High-Performance Graphite Recovered from Spent Lithium-Ion Batteries

Abstract

With the wide usage of Li-ion batteries (LIBs) in portable electronics, electric vehicles, and grid storage, recycling and reusing LIBs have attracted wide attention. However, due to the low added value and rigorous separation steps, recycling and recovering graphite anode materials are discarded. Although some direct physical recycling processes have been reported, all of them are limited by rigorous separation steps and lab scales. In this paper, a scalable recycling process for graphite anode materials from spent LIBs by a hydrometallurgical process without separation steps is reported. After the leaching process, graphite was separated by filtration as a residue with impurities. Then, all residual cathode materials, other metal impurities, most binding materials, and aluminum oxide were removed after releaching and fusion steps. Finally, high-quality graphite powder was obtained, and the recycled graphite exhibits a comparable discharge capacity of 377.3 mAh/g at 0.1 C.

Current and future lithium-ion battery manufacturing

“… Recycling becomes an inevitable topic with the surging of LIB manufacturing capacity. Battery recycling technology has been widely studied in recent years, which mainly focuses on material recovery ( Chen et al., 2019 ; Ma et al., 2019 ). The manufacturing processes could play a big role in recycling and need to be studied.…”

A review of physical processes used in the safe recycling of lithium ion batteries

“…For example, pyrometallurgical recycling is only economical for batteries with a high cobalt or nickel content, due to the energy requirements of the process and the value of cobalt and copper [4], whereas cells with a manganese or iron rich content make this process economically unviable. Whilst few studies have been published which include cycling data for recycled graphite [13,23,24], all include some form of treatment in order to remove electrolyte, SEI, or binder, and thus improve performance. Moradi and Botte [25] emphasised the need to match the 99.9 % purity of new battery grade graphite in a recycled graphite product.…”

An Urgent Call to Spent LIB Recycling: Whys and Wherefores for Graphite Recovery

“…Rothermel et al [ 37 ] have investigated the suitability of spent LIBs graphite as an anode for the LIBs before and after electrolyte extraction. Also, the hydrometallurgical method without separation steps has been reported by Wang and his co‐workers [ 38 ] elucidate the recovered graphite could be reached a comparable capacity of 377 mAh g –1 at 0.1 C. Wang et al [ 39 ] reclaimed the graphite with simple water treatment regains 345 mAh g −1 after 100 cycles where residual Li present in the graphite layers react with water separated the SEI layer by producing H 2 gas. Recently, Subramanyan et al [ 40 ] reported the possibility of using the mechanically separated graphitic anode toward the fabrication of ≈1.4 V class Li‐ion cells with LiCrTiO 4 cathode by utilizing the Ti 4+/3+ couple.…”