<p>This study explores a practical and sustainable approach to processing spent cylindrical lithium-ion batteries (LIBs) with NCA-based cathodes (Li(Ni<sub>x</sub>Co<sub>y</sub>Al<sub>z</sub>)O<sub>2</sub>) through direct pyrolysis and water leaching. The process begins with a safe and effective discharge of the spent LIBs using natural seawater, followed by pyrolysis in an inert argon atmosphere at holding temperatures ranging from 500&#xa0;°C to 900&#xa0;°C. After pyrolysis, the LIBs were dismantled, and the resulting black mass was subjected to water leaching to assess its lithium solubility. Analysis of the pyrolyzed black mass contained varying proportions of unreduced Li(Ni<sub>x</sub>Co<sub>y</sub>Al<sub>z</sub>)O<sub>2</sub>, Li<sub>2</sub>CO<sub>3</sub>, LiAlO<sub>2</sub>, NiO, metallic Ni–Co, and graphite, depending on the pyrolysis temperature. The optimal pyrolysis condition at a peak temperature of 600&#xa0;°C for 120 min yielded the highest lithium extraction of 63.6%. The direct pyrolysis route eliminates the need for physical pre-treatment and thus simplifying the overall process. While further lithium recovery may require additional pH-adjusted leaching step, the water leaching process minimizes hazardous chemical use and reduces corrosive waste, making the method more environmentally sustainable.</p> Graphical Abstract <p></p>

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Toward Practical and Sustainable Processing of Spent Cylindrical NCA Lithium-Ion Battery: Effects of Pyrolysis on Cathode Phase Evolution and Lithium Recovery via Water Leaching

  • Taufiq Hidayat,
  • Angelina Timothy,
  • Teresia Santoso,
  • Nadira Aby Xavier,
  • Delvin S. M. Fadhlurrahman,
  • Zela Tanlega,
  • Zulfiadi Zulhan,
  • Meditya Wasesa,
  • Fajar Nurjaman,
  • Erik Prasetyo

摘要

This study explores a practical and sustainable approach to processing spent cylindrical lithium-ion batteries (LIBs) with NCA-based cathodes (Li(NixCoyAlz)O2) through direct pyrolysis and water leaching. The process begins with a safe and effective discharge of the spent LIBs using natural seawater, followed by pyrolysis in an inert argon atmosphere at holding temperatures ranging from 500 °C to 900 °C. After pyrolysis, the LIBs were dismantled, and the resulting black mass was subjected to water leaching to assess its lithium solubility. Analysis of the pyrolyzed black mass contained varying proportions of unreduced Li(NixCoyAlz)O2, Li2CO3, LiAlO2, NiO, metallic Ni–Co, and graphite, depending on the pyrolysis temperature. The optimal pyrolysis condition at a peak temperature of 600 °C for 120 min yielded the highest lithium extraction of 63.6%. The direct pyrolysis route eliminates the need for physical pre-treatment and thus simplifying the overall process. While further lithium recovery may require additional pH-adjusted leaching step, the water leaching process minimizes hazardous chemical use and reduces corrosive waste, making the method more environmentally sustainable.

Graphical Abstract