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<p>The rapidly growing volume of spent lithium-ion batteries (LIBs) poses an urgent recycling challenge, as conventional pyro-/hydro-metallurgical methods remain inefficient and require harsh operating conditions. Herein, we develop an efficient, pilot-scale radiation-driven leaching strategy for processing kilogram quantities of spent ternary cathode material dispersed in aqueous citric acid. In minutes, ambient and controllable electron beam irradiation achieves near-complete (&gt;99%) leaching of valuable transition metals and lithium. Mechanistic studies reveal that the hydrated electrons and citric acid-derived radicals generated jointly during water radiolysis drive rapid cathode amorphization by reducing high-valence metal centers and cleaving metal-oxygen bonds. Concurrently, direct irradiation induces lattice defects and oxygen vacancies, synergistically enhancing amorphization and strengthening radical-metal site coupling, thereby accelerating dissolution. Furthermore, the leachate is repurposed into effective cathode materials and oxygen evolution reaction catalysts, enabling an economically viable closed-loop recycling process. Energy efficiency and techno-economic analyses indicate that industrial-scale radiation technology offers a practical solution for scalable spent LIB recycling.</p>

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Effective recycling of spent lithium-ion batteries via radiolytic radical reactions

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2026年5月7日

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  • Hanzhi Yu,
  • Changjiang Hu,
  • Zhiwen Jiang,
  • Hang Zhang,
  • Chunyang Ma,
  • Jun Ma

摘要

The rapidly growing volume of spent lithium-ion batteries (LIBs) poses an urgent recycling challenge, as conventional pyro-/hydro-metallurgical methods remain inefficient and require harsh operating conditions. Herein, we develop an efficient, pilot-scale radiation-driven leaching strategy for processing kilogram quantities of spent ternary cathode material dispersed in aqueous citric acid. In minutes, ambient and controllable electron beam irradiation achieves near-complete (>99%) leaching of valuable transition metals and lithium. Mechanistic studies reveal that the hydrated electrons and citric acid-derived radicals generated jointly during water radiolysis drive rapid cathode amorphization by reducing high-valence metal centers and cleaving metal-oxygen bonds. Concurrently, direct irradiation induces lattice defects and oxygen vacancies, synergistically enhancing amorphization and strengthening radical-metal site coupling, thereby accelerating dissolution. Furthermore, the leachate is repurposed into effective cathode materials and oxygen evolution reaction catalysts, enabling an economically viable closed-loop recycling process. Energy efficiency and techno-economic analyses indicate that industrial-scale radiation technology offers a practical solution for scalable spent LIB recycling.