Lithium-ion batteries (LIBs) have been used widely in portable electronics, and hybrid-electric and all-electric vehicles for many years. However, there is a growing need to develop new cathode materials that will provide higher cell energy densities for advanced applications. Several candidates, including Li₂MnO₃-stabilized LiM′O₂ (M′ = Mn/Ni/Co) structures, Li₂Ru_0.75Sn_0.25O₃ (i.e., 3Li₂RuO₃–Li₂SnO₃), and disordered Li₂MoO₃–LiCrO₂ compounds can yield capacities exceeding 200 mA h g⁻¹, alluding to the constructive role that Li₂MO₃ (M⁴⁺) end-member compounds play in the electrochemistry of these systems. Here, we catalog the family of Li₂MO₃ compounds as active cathodes or inactive stabilizing agents using high-throughput density functional theory (HT-DFT). With an exhaustive search based on design rules that include phase stability, cell potential, resistance to oxygen evolution, and metal migration, we predict a number of new Li₂M_IO₃–Li₂M_IIO₃ active/inactive electrode pairs, in which M_I and M_II are transition- or post-transition metal ions, that can be tested experimentally for high-energy-density LIBs.

中文翻译：

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高容量富锂分层氧化物电极的材料设计：Li ₂ MnO ₃及更高

锂离子电池（LIB）已在便携式电子产品以及混合动力和全电动汽车中广泛使用了很多年。然而，对开发新的阴极材料的需求不断增长，该材料将为高级应用提供更高的电池能量密度。包括Li ₂ MnO ₃稳定的LiM'O ₂（M'= Mn / Ni / Co）结构，Li ₂ Ru _0.75 Sn _0.25 O ₃（即3Li ₂ RuO ₃ -Li ₂ SnO ₃）和无序结构在内的几种候选物Li ₂ MoO ₃ –LiCrO ₂所述化合物可产生超过200 mA hg ^-1的容量，这暗示了Li ₂ MO ₃（M ⁴⁺）端基化合物在这些系统的电化学中起的建设性作用。在这里，我们使用高通量密度泛函理论（HT-DFT）将Li ₂ MO ₃化合物家族分类为活性阴极或惰性稳定剂。通过基于包括相稳定性，电池电势，抗氧析出性和金属迁移的设计规则的详尽搜索，我们预测了许多新的Li ₂ M _I O ₃ –Li ₂ M _II O ₃活性/非活性电极对，其中M _I和M _II是过渡或过渡金属离子，可以通过实验测试高能量密度的LIB。