Youyou Fang, Yuefeng Su, Jinyang Dong, Jiayu Zhao, Haoyu Wang, Ning Li, Yun Lu, Yujia Wu, Wenbo Li, Ni Yang, Xiaojuan Wu, Feng Wu, Lai Chen
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引用次数: 0
摘要
电动汽车和便携式储能系统的迅速发展需要锂离子电池(lib)的能量密度和成本效益的进步,而富锂锰基氧化物(LLO)材料在这些领域自然脱颖而出。尽管这些材料具有固有的优势,但它们在实际应用中遇到了很大的障碍,包括初始库仑效率(ICE)低、循环/速率性能降低、循环过程中的电压衰减等,阻碍了它们的广泛应用。为此,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Li4Mn5O12层集成在一起。长期的电化学和结构分析表明,这种IEDC异质结构有效地减少了极化,减轻了结构畸变,并增强了电子/离子扩散。密度泛函理论计算表明,层状尖晶石界面存在广泛的Li+渗透网络和较低的Li+迁移能。采用IEDC界面工程(LMOSG)设计的LLO阴极,在0.1℃下的ICE值提高了82.9%,在0.1℃下的初始放电容量提高了296.7 mAh g−1,在5℃下的倍率能力提高了176.5 mAh g−1,在500次循环后,在5℃下的保留率达到了73.7%。这些发现和新的双导电表面结构设计为高性能电极材料的发展提供了有希望的方向。
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.
期刊介绍:
Carbon Energy is an international journal that focuses on cutting-edge energy technology involving carbon utilization and carbon emission control. It provides a platform for researchers to communicate their findings and critical opinions and aims to bring together the communities of advanced material and energy. The journal covers a broad range of energy technologies, including energy storage, photocatalysis, electrocatalysis, photoelectrocatalysis, and thermocatalysis. It covers all forms of energy, from conventional electric and thermal energy to those that catalyze chemical and biological transformations. Additionally, Carbon Energy promotes new technologies for controlling carbon emissions and the green production of carbon materials. The journal welcomes innovative interdisciplinary research with wide impact. It is indexed in various databases, including Advanced Technologies & Aerospace Collection/Database, Biological Science Collection/Database, CAS, DOAJ, Environmental Science Collection/Database, Web of Science and Technology Collection.