Crystalline Free-Standing Two-Dimensional Zwitterionic Organic Nanosheets for Efficient Conduction of Lithium Ions

Crystalline two-dimensional organic nanosheets (2D-ONs) having atomic or near-atomic thickness with infinite lateral dimensions are of crucial significance for their possible application as a material for energy storage. The presence of nanofluidic channels with a designed array of molecular interlayers in such 2D-ONs, for a favorable lithium-ion transport, has special significance for improving the efficacy of lithium-ion batteries. However, the rational design of crystalline 2D-ONs remains a challenge because of the lack of appropriate monomers and convenient preparation methods. Herein, we report a unique lithium-ion conducting behavior of zwitterionic 2D-ONs, formed through self-assembly of a small organic molecule AM-1. Different microscopic studies confirm the near-atomic thickness (∼3.5 nm) of these 2D-ONs. Results of the single-crystal X-ray diffraction studies confirm the presence of a one-dimensional (1D) channel in crystalline 2D-ONs, which was generated during the self-assembly process of the zwitterionic monomer scaffold. The presence of immobilized ionic centers with well-defined directional channels in the 2D-ONs favors the transportation of lithium ions with a room-temperature lithium-ion conductivity of 5.14 × 10–5 S cm–1, which is rather unique for self-assembled 2D-ONs.