Supporting Data for Operando monitoring of single-particle kinetic state-of-charge heterogeneities and cracking in high-rate Li-ion anodes

This data set contains all the data presented in the main text figures (for the manuscript titled 'Operando monitoring of single-particle kinetic state-of-charge heterogeneities and cracking in high-rate Li-ion anodes'). The information on how the data was acquired and processed is detailed in the open access manuscript + SI. This data set also contains the MATLAB code used to conduct the phase field modelling in the same manuscript.
Figure 1: (Panel b) Galvanostatic cycling data of NWO (voltage vs specific capacity) for five cycles cycles at 1C, 5C and 20C. (Panel c) Li-ion self-diffusion coefficient in NWO, as a function of temperature and Li-concentration.
Figure 2: (Panel a) SEM image of NWO particles. (Panel c) Unprocessed optical images of a NWO particle during a galvanostatic cycle at 5C. (Panel d) Cell voltage, single particle scattering intensity, and single particle length change, during galvanostatic cycles at 1C, 5C and 20C. (Panel e) Change in the c-lattice parameter of NWO, measured by operando and ex situ XRD, as a function of Li-content. Optically-determined length change for multiple individual NWO particles.
Figure 3: (Panel a&d) Cell voltage and applied current for two galvanostatic cycles at 5C, initially preceded by a 2.8V hold. (Panel b) Differential optical images showing a particle of NWO at the beginning of the first 5C cycle shown in a. (Panel c) Cell voltage for the first 50s of the first 5C cycle. Differential linecut along a NWO particle during this same time period. (Panel e) Differential optical images showing a particle of NWO at the beginning of the second 5C cycle shown in d. (Panel f) Cell voltage for the first 50s of the second 5C cycle. Differential linecut along a NWO particle during this same time period. (Panel g) Simulated change in Li-content along a NWO particle, during the first 30 s of lithiation from a starting composition of x=0.08. (Panel h) Simulated change in Li-content along a NWO particle, during the first 30 s of lithiation from a starting composition of x=0.14. (Panel i) Experimentally-determined and simulated lithiation front velocities at 1C, 5C and 20C.
Figure 4: (Panels a,d,I,j) Unprocessed optical images of a NWO particle at various stages between cycles. (Panels b,c,g) Cell voltage during delithiation at C/2, 5C or 20C. Differential linecut along the NWO particle during the same time periods. (Panels e,f,h) Differential optical images showing the particle of NWO at the time-points indicated in panels c and g.
Figure 5: (Panels a,b,c) Statistical data obtained from optical images of a consistent set of particles, between ‘cracking cycles’. See explanatory document. (Panel d) Unprocessed optical images of NWO particles after 20 cycles.

本数据集收录了主文本中所示图例所包含的全部数据（该文稿题目为《高倍率锂离子正极单粒子动力学状态电荷异质性和裂解的实时监测》）。数据采集及处理的相关信息详尽地记载于开放获取的文稿及补充信息中。此外，该数据集还包含了用于同一文稿中相位场建模的 MATLAB 编程代码。

图1：（子图b）NWO 在1C、5C 和 20C 下进行五次循环的恒电流充放电数据（电压与比容量关系）。（子图c）NWO 中的锂离子自扩散系数，作为温度和锂浓度的函数。

图2：（子图a）NWO 粒子的扫描电子显微镜（SEM）图像。（子图c）在5C 恒电流循环期间未经处理的 NWO 粒子的光学图像。（子图d）在1C、5C 和 20C 恒电流循环期间，单粒子散射强度和单粒子长度变化与电池电压的关系。（子图e）通过原位和离位 XRD 测量的 NWO 的 c 晶格参数变化，作为锂含量的函数。多个单个 NWO 粒子的光学确定的长度变化。

图3：（子图a&d）在5C 下进行两次恒电流循环的电池电压和施加电流，初始时电压保持在 2.8V。 （子图b）显示在 a 中第一个 5C 循环开始的 NWO 粒子的微分光学图像。（子图c）第一个 5C 循环前 50 秒的电池电压。在同一时间段内沿 NWO 粒子进行的微分线切割。（子图e）显示在 d 中第二个 5C 循环开始的 NWO 粒子的微分光学图像。（子图f）第二个 5C 循环前 50 秒的电池电压。在同一时间段内沿 NWO 粒子进行的微分线切割。（子图g）从起始组成 x=0.08 开始的锂化过程中，NWO 粒子沿线的锂含量模拟变化。（子图h）从起始组成 x=0.14 开始的锂化过程中，NWO 粒子沿线的锂含量模拟变化。（子图i）在 1C、5C 和 20C 下通过实验确定和模拟的锂化前沿速度。

图4：（子图a,d,I,j）在循环之间各个阶段未经处理的 NWO 粒子的光学图像。（子图b,c,g）在 C/2、5C 或 20C 解锂过程中的电池电压。在同一时间段内沿 NWO 粒子进行的微分线切割。（子图e,f,h）在 c 和 g 中所示时间点，显示 NWO 粒子的微分光学图像。

图5：（子图a,b,c）从一致粒子的光学图像中获得的统计数据，在‘裂解循环’之间。详见说明文档。（子图d）经过 20 次循环后的 NWO 粒子的未经处理的光学图像。