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Assessing Long-Term Cycling Stability of Single-Crystal Versus Polycrystalline Nickel-Rich NCM in Pouch Cells with 6 mAh cm−2 Electrodes
Small ( IF 13.0 ) Pub Date : 2022-02-18 , DOI: 10.1002/smll.202107357 Wengao Zhao 1 , Lianfeng Zou 2 , Leiting Zhang 3 , Xinming Fan 4, 5 , Hehe Zhang 6 , Francesco Pagani 1 , Enzo Brack 1 , Lukas Seidl 1 , Xing Ou 4 , Konstantin Egorov 1 , Xueyi Guo 4 , Guorong Hu 4 , Sigita Trabesinger 3 , Chongmin Wang 2 , Corsin Battaglia 1
Small ( IF 13.0 ) Pub Date : 2022-02-18 , DOI: 10.1002/smll.202107357 Wengao Zhao 1 , Lianfeng Zou 2 , Leiting Zhang 3 , Xinming Fan 4, 5 , Hehe Zhang 6 , Francesco Pagani 1 , Enzo Brack 1 , Lukas Seidl 1 , Xing Ou 4 , Konstantin Egorov 1 , Xueyi Guo 4 , Guorong Hu 4 , Sigita Trabesinger 3 , Chongmin Wang 2 , Corsin Battaglia 1
Affiliation
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Lithium-ion batteries based on single-crystal LiNi1−x−yCoxMnyO2 (NCM, 1−x−y ≥ 0.6) cathode materials are gaining increasing attention due to their improved structural stability resulting in superior cycle life compared to batteries based on polycrystalline NCM. However, an in-depth understanding of the less pronounced degradation mechanism of single-crystal NCM is still lacking. Here, a detailed postmortem study is presented, comparing pouch cells with single-crystal versus polycrystalline LiNi0.60Co0.20Mn0.20O2 (NCM622) cathodes after 1375 dis-/charge cycles against graphite anodes. The thickness of the cation-disordered layer forming in the near-surface region of the cathode particles does not differ significantly between single-crystal and polycrystalline particles, while cracking is pronounced for polycrystalline particles, but practically absent for single-crystal particles. Transition metal dissolution as quantified by time-of-flight mass spectrometry on the surface of the cycled graphite anode is much reduced for single-crystal NCM622. Similarly, CO2 gas evolution during the first two cycles as quantified by electrochemical mass spectrometry is much reduced for single-crystal NCM622. Benefitting from these advantages, graphite/single-crystal NMC622 pouch cells are demonstrated with a cathode areal capacity of 6 mAh cm−2 with an excellent capacity retention of 83% after 3000 cycles to 4.2 V, emphasizing the potential of single-crystalline NCM622 as cathode material for next-generation lithium-ion batteries.
中文翻译：
评估具有 6 mAh cm-2 电极的软包电池中单晶与多晶富镍 NCM 的长期循环稳定性
基于单晶 LiNi 1− x - y Co x Mn y O 2 (NCM, 1− x - y ≥ 0.6) 正极材料的锂离子电池由于其改进的结构稳定性而获得了越来越多的关注，从而与相比具有更长的循环寿命到基于多晶NCM的电池。然而，仍然缺乏对单晶 NCM 不太明显的降解机制的深入了解。在这里，进行了详细的验尸研究，比较了单晶与多晶 LiNi 0.60 Co 0.20 Mn 0.20 O 2的软包电池(NCM622) 阴极在 1375 次放电/充电循环后对石墨阳极。在阴极颗粒的近表面区域形成的阳离子无序层的厚度在单晶和多晶颗粒之间没有显着差异，而多晶颗粒的破裂很明显，但单晶颗粒几乎没有破裂。对于单晶 NCM622，通过飞行时间质谱在循环石墨阳极表面上量化的过渡金属溶解大大减少。同样，CO 2对于单晶 NCM622，通过电化学质谱法量化的前两个循环中的气体释放量大大减少。得益于这些优势，石墨/单晶 NMC622 软包电池的阴极面积容量为 6 mAh cm -2，在 3000 次循环至 4.2 V 后具有 83% 的出色容量保持率，强调了单晶 NCM622 的潜力：下一代锂离子电池的正极材料。
更新日期：2022-02-18
中文翻译：
评估具有 6 mAh cm-2 电极的软包电池中单晶与多晶富镍 NCM 的长期循环稳定性
基于单晶 LiNi 1− x - y Co x Mn y O 2 (NCM, 1− x - y ≥ 0.6) 正极材料的锂离子电池由于其改进的结构稳定性而获得了越来越多的关注，从而与相比具有更长的循环寿命到基于多晶NCM的电池。然而，仍然缺乏对单晶 NCM 不太明显的降解机制的深入了解。在这里，进行了详细的验尸研究，比较了单晶与多晶 LiNi 0.60 Co 0.20 Mn 0.20 O 2的软包电池(NCM622) 阴极在 1375 次放电/充电循环后对石墨阳极。在阴极颗粒的近表面区域形成的阳离子无序层的厚度在单晶和多晶颗粒之间没有显着差异，而多晶颗粒的破裂很明显，但单晶颗粒几乎没有破裂。对于单晶 NCM622，通过飞行时间质谱在循环石墨阳极表面上量化的过渡金属溶解大大减少。同样，CO 2对于单晶 NCM622，通过电化学质谱法量化的前两个循环中的气体释放量大大减少。得益于这些优势，石墨/单晶 NMC622 软包电池的阴极面积容量为 6 mAh cm -2，在 3000 次循环至 4.2 V 后具有 83% 的出色容量保持率，强调了单晶 NCM622 的潜力：下一代锂离子电池的正极材料。
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