ion batteries. However, unsatisfying cyclic stability hinders its practical application, mainly resulting from harmful phase transition and irreversible oxygen redox, especially in high-voltage regions. Herein, a co-doped strategy by incorporating Li⁺, Mg²⁺, Ca²⁺, and Sb⁵⁺ into the O3-Na_0.8Ni_0.4Fe_0.2Mn_0.4O₂ cathode materials is proposed. Both suppressing the undesired phase transition over 4.1 V (vs Na/Na⁺) and reducing the anisotropic strain are achieved with the novel Na_0.8Ni_0.3Fe_0.2Mn_0.3Li_0.1Mg_0.02Ca_0.05Sb_0.03O₂ (LMCS NFM). Moreover, restricted but highly reversible oxygen redox is observed due to strong attraction from Sb⁵⁺ and special “Li–O-vacancy” and “Mg–O-vacancy” configurations. The strategy brings about excellent high-voltage cyclic stability with a reversible capacity of 130 mAh g⁻¹ and a capacity retention of 85% after 250 cycles at 4.2 V, and less thermal runaway risk and moisture sensitivity, increasing the probability of O3-type oxide cathode practical applications.

中文翻译：

调控相变和氧氧化还原实现稳定的钠离子电池高压O3型正极材料

O3型层状氧化物是有前途的钠离子电池正极材料。然而，循环稳定性不理想阻碍了其实际应用，这主要是由于有害的相变和不可逆的氧氧化还原，特别是在高压区域。在此，提出了将Li ⁺、Mg ²⁺、Ca ²⁺和Sb ⁵⁺掺入O3-Na _0.8 Ni _0.4 Fe _0.2 Mn _0.4 O ₂正极材料中的共掺杂策略。新型 Na _0.8 Ni _0.3 Fe _0.2 Mn _0.3 Li _0.1 Mg _0.02 Ca _0.05 Sb _0.03 O ₂ (LMCS NFM)既抑制了 4.1 V（相对于 Na/Na ⁺ ）的不需要的相变，又降低了各向异性应变。此外，由于 Sb ⁵⁺的强烈吸引力以及特殊的“Li-O-空位”和“Mg-O-空位”构型，观察到了受限但高度可逆的氧氧化还原。该策略带来了优异的高电压循环稳定性，可逆容量为130 mAh g ^-1，4.2 V下250次循环后容量保持率为85%，热失控风险和湿度敏感性更低，增加了O3型的概率氧化物阴极实际应用。

更新日期：2023-10-17

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