Stable quasi-solid-state lithium-organic battery based on composite gel polymer electrolyte and compatible organic cathode material

High-performance organic small-molecule electrode materials are troubled with their high solubility in liquid electrolytes. The construction of quasi-solid-state lithium organic batteries (LOBs) using gel polymer electrolytes with high mechanical properties, compromised ionic conductivity, high safety, and eco-friendly is an effective way to inhibit the dissolution of active materials. Herein, two hexaazatriphenylene (HATN)-based organic cathode materials (HATNA-6OCH3 and HATNA-6OH) are synthesized and then matched with polyvinylidene fluoride-hexafluoropropylene (PVDF-HFP)-based gel polymer electrolytes to construct quasi-solid-state LOBs. Thanks to the enhanced interfacial compatibility between organic cathode material and gel polymer electrolyte, HATNA-6OH with compatible hydroxyl group shows the enhanced electrochemical properties compared with HATNA-6OCH3. Further, the electrochemical performance is improved when HATNA-6OH is combined with a gel polymer electrolyte modified with a succinonitrile (SN) plasticizer (GPE-0.4SN), including a high specific capacity of 153.3 mAh g-1 at 50 mA g-1 and a good reversible capacity of 88 mAh g-1 after 100 cycles at 200 mA g-1. In addition, the good electrochemical properties and lithium-ion storage mechanism of HATNA-6OH have been elucidated using density functional theory (DFT) and spectral characterizations.