Regenerated Ni-Rich Cathode Materials from Spent Li-Ion Batteries by a Closed Loop Process

The demand for rechargeable lithium-ion batteries (LIBs) has increased exponentially since they were first commercialized by Sony in 1991. [1] Due to the high energy density and excellent cycle stability, LIBs have been widespread utilized in electric vehicles and other applications. However, the lifespan of LIBs is limited. Thus, tons of spent LIBs are generated during the recent decades. More importantly, the price of raw materials, including lithium and cobalt salts, for producing LIBs grows significantly. [2, 3] Therefore, recycling these End-of-Life LIBs becomes a non-negligible part in the whole manufacturing process and hydrometallurgical process is the most common recycling method. Here, our group has demonstrated a closed loop recycling process, combining inorganic acid etching and coprecipitation reaction, to produce regenerated Ni-rich cathode materials. The regenerated LiNi 0.83 Mn 0.06 Co 0.11 O 2 shows excellent performance: the first cycle discharge capacity is 214.1mAh/g at 0.05C in the voltage range of 2.8 - 4.3V and the initial columbic efficiency is 90.9%. The performance of our regenerated cathode materials is comparable to commercial cathode materials. In order to further optimize the properties of the regenerated LiNi 0.83 Mn 0.06 Co 0.11 O 2 , different elements, like Al, with various doping or coating methods will be utilized. Manthiram A. A reflection on lithium-ion battery cathode chemistry . Nature Communications 2020; 11(1):1550. Li W, Lee S, Manthiram A. High‐Nickel NMA: A Cobalt‐Free Alternative to NMC and NCA Cathodes for Lithium‐Ion Batteries . Advanced materials (Weinheim) 2020; 32(33):2002718-n/a. Hou J, Ma X, Fu J, Vanaphuti P, Yao Z, Liu Y, et al. A green closed-loop process for selective recycling of lithium from spent lithium-ion batteries . Green Chemistry 2022; 24(18):7049-7060.