Xiao Bo-Hao, Li Jian-Xi, Xu Hong-Yi, Huang Jia-Le, Luo Yin-Lin, Xiao Kang, Liu Zhao-Qing
Department School of Chemistry and Chemical Engineering, Guangzhou University, Guangzhou, 510006, China.
School of Chemistry and Chemical Engineering/Institute of Clean Energy and Materials/Key Laboratory for Clean Energy and Materials, Guangzhou University, Guangzhou, 510006, China.
Angew Chem Int Ed Engl. 2023 Sep 25;62(39):e202309614. doi: 10.1002/anie.202309614. Epub 2023 Aug 24.
Conducting polymers with high theoretical capacitance and deformability are among the optimal candidates for compressible supercapacitor electrode materials. However, achieving both mechanical and electrochemical stabilities in a single electrode remains a great challenge. To address this issue, the "Polymer Chainmail" is proposed with reversible deformation capability and enhances stability because of the steric hindrance and charge compensation effect of doped anions. As a proof of concept, four common anions are selected as dopants for Poly(3,4-ethylenedioxythiophene) (PEDOT), and their effects on the adsorption and diffusion of H on PEDOT are verified using density functional theory calculations. Owing to the film formation effect, the doped PEDOT/nitrogen-doped carbon foam exhibits good mechanical properties. Furthermore, the composite demonstrates excellent rate performance and stability due to suitable anion doping. This finding provides new insights into the preparation of electrochemically stable conductive polymer-based compressible electrode materials.
具有高理论电容和可变形性的导电聚合物是可压缩超级电容器电极材料的最佳候选者之一。然而，在单个电极中同时实现机械稳定性和电化学稳定性仍然是一个巨大的挑战。为了解决这个问题，提出了“聚合物链甲”，它具有可逆变形能力，并且由于掺杂阴离子的空间位阻和电荷补偿效应而增强了稳定性。作为概念验证，选择了四种常见阴离子作为聚（3,4-亚乙基二氧噻吩）（PEDOT）的掺杂剂，并使用密度泛函理论计算验证了它们对H在PEDOT上的吸附和扩散的影响。由于成膜效应，掺杂的PEDOT/氮掺杂碳泡沫表现出良好的机械性能。此外，由于合适的阴离子掺杂，该复合材料表现出优异的倍率性能和稳定性。这一发现为制备电化学稳定的基于导电聚合物的可压缩电极材料提供了新的见解。
