了解 {100} 暴露晶面对尖晶石 LiMn2O4 阴极电化学的关键作用,Inorganic Chemistry Frontiers

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了解 {100} 暴露晶面对尖晶石 LiMn2O4 阴极电化学的关键作用
Inorganic Chemistry Frontiers ( IF 6.1 ) Pub Date : 2023-08-05 , DOI: 10.1039/d3qi01019h
Peiyu Hou ₁ , Yuhang Tian ₁ , Zezhou Lin ₂ , Mohan Dong ₁ , Feng Li ₁

Affiliation

_{人们提出调整尖晶石LiMn 2} O ₄阴极中的{111}、{110}和{100}的暴露晶面，以提高先进锂离子电池的结构稳定性。然而，这些不同的暴露晶面对电化学性能的作用仍然存在争议。在此，我们设计了仅具有暴露的{111}面的八面体LiMn ₂ O _{4和具有暴露的{111}和{100}面的截断八面体LiMn}₂ O ₄ (TO-LMO)。采用该缺锂复合材料作为中间相制备了具有不同比例的暴露{100}/{111}面的TO-LMO。结果表明，被部分 {100} 面截断的暴露的 {111} 面降低了 Mn²⁺含量溶解到电解质中并提高循环稳定性，特别是在高工作温度下。随着暴露的{100}/{111}面的比例增加，这种改进变得显着。具有更高比例的暴露{100}/{111}面的TO-LMO表现出优异的循环稳定性，在50℃下循环200次后容量保持率为91.2%，并且具有高倍率能力，可逆容量达到100 mA hg^{- 1}在 10C。这些发现揭示了{100}暴露晶面对尖晶石锰基阴极电化学性能的改善具有重要影响。

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Understanding the key role of {100} exposed crystal facets on the electrochemistry of the spinel LiMn2O4 cathode

Tuning the exposed crystal facets of {111}, {110}, and {100} in the spinel LiMn₂O₄ cathode has been proposed to boost their structural stability for advanced lithium-ion batteries. Nevertheless, the role of these varied exposed crystal facets on the electrochemical properties is still controversial. Herein, we design octahedral LiMn₂O₄ with only exposed {111} facets and truncated octahedral LiMn₂O₄ (TO-LMO) with exposed {111} and {100} facets. The TO-LMO with different ratios of exposed {100}/{111} facets are prepared by employing the Li-deficient composite as an intermediate phase. It is demonstrated that the exposed {111} facets truncated by a portion of {100} facets reduce the Mn²⁺ content dissolving into the electrolytes and improve the cycling stability, especially at high operating temperatures. The improvement becomes remarkable with an increasing ratio of exposed {100}/{111} facets. The TO-LMO with a higher ratio of exposed {100}/{111} facets shows superior cycling stability with a capacity retention of 91.2% after 200 cycles at 50 °C and high-rate capability with a reversible capacity reaching 100 mA h g⁻¹ at 10C. These findings reveal the vital effect of {100} exposed crystal facets on the improvement of electrochemistry for spinel Mn-based cathodes.

更新日期：2023-08-05

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