Yu Jie, Chen Lan, Wu Qiong, Wang Junhao, Cheng Linqi, Wang Heng-Guo
Key Laboratory of Functional Materials Physics and Chemistry of the Ministry of Education, Jilin Normal University, Changchun 130103, PR China; Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education and Faculty of Chemistry, Northeast Normal University, Changchun 130024, PR China.
Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education and Faculty of Chemistry, Northeast Normal University, Changchun 130024, PR China.
J Colloid Interface Sci. 2023 Nov;649:159-165. doi: 10.1016/j.jcis.2023.06.052. Epub 2023 Jun 10.
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-6OCH 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-6OCH. 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 at 50 mA g and a good reversible capacity of 88 mAh g after 100 cycles at 200 mA g. 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.
高性能有机小分子电极材料因其在液体电解质中的高溶解度而受到困扰。使用具有高机械性能、适中离子电导率、高安全性和环境友好性的凝胶聚合物电解质构建准固态锂有机电池（LOBs）是抑制活性材料溶解的有效方法。在此，合成了两种基于六氮杂三亚苯（HATN）的有机正极材料（HATNA-6OCH和HATNA-6OH），然后与基于聚偏二氟乙烯-六氟丙烯（PVDF-HFP）的凝胶聚合物电解质匹配，构建准固态LOBs。由于有机正极材料与凝胶聚合物电解质之间的界面相容性增强，具有相容羟基的HATNA-6OH与HATNA-6OCH相比，电化学性能得到增强。此外，当HATNA-6OH与用丁二腈（SN）增塑剂改性的凝胶聚合物电解质（GPE-0.4SN）结合时，电化学性能得到改善，包括在50 mA g下具有153.3 mAh g的高比容量以及在200 mA g下100次循环后具有88 mAh g的良好可逆容量。此外，利用密度泛函理论（DFT）和光谱表征阐明了HATNA-6OH良好的电化学性能和锂离子存储机制。
