Isomer Effect on Energy Storage of π‐Extended S‐Shaped Double[6]Heterohelicene

Abstract Recently, chiral and nonplanar cutouts of graphene have been the favorites due to their unique optical, electronic, and redox properties and high solubility compared with their planar counterparts. Despite the remarkable progress in helicenes, π‐extended heterohelicenes have not been widely explored. As an anode in a lithium‐ion battery, the racemic mixture of π‐extended double heterohelical nanographene containing thienothiophene core exhibited a high lithium storage capability, attaining a specific capacity of 424 mAh g −1 at 0.1 A g −1 with excellent rate capability and superior long‐term cycling performance over 6000 cycles with negligible fade. As a first report, the π‐extended helicene isomer ( PP and MM ), with the more interlayer distance that helps faster diffusion of ions, has exhibited a high capacity of 300 mAh g −1 at 2 A g −1 with long‐term cycling performance over 1500 cycles compared to the less performing MP and PM isomer and racemic mixture (150 mAh g −1 at 2 A g −1 ). As supported by single‐crystal X‐ray analysis, a unique molecular design of nanographenes with a fixed (helical) molecular geometry, avoiding restacking of the layers, renders better performance as an anode in lithium‐ion batteries. Interestingly, the recycled nanographene anode material displayed comparable performance.