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Origin of Structural Evolution in Capacity Degradation for Overcharged NMC622 via Operando Coupled Investigation
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2017-07-17 00:00:00 , DOI: 10.1021/acsami.7b06326 Qi Wang 1 , Chong-Heng Shen 1 , Shou-Yu Shen 1 , Yue-Feng Xu 1 , Chen-Guang Shi 1 , Ling Huang 1 , Jun-Tao Li 2 , Shi-Gang Sun 1, 2
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2017-07-17 00:00:00 , DOI: 10.1021/acsami.7b06326 Qi Wang 1 , Chong-Heng Shen 1 , Shou-Yu Shen 1 , Yue-Feng Xu 1 , Chen-Guang Shi 1 , Ling Huang 1 , Jun-Tao Li 2 , Shi-Gang Sun 1, 2
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The nickel-rich layered oxide materials have been selected as promising cathode materials for the next generation lithium ion batteries because of their large capacity and comparably high operating voltage. However, at high voltage (beyond 4.30 V vs Li/Li+), the members of this family are all suffering from a rapid capacity decay, which was commonly concerned with crystal lattice distortion and related cation disordering. In this work, the quasi-spherical Ni-rich layered LiNi0.6Co0.2Mn0.2O2 (QS-NMC622) material was successfully synthesized through the carbonate co-precipitation method. A coupled measurement, which is a combination of potentiostatic intermittent titration technique (PITT) and in situ X-ray diffraction (XRD), was deployed to simultaneously capture the structural changes and lithium ion diffusion coefficient of QS-NMC622 material during the first cycle. With help of in situ XRD patterns and high-resolution transmission electron microscope (HR-TEM) images, a defective spinel framework of Fd3̅m space group was detected along with a rapid decreasing lattice-parameter c and lattice distortion at deep delithiated state, which causes poor kinetics related to lithium ion mobility. The new-born framework seems to transform and remain as full spinel structure in the parent phase to the end of charge/discharge with high voltage, which could deteriorate both the surface and body structure stability during the subsequent cycles. This established coupled in situ measurement could be applied to simultaneously investigate the structure transformation and kinetics of cathode materials during charge/discharge.
中文翻译：
基于Operando耦合研究的NMC622过充容量退化中结构演化的起源。
富镍层状氧化物材料因其大容量和相当高的工作电压而被选作下一代锂离子电池的有前途的正极材料。然而，在高电压下（超过4.30 V vs Li / Li +），该家族的成员都遭受容量快速衰减的困扰，这通常与晶格畸变和相关的阳离子无序有关。在这项工作中，准球形富镍层状LiNi 0.6 Co 0.2 Mn 0.2 O 2（QS-NMC622）材料是通过碳酸盐共沉淀法成功合成的。耦合测量是恒电位间歇滴定技术（PITT）和原位X射线衍射（XRD）的结合，用于在第一个循环中同时捕获QS-NMC622材料的结构变化和锂离子扩散系数。与原位X射线衍射图案和高分辨率透射电子显微镜（HR-TEM）图像，一个有缺陷的尖晶石框架帮助的Fd 3米的空间群是用快速减小晶格参数沿检测Ç深去锂化状态下的晶格畸变，导致与锂离子迁移率相关的动力学较差。新生的骨架似乎在母相中转变并保持为完整的尖晶石结构，直到高压下的充电/放电结束，这可能会在随后的循环中破坏表面和车身结构的稳定性。这种建立的耦合原位测量可用于同时研究正极材料在充电/放电过程中的结构转变和动力学。
更新日期：2017-07-18
中文翻译：
基于Operando耦合研究的NMC622过充容量退化中结构演化的起源。
富镍层状氧化物材料因其大容量和相当高的工作电压而被选作下一代锂离子电池的有前途的正极材料。然而，在高电压下（超过4.30 V vs Li / Li +），该家族的成员都遭受容量快速衰减的困扰，这通常与晶格畸变和相关的阳离子无序有关。在这项工作中，准球形富镍层状LiNi 0.6 Co 0.2 Mn 0.2 O 2（QS-NMC622）材料是通过碳酸盐共沉淀法成功合成的。耦合测量是恒电位间歇滴定技术（PITT）和原位X射线衍射（XRD）的结合，用于在第一个循环中同时捕获QS-NMC622材料的结构变化和锂离子扩散系数。与原位X射线衍射图案和高分辨率透射电子显微镜（HR-TEM）图像，一个有缺陷的尖晶石框架帮助的Fd 3米的空间群是用快速减小晶格参数沿检测Ç深去锂化状态下的晶格畸变，导致与锂离子迁移率相关的动力学较差。新生的骨架似乎在母相中转变并保持为完整的尖晶石结构，直到高压下的充电/放电结束，这可能会在随后的循环中破坏表面和车身结构的稳定性。这种建立的耦合原位测量可用于同时研究正极材料在充电/放电过程中的结构转变和动力学。
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