Polymer binders for the cathodes of lithium-ion batteries play a pivotal role in enhancing the battery energy density, cycle life and interfacial stability. Conventional polyvinylidene fluoride (PVDF) binders have difficulty meeting the multiple requirements of high specific energy electrodes due to their inherent drawbacks including electrical insulation, mechanical rigidity and interfacial inertness. In recent years, function-oriented binders have emerged as a research hotspot, which are endowed with properties such as electrical conductivity, mechanical adaptability, self-healing capability and high voltage tolerance via rational molecular structure design. This review systematically reviews the molecular design strategies of polymer-based cathode binders, including the introduction of polar groups (e.g., hydroxyl and carboxyl groups) to strengthen hydrogen bonding and electrostatic interactions, the construction of conjugated polymers or ion-conductive networks to improve electrical conductivity, and the utilization of dynamic chemical bonds to achieve self-healing function. In addition, high voltage-tolerant binders can significantly suppress capacity fading of high-voltage cathodes via chelating transition metal ions, optimizing electrode dispersibility and forming a stable interfacial layer. By integrating molecular dynamics simulations with experimental characterizations, the correlation between the molecular structure of binders and the electrochemical performance of electrodes is elucidated, which provides a theoretical framework for the design of next-generation high-performance binders.



