Electrode delamination technologies for spent lithium-ion batteries: Interfacial mechanisms, methodological advances and multi-dimensional comprehensive evaluation

The rapid growth of new energy vehicles and energy storage has led to a surge in retired lithium-ion batteries, making efficient recycling crucial for resource conservation and environmental risk mitigation. Electrode delamination, a key front-end process, separates active materials from current collectors with high efficiency and low damage, directly affecting downstream metal recovery and material regeneration value. This review systematically investigates interfacial structures and binding mechanisms-mechanical interlocking, physical adsorption, and chemical bonding-and establishes a delamination theoretical framework based on an interfacial toughness model. The principles and limitations of conventional methods including mechanical, thermal decomposition, solvent dissolution, and physical field-assisted delamination are analyzed. Cutting-edge technologies, such as green deep eutectic solvents, high-voltage pulsed delamination, and laser precision delamination, are thoroughly reviewed, and prospective stimuli-responsive smart binder designs are further discussed as forward-looking recycling strategies. A multi-dimensional evaluation system incorporating delamination efficiency, material integrity, purity, and economic and environmental indicators is developed, alongside a full-chain assessment method centering on the electrochemical performance of recovered materials. Key challenges in initial disassembly-residual charge management, irregularly shaped modules, and process compatibility-and engineering hurdles of scaling up, equipment cost, and safety/environmental protection during industrialization are discussed. Future directions emphasize interdisciplinary integration, recycling-oriented design, and low-cost, highly adaptable technologies, highlighting high-voltage pulsed, laser precision delamination, and smart binder systems as promising for high-value direct regeneration. This review offers a systematic reference to advance electrode delamination toward precision, green, low-carbon, and large-scale application.