<br>层状富锂锰基氧化物的离子-电子双导体界面工程和架构设计,Carbon Energy

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层状富锂锰基氧化物的离子-电子双导体界面工程和架构设计
Carbon Energy ( IF 19.5 ) Pub Date : 2024-11-08 , DOI: 10.1002/cey2.642
Youyou Fang _{1,

2} , Yuefeng Su _{1,

2} , Jinyang Dong _{1,

2} , Jiayu Zhao _{1,

2} , Haoyu Wang ₁ , Ning Li _{1,

2} , Yun Lu _{1,

2} , Yujia Wu _{1,

2} , Wenbo Li _{1,

2} , Ni Yang ₂ , Xiaojuan Wu ₃ , Feng Wu _{1,

2} , Lai Chen _{1,

2}

Affiliation

电动汽车和便携式储能系统的蓬勃发展需要提高锂离子电池（LIB）的能量密度和成本效益，而富锂锰基氧化物（LLO）材料自然在这些领域脱颖而出。尽管具有固有的优势，但这些材料遇到了重大的实际障碍，包括初始库仑效率（ICE）低、循环/速率性能下降以及循环过程中的电压衰减，阻碍了它们的广泛采用。作为回应，我们引入了一种离子-电子双导电（IEDC）表面控制策略，该策略将电子导电石墨烯框架与离子导电异质外延尖晶石 Li ₄ Mn ₅ O ₁₂ 层集成在一起。长时间的电化学和结构分析表明，这种 IEDC 异质结构有效地最大限度地减少了极化，减轻了结构畸变，并增强了电子/离子扩散。密度泛函理论计算突出了广泛的锂 ⁺ 渗流网络和层状尖晶石界面处较低的锂 ⁺ 迁移能。采用 IEDC 接口工程（LMOSG）设计的 LLO 阴极具有改进的 ICE（0.1 C 时为 82.9%）、更高的初始放电容量（0.1 C 时为 296.7 mAh g ⁻¹ ）、出色的倍率能力（5 C 时为 176.5 mAh g ⁻¹ ）和出色的循环稳定性（500 次循环后，5 C 时保留率为 73.7%）。这些发现和新颖的双导电表面结构设计为推进高性能电极材料提供了有希望的方向。

"点击查看英文标题和摘要"

Ionic-electronic dual-conductor interface engineering and architecture design in layered lithium-rich manganese-based oxides

The burgeoning growth in electric vehicles and portable energy storage systems necessitates advances in the energy density and cost-effectiveness of lithium-ion batteries (LIBs), areas where lithium-rich manganese-based oxide (LLO) materials naturally stand out. Despite their inherent advantages, these materials encounter significant practical hurdles, including low initial Coulombic efficiency (ICE), diminished cycle/rate performance, and voltage fading during cycling, hindering their widespread adoption. In response, we introduce an ionic-electronic dual-conductive (IEDC) surface control strategy that integrates an electronically conductive graphene framework with an ionically conductive heteroepitaxial spinel Li₄Mn₅O₁₂ layer. Prolonged electrochemical and structural analyses demonstrate that this IEDC heterostructure effectively minimizes polarization, mitigates structural distortion, and enhances electronic/ionic diffusion. Density functional theory calculations highlight an extensive Li⁺ percolation network and lower Li⁺ migration energies at the layered-spinel interface. The designed LLO cathode with IEDC interface engineering (LMOSG) exhibits improved ICE (82.9% at 0.1 C), elevated initial discharge capacity (296.7 mAh g⁻¹ at 0.1 C), exceptional rate capability (176.5 mAh g⁻¹ at 5 C), and outstanding cycle stability (73.7% retention at 5 C after 500 cycles). These findings and the novel dual-conductive surface architecture design offer promising directions for advancing high-performance electrode materials.

更新日期：2024-11-08

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