4.7 Article

Recovery and Reuse of Anode Graphite from Spent Lithium-Ion Batteries via Citric Acid Leaching

Journal

ACS APPLIED ENERGY MATERIALS
Volume 4, Issue 6, Pages 6261-6268

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsaem.1c01029

Keywords

spent lithium-ion batteries; anode graphite; citric acid; leaching; recovery

Funding

  1. National Natural Science Foundation of China [51972030]
  2. S&T Major Project of Inner Mongolia Autonomous Region in China [2020ZD0018]
  3. Beijing Outstanding Young Sc ientists Program [BJJWZYJH01201910007023]
  4. Guangdong Key Laboratory of Battery Safety [2019B121203008]

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This research focused on the recovery and regeneration of anode graphite from retired lithium-ion batteries. By using environmentally friendly citric acid as the extraction reagent, lithium was successfully extracted from spent graphite with a leaching rate of 97.58%. The regenerated graphite anode material showed excellent electrochemical performance, maintaining high discharge capacity and Coulombic efficiency after 80 cycles.
With the rapid growth of retired lithium-ion batteries (LIBs), the recycling of electrode materials has become a hot topic in research. Considering the economic factors, the recovery of cathode electrodes has always been the focus of research. Until now, the recovery of anode electrode materials has gained much attention due to their large proportion in batteries. This research focuses on the recovery and regeneration of anode graphite. Based on the existing form of lithium in anode graphite carbon powder, environmentally friendly citric acid is selected as the extraction reagent to extract lithium and regenerate spent graphite. Through orthogonal experiments and conditional experiments, the optimal conditions for extracting the lithium element from the spent LIB anodes were a temperature of 90 degrees C, S/L ratio of 1:50 g mL(-1), CAC of 0.2 mol L-1, and time of 50 min, and the leaching rate of lithium ions can reach 97.58%. The electrochemical performance tests showed that the regenerated graphite anode material after the extraction of lithium had a high discharge capacity of 330 mA h g(-1) after 80 cycles at 0.5 C, and the Coulombic efficiency is maintained above 99%. By comparing the regenerated graphite and the pretreated spent graphite, the regenerated leached graphite has obviously excellent electrochemical performance, and its properties can be comparable to those of artificial graphite. This experimental result provides a theoretical basis for the subsequent recycling of anode electrode graphite.

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