<br>Na0.766+xLixNi0.33−xMn0.5Fe0.1Ti0.07O2 向超耐用钠离子电池的双相到单相结构演变,Carbon Energy

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Na0.766+xLixNi0.33−xMn0.5Fe0.1Ti0.07O2 向超耐用钠离子电池的双相到单相结构演变
Carbon Energy ( IF 19.5 ) Pub Date : 2024-04-17 , DOI: 10.1002/cey2.565
Mengting Liu ₁ , Zhiwei Cheng ₁ , Xu Zhu ₁ , Haojie Dong ₁ , Tianran Yan ₂ , Liang Zhang ₂ , Lu Zheng ₁ , Hu‐Rong Yao ₃ , Xian‐Zuo Wang ₁ , Lianzheng Yu ₁ , Bing Xiao ₁ , Yao Xiao ₄ , Peng‐Fei Wang ₁

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具有O3/P2双相晶体结构的层状复合氧化物材料通常表现出O3相的高容量和P2相的高工作电压的组合。然而，它们的实际应用受到热力学相调节困难、复杂的电化学相变和不令人满意的循环寿命的严重阻碍。在此，我们提出了一种通过Li ⁺取代从Na _{0.766+ x} Li _x Ni _{0.33− x} Mn _0.5 Fe _0.1 Ti _0.07 O ₂的双相到单相的有效结构演化策略。 Li ⁺取代的作用不仅通过改变过渡金属（TM）阳离子的局部配位来简化不利的相变，而且还稳定正极-电解质界面，以防止TM阳离子在电池循环过程中降解。因此，热力学稳定的O3-Na _0.826 Li _0.06 Ni _0.27 Mn _0.5 Fe _0.1 Ti _0.07 O ₂正极在0.1 C下具有139.4 mAh g ^-1的高容量，并在高倍率下表现出更长的循环寿命，容量保持率为5 C 下 500 次循环时为 81.6%。这项工作在层状正极材料的热力学结构演化和电化学之间建立了牢固的关系，有助于长寿命钠离子电池的发展。

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Biphase-to-monophase structure evolution of Na0.766+xLixNi0.33−xMn0.5Fe0.1Ti0.07O2 toward ultradurable Na-ion batteries

Layered composite oxide materials with O3/P2 biphasic crystallographic structure typically demonstrate a combination of high capacities of the O3 phase and high operation voltages of the P2 phase. However, their practical applications are seriously obstructed by difficulties in thermodynamic phase regulation, complicated electrochemical phase transition, and unsatisfactory cycling life. Herein, we propose an efficient structural evolution strategy from biphase to monophase of Na_0.766+xLi_xNi_0.33−xMn_0.5Fe_0.1Ti_0.07O₂ through Li⁺ substitution. The role of Li⁺substitution not only simplifies the unfavorable phase transition by altering the local coordination of transition metal (TM) cations but also stabilizes the cathode–electrolyte interphase to prevent the degradation of TM cations during battery cycling. As a result, the thermodynamically robust O3-Na_0.826Li_0.06Ni_0.27Mn_0.5Fe_0.1Ti_0.07O₂ cathode delivers a high capacity of 139.4 mAh g⁻¹ at 0.1 C and shows prolonged cycling life at high rates, with capacity retention of 81.6% at 5 C over 500 cycles. This work establishes a solid relationship between the thermodynamic structure evolution and electrochemistry of layered cathode materials, contributing to the development of long-life sodium-ion batteries.

更新日期：2024-04-17

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