Synchrotron X-ray quantitative evaluation of transient deformation and damage phenomena in a single nickel-rich cathode particle,Energy & Environmental Science

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Synchrotron X-ray quantitative evaluation of transient deformation and damage phenomena in a single nickel-rich cathode particle
Energy & Environmental Science ( IF 32.4 ) Pub Date : 2020-08-27 , DOI: 10.1039/d0ee02290j
León Romano Brandt _{1,

2,

3,

4,

5} , John-Joseph Marie _{4,

6,

7,

8} , Thomas Moxham _{1,

2,

3,

4,

5} , Dominic P. Förstermann _{4,

6,

7,

8} , Enrico Salvati _{1,

2,

3,

4,

5} , Cyril Besnard _{1,

2,

3,

4,

5} , Chrysanthi Papadaki _{1,

2,

3,

4,

5} , Zifan Wang _{1,

2,

3,

4,

5} , Peter G. Bruce _{4,

6,

7,

8,

9} , Alexander M. Korsunsky _{1,

2,

3,

4,

5}

Affiliation

The performance and durability of Ni-rich cathode materials are controlled in no small part by their mechanical durability, as chemomechanical breakdown at the nano-scale leads to increased internal resistance and decreased storage capacity. The mechanical degradation is caused by the transient lithium diffusion processes during charge and discharge of layered oxide spherical cathode micro-particles, leading to highly anisotropic incompatible strain fields. Experimental characterisation of the transient mechanisms underlying crack and void formation requires the combination of very high resolution in space (sub-micron) and time (sub-second) domains without charge interruption. The present study is focused on sub-micron focused operando synchrotron X-ray diffraction and in situ Ptycho-Tomographic nano-scale imaging of a single nano-structured LiNi_0.8Co_0.1Mn_0.1O₂ core–shell particle during charge to obtain a thorough understanding of the anisotropic deformation and damage phenomena at a particle level. Preferential grain orientation within the shell of a spherical secondary cathode particle provides improved lithium transport but is also associated with spatially varying anisotropic expansion of the hexagonal unit cell in the c-axis and contraction in the a-axis. These effects were resolved in relation to the grain orientation, and the link established with the nucleation and growth of intergranular cracks and voids that causes electrical isolation of active cathode material. Coupled multi-physics Finite Element Modelling of diffusion and deformation inside a single cathode particle during charge and discharge was validated by comparison with experimental evidence and allowed unequivocal identification of key mechanical drivers underlying Li-ion battery degradation.

中文翻译：

同步X射线定量评估单个富镍阴极颗粒中的瞬态变形和破坏现象

富镍正极材料的性能和耐用性在很大程度上受到其机械耐用性的控制，因为纳米级的化学机械击穿导致内部电阻增加和存储容量降低。机械降解是由层状氧化物球形阴极微粒的充电和放电过程中的瞬时锂扩散过程引起的，从而导致高度各向异性的不相容应变场。裂纹和空洞形成的瞬态机理的实验表征需要在空间（亚微米）和时间（亚秒）范围内具有非常高的分辨率，而又不中断电荷。本研究集中于亚微米聚焦操作同步加速器X射线衍射和原位对单个纳米结构的LiNi _0.8 Co _0.1 Mn _0.1 O ₂核-壳粒子在充电过程中进行的Ptycho层析纳米级成像，可以全面了解粒子水平上的各向异性变形和破坏现象。一个球形次级阴极颗粒的壳中优先晶粒取向提供了改进的锂传输，但也与空间上变化的各向异性膨胀在所述六方晶胞的相关Ç -轴和收缩在一个-轴。这些影响与晶粒取向有关，与晶间裂纹和空洞的形核和生长的联系得以建立，这导致活性阴极材料发生电隔离。通过与实验证据进行比较，验证了在充电和放电过程中单个阴极粒子内部扩散和变形的多物理场有限元耦合建模，可以明确识别锂离子电池退化的关键机械驱动因素。

更新日期：2020-10-14

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