n-Type Glycolated Imide-Fused Polycyclic Aromatic Hydrocarbons with High Capacity for Liquid/Solid- Electrolyte-based Electrochemical Devices

摘要

Currently, n-type small-molecule mixed ionic-electronic conductors remainless explored and their molecular design rules are not mature enough.Herein, two n-type glycolated imide-fused polycyclic aromatic hydrocarbons(IPAHs), d-gdiPDI and t-gdiPDI, are developed to probe the effects ofmolecular conformation on the electronic, electrochemical, morphological,and coupled ionic-electronic transport properties. It is found that the highlytwisted scaffold in d-gdiPDI, compared to the nearly planar one of t-gdiPDI,has a strong positive effect on the charge storage properties and thus the performanceof organic electrochemical transistors (OECTs). d-gdiPDI exhibitsa volumetric capacitance of 657 F cm~(?3), obviously outperforming that oft-gdiPDI (261 F cm~(?3)), which is the highest value reported to date for smallmoleculeOECT materials. Moreover, a high charge-storage capacity of upto 479 F g~(?1) is observed for d-gdiPDI. Arising from such high ionic-electroniccoupling characteristic, d-gdiPDI-based OECTs present a ≈2 × times highergeometry-normalized transconductance (g_(m,norm)) of 105.3 mS cm~(?1) relativeto that of t-gdiPDI counterparts. Significantly, further application of d-gdiPDIin solid-electrolyte OECTs delivers a g_(m,norm) of 142.4 mS cm~(?1). These findingsindicate that IPAHs are very promising candidates for n-type small-moleculeOECTs and highlight the superiority of twisting conformation manipulation inmaterials design toward high-performance electrochemical devices.