(Digital Presentation) Recycled Cathode Materials Enabled Superior Performance for Lithium-Ion Batteries
Authors: Ma Xiaotu , Wang Yan 
Published: July 2022

With the widely equipped Lithium-ion batteries (LIBs) in electronics and electric vehicles, proper handle spent LIBs has been the subject of increasing concern. Significantly raised concerns about resource constraints and environmental issues are brought by spent LIBs. Therefore, properly handling spent LIBs is urgent and necessary.[1] However, until now, getting manufacturers to recruit recycled materials has been a hard sell because recycled materials are deemed as inferior to commercial materials, which limits the development of recycling. Although previous publications stated that their recovered materials had a comparable performance as commercial materials, the results, based on coin cells and low electrode loading, cannot convince manufacturers to employ recycled materials in the new LIBs.[2] Here, we demonstrate that recycled cathode materials with optimized microstructure have the best industrial relevant testing results (up to 11Ah cells) so far and compare them with state-of-the-art commercial equivalent. Interestingly, the recycled materials not only pass all the aggressive industrial plug-in hybrid electric vehicle (PHEV) battery tests, but also outperform control counterparts in some tests. Specifically, 1 Ah cells with the recycled LiNi1/3Mn1/3Co1/3O2 have the best cycle life result reported for recycled materials and enable 4,200 cycles and 11,600 cycles at 80% and 70% capacity retention, which is 33% and 53% better than the state-of-the-art, commercial LiNi1/3Mn1/3Co1/3O2. Meanwhile, its rate performance is 88.6% better than commercial powders at 5C. Through detailed experimental and modeling analysis of pristine and cycled materials, we discover that the unique porous and larger inside void microstructure enables the superior rate and cycle performance and less phase transformation. Compared with the control sample, the surface area of the recycled LiNi1/3Mn1/3Co1/3O2 is 82.14% larger and the cumulative pore volume is 61.25% larger. Even some recycled particles have an outer diameter of the void space equal to 40% to 60% of the particle diameter. The unique microstructure can reduce 16% hoop stress during the discharge/charge process compared to control materials, and improve the lithium chemical diffusion coefficient, enabling the superior performance of cycle life and rate performance and less phase transformation. The results pave the way to re-introduce recycled materials into new batteries.[3]

[1] M. Chen, X. Ma, B. Chen, R. Arsenault, P. Karlson, N. Simon, Y. Wang, Recycling End-of-Life Electric Vehicle Lithium-Ion Batteries, Joule 2019, 3, 2622.10.1016/j.joule.2019.09.014
[2] X. Ma, L. Azhari, Y. Wang, Li-ion battery recycling challenges, Chem 2021.10.1016/j.chempr.2021.09.013
[3] X. Ma, M. Chen, Z. Zheng, D. Bullen, J. Wang, C. Harrison, E. Gratz, Y. Lin, Z. Yang, Y. Zhang, F. Wang, D. Robertson, S.-B. Son, I. Bloom, J. Wen, M. Ge, X. Xiao, W.-K. Lee, M. Tang, Q. Wang, J. Fu, Y. Zhang, B. C. Sousa, R. Arsenault, P. Karlson, N. Simon, Y. Wang, Recycled cathode materials enabled superior performance for lithium-ion batteries, Joule 2021.10.1016/j.joule.2021.09.005