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March 14, 2026Advanced Materials7 citationsOpen Access

From Spent Batteries to Green Hydrogen: Catalytic Upcycling of Lithium‐Ion Battery Cathodes for Water Electrolysis

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MWMin WangChina University of Petroleum, East ChinaLLLiming LeiChengdu University of TechnologyCZCenkai ZhaoChina University of Petroleum, East China

Key Points

  • The aim is to explore the recycling and upcycling of lithium-ion battery cathodes for generating hydrogen through water electrolysis.
  • Reviewed three dominant cathode families: LiCoO2, LiNixCoyMn1-x-yO2, and LiFePO4.
  • Evaluated various pretreatment protocols and recycling strategies including pyrometallurgical and hydrometallurgical methods.
  • Discussed the role of structure-activity correlations in developing high-performance electrocatalysts.
  • Identified key structural features that enhance electrocatalytic performance for hydrogen and oxygen evolution.
  • Proposed a design framework that encompasses multiscale optimization and insights from machine learning for future applications.
  • Highlighted the environmental and strategic importance of upcycling as part of a closed-loop materials ecosystem.

Abstract

The accelerating global "dual-carbon" transition and the rapid proliferation of electric vehicles are driving an unprecedented surge in spent lithium-ion batteries (LIBs), with the first major retirement peak expected around 2030. Cathode materials form a pivotal bridge between urban mining and green-hydrogen technologies, coupling environmental risks with the strategic importance of critical metals. This review delivers a comprehensive overview of the recycling and upcycling landscape for the three dominant cathode families-LiCoO2, LiNixCoyMn1-x-yO2, and LiFePO4. We outline the compositional and structural features of these materials, evaluate pretreatment protocols, and critically compare pyrometallurgical, hydrometallurgical, and direct-regeneration strategies. We then highlight how multiscale structure-activity correlations guide the transformation of regenerated cathodes into high-performance electrocatalysts, with emphasis on defect engineering, electronic-structure modulation, interfacial coupling, and the assembly of conductive networks to accelerate both hydrogen- and oxygen-evolution pathways. Finally, we propose a forward-looking design framework that integrates atomic-site dynamics, multimetallic synergy, and process-environment co-optimization, while underscoring emerging opportunities in machine-learning-guided inverse design, operando mechanistic mapping, and device-level implementation. This review provides a conceptual blueprint for integrating battery recycling with green-hydrogen production in a closed-loop materials ecosystem.

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Cite This Study

Wang et al. (2026) studied this question.

synapsesocial.com/papers/69b4fb9db39f7826a300be3dhttps://doi.org/10.1002/adma.202523322
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