High‐Performance Dendrite‐Free Lithium Textile Anodes Using Interfacial Interaction‐Mediated Ultrathin Metal Organic Framework Multilayers

Abstract Lithium (Li) metal batteries are among the most promising candidates for next‐generation high‐energy‐density battery systems. Their wider adoption, however, is hindered by safety and stability issues, primarily due to the uncontrollable growth of Li dendrites. Herein, a high‐performance dendrite‐free Li textile anode is introduced for high capacity and long‐term stability using interfacial interaction‐mediated ultrathin metal‐organic framework (MOF) multilayers. The repeated coordination bonding‐based layer‐by‐layer (LbL) assembly of Ag ions and trithiocyanuric acid (TCA) generates uniform and ultrathin MOF multilayers with a thickness of less than 40 nm on Ni‐electroplated polyester textiles. During electrochemical operations, Ag ions in the MOF are chemically reduced in situ to form highly lithiophilic Ag nanoparticles (NPs) without requiring any additional treatment, which significantly lowers the Li nucleation energy barrier. Additionally, the organic TCA in the MOF structure promotes the formation of a Li 3 N‐rich solid electrolyte interphase layer, thereby enhancing stability over 2000 h (at 1 mA cm −2 ) in a symmetric cell configuration. Furthermore, a full cell with a LiFePO 4 cathode demonstrates remarkable capacity retention of ≈96.5% after 1300 cycles at 1 C. The approach underscores the critical role of interfacial interactions and ultrathin lithiophilic layers in advancing the performance of Li metal batteries.