Key Laboratory of Applied Surface and Colloid Chemistry (Ministry of Education), School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi'an 710119, PR China.
Key Laboratory of Applied Surface and Colloid Chemistry (Ministry of Education), School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi'an 710119, PR China.
J Colloid Interface Sci. 2023 Aug;643:541-550. doi: 10.1016/j.jcis.2023.03.106. Epub 2023 Mar 21.
The integration of multiple electron-accepting skeletons into polymeric structures is the forefront of materials research for high-energy sustainable energy storage. Herein, we report the synthesis of two novel non-conjugated polymers (NCP1 and NCP2) and a model small molecule (M1) incorporated with bio-derived 4-elecron-uptaking carbonylpyridinium redox-units for alkali-ion batteries. Compared to model small molecules, the polymers exhibited improved battery performance when applied as anode materials for Li-, Na-, and K-ion batteries (LIBs/SIBs/KIBs) owing to their high electrochemical activity and effective ability to suppress dissolution. By judicious selection of the benzothiadiazole redox-active linker, the performance of NCP2 was further enhanced, delivering the highest capacity and the best cycling stability; at mass loadings of up to 3.5 and 4.7 mg cm, the specific capacity remained at 215 and 150 mAh g after 200 cycles, respectively. The Li/Na/K insertion/extraction mechanisms of NCP2 were elucidated based on experimental analyses. The insertion/extraction of Li was much faster than that of Na and K. This study broadens the family of bio-derived carbonylpyridinium-based polymer materials for next-generation electrochemical energy storage applications.
将多个电子受体骨架整合到聚合物结构中是高能可持续储能材料研究的前沿。本文报道了两种新型非共轭聚合物（NCP1 和 NCP2）和一个模型小分子（M1）的合成，它们都含有生物衍生的 4 电子摄取羰基吡啶鎓氧化还原单元，用于碱离子电池。与模型小分子相比，聚合物作为锂离子电池（LIBs）/钠离子电池（SIBs）/钾离子电池（KIBs）的阳极材料，由于其高电化学活性和有效抑制溶解的能力，表现出了改进的电池性能。通过合理选择苯并噻二唑氧化还原活性连接体，进一步提高了 NCP2 的性能，提供了最高的容量和最佳的循环稳定性；在质量负载高达 3.5 和 4.7 mg cm 时，其比容量在 200 次循环后分别保持在 215 和 150 mAh g。基于实验分析，阐明了 NCP2 的 Li/Na/K 插入/提取机制。Li 的插入/提取速度远快于 Na 和 K。本研究拓宽了生物衍生羰基吡啶鎓基聚合物材料的家族，以用于下一代电化学储能应用。
