Graphite Recycling from Spent Lithium‐Ion Batteries

Abstract

The present work reports on challenges in utilization of spent lithium-ion batteries (LIBs)-an increasingly important aspect associated with a significantly rising demand for electric vehicles (EVs). In this context, the feasibility of anode recycling in combination with three different electrolyte extraction concepts is investigated. The first method is based on a thermal treatment of graphite without electrolyte recovery. The second method additionally utilizes a subcritical carbon-dioxide (subcritical CO )-assisted electrolyte extraction prior to thermal treatment. And the final investigated approach uses supercritical carbon dioxide (scCO ) as extractant, subsequently followed by the thermal treatment. It is demonstrated that the best performance of recycled graphite anodes can be achieved when electrolyte extraction is performed using subcritical CO . Comparative studies reveal that, in the best case, the electrochemical performance of recycled graphite exceeds the benchmark consisting of a newly synthesized graphite anode. As essential efforts towards electrolyte extraction and cathode recycling have been made in the past, the electrochemical behavior of recycled graphite, demonstrating the best performance, is investigated in combination with a recycled LiNi Co Mn O cathode.

Simple and Eco‐Friendly Fabrication of Electrode Materials and Their Performance in High‐Voltage Lithium‐Ion Batteries

“…As expected, Li was the element with the highest content, involved in the charging and discharging processes of the battery and present in the electrolyte, together with P, also found in a high content; F was beyond the detection ability of the equipment used. The values of both elements were much higher than those measured by Rothermel et al . in aged graphite (70 % SOH), 450 and 786 ppb, for Li and P, respectively.…”

“…To date, only a few studies have focused on spent LIB anodes as starting material to prepare battery‐grade graphite . Four of them describe the performance of regenerated graphite as LIB negative electrode in half‐cell configuration and only one in full‐cell configuration, using LiNi 1/3 Co 1/3 Mn 1/3 O 2 as cathode material . The investigations of Rothermel et al .…”

“…In addition, this approach paves the way for promoting urban mining and waste valorization, and it is particularly convenient for countries with scarce or no natural graphite resources . To date, only a few studies have focused on spent LIB anodes as starting material to prepare battery‐grade graphite . Four of them describe the performance of regenerated graphite as LIB negative electrode in half‐cell configuration and only one in full‐cell configuration, using LiNi 1/3 Co 1/3 Mn 1/3 O 2 as cathode material .…”

“…Four of them describe the performance of regenerated graphite as LIB negative electrode in half‐cell configuration and only one in full‐cell configuration, using LiNi 1/3 Co 1/3 Mn 1/3 O 2 as cathode material . The investigations of Rothermel et al . are of special interest because they involved an extensive study on recycled graphite from both a structural and an electrochemical point‐of‐view.…”

Burgeoning Prospects of Spent Lithium‐Ion Batteries in Multifarious Applications

“…Recovered graphite has been used as a raw material to construct high capacity anode material with two different approaches. [117,118] In the very rare study of electrolyte recycling, Rothermel et al [79] extracted the electrolyte from recovered graphite using subcritical carbon dioxide and investigated the feasibility analysis of graphite as a LIB material via electrochemical studies. Further, the alcohol/water suspension of graphite is passed into a spray-drier to develop reconstructed graphite.…”