Emerging macromolecular brush-based materials for stabilizing lithium metal anodes

Li-metal anode (LMA) has attracted significant attention as a prospective anode material for next-generation Li-metal batteries (LMBs). However, the development of LMBs is hampered by safety concerns, including the risk of short-circuiting, fire, and explosions. These safety issues derive mostly from undesirable reactions of the LMA during cycling, such as dendrite growth, dead Li formation, and volume changes. In response to these challenges, molecular brushes, characterized by their well-defined architecture and multifunction integration, have emerged as a valuable solution to stabilize LMA. This comprehensive review focuses on the design and application of molecular brushes in the field of LMBs, aiming to unveil their structure–function relationship and their pivotal role in enhancing stability of LMA. Moreover, we provide an overview of recent computational studies that have elucidated the conformation and dynamics of molecular brushes in LMBs. Finally, we discuss existing challenges and present future prospects with the goal of motivating the progress of high-performance LMBs.