Multiscale dynamics of charging and plating in graphite electrodes coupling operando microscopy and phase-field modelling.
Multiscale dynamics of charging and plating in graphite electrodes coupling operando microscopy and phase-field modelling.
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DOI：
10.1038/s41467-023-40574-6
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发表时间：
2023-08-24
影响因子：
16.6
通讯作者：
Shearing, Paul R.
中科院分区：
文献类型：
--
作者：
Lu, Xuekun;Lagnoni, Marco;Bertei, Antonio;Das, Supratim;Owen, Rhodri E.;Li, Qi;O'Regan, Kieran;Wade, Aaron;Finegan, Donal P.;Kendrick, Emma;Bazant, Martin Z.;Brett, Dan J. L.;Shearing, Paul R.
石墨阳极中的相分离动力学显著影响锂电镀倾向，这是损害汽车锂离子电池的安全性和快速充电能力的主要降解机制。在这项研究中，我们提出了全面的调查采用operando高分辨率光学显微镜结合非平衡态热力学实施的多维（1D+1D到3D）相场建模框架，以揭示石墨电极中的相分离和电镀的速率相关的空间动力学。在这里，我们可视化，并提供多阶段相分离，电镀，颗粒间/内锂交换和镀锂回插现象的机理理解。观察到颗粒内锂化异质性对颗粒尺寸、形状、取向、表面条件和颗粒水平的C-速率的强烈依赖性，这导致通过基于3D图像的相场模型空间分辨的电镀的早期发生。此外，我们强调在不同的充电状态（SOC）的不同的弛豫过程，其中，在中间SOC，石墨不稳定的石墨颗粒经历剧烈的颗粒内锂再分布和颗粒间锂交换，而电极平衡慢得多，在低和高SOC。这些基于物理学的对不同SOC依赖性弛豫效率的见解为开发先进的快速充电协议以抑制电镀和缩短恒定电压状态提供了新的视角。需要更好地理解石墨电极中的空间动力学，以改进锂离子电池的快速充电协议。在这里，作者强调，锂化异质性导致早期锂电镀开始，并发现不同的电荷状态下的不同弛豫行为。
The phase separation dynamics in graphitic anodes significantly affects lithium plating propensity, which is the major degradation mechanism that impairs the safety and fast charge capabilities of automotive lithium-ion batteries. In this study, we present comprehensive investigation employing operando high-resolution optical microscopy combined with non-equilibrium thermodynamics implemented in a multi-dimensional (1D+1D to 3D) phase-field modeling framework to reveal the rate-dependent spatial dynamics of phase separation and plating in graphite electrodes. Here we visualize and provide mechanistic understanding of the multistage phase separation, plating, inter/intra-particle lithium exchange and plated lithium back-intercalation phenomena. A strong dependence of intra-particle lithiation heterogeneity on the particle size, shape, orientation, surface condition and C-rate at the particle level is observed, which leads to early onset of plating spatially resolved by a 3D image-based phase-field model. Moreover, we highlight the distinct relaxation processes at different state-of-charges (SOCs), wherein thermodynamically unstable graphite particles undergo a drastic intra-particle lithium redistribution and inter-particle lithium exchange at intermediate SOCs, whereas the electrode equilibrates much slower at low and high SOCs. These physics-based insights into the distinct SOC-dependent relaxation efficiency provide new perspective towards developing advanced fast charge protocols to suppress plating and shorten the constant voltage regime. Improved understanding of the spatial dynamics in graphite electrodes is needed to improve fast-charging protocols for Li-ion batteries. Here, authors highlight that lithiation heterogeneity leads to early lithium plating onset and find distinct relaxation behaviors at various states of charge.
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影响因子：
16.6
作者：
Cai, Wenlong;Yan, Chong;Zhang, Qiang
通讯作者：
Zhang, Qiang
影响因子：
27.8
作者：
Ebner, Martin;Chung, Ding-Wen;Wood, Vanessa
通讯作者：
Wood, Vanessa
影响因子：
6.6
作者：
Amietszajew, Tazdin;McTurk, Euan;Bhagat, Rohit
通讯作者：
Bhagat, Rohit
影响因子：
3.7
作者：
Chandesris, Marion;Caliste, Damien;Pochet, Pascal
通讯作者：
Pochet, Pascal
DOI：
10.1007/978-1-4419-9669-5_5
发表时间：
2011-01-01
期刊：
THEORY AND PRACTICE OF METAL ELECTRODEPOSITION
影响因子：
--
作者：
Gamburg, Yuliy D.;Zangari, Giovanni
通讯作者：
Zangari, Giovanni