Wang Gang, Chandrasekhar Naisa, Biswal Bishnu P, Becker Daniel, Paasch Silvia, Brunner Eike, Addicoat Matthew, Yu Minghao, Berger Reinhard, Feng Xinliang
Center for Advancing Electronics Dresden (cfaed) and Department of Chemistry and Food Chemistry, Technische Universität Dresden, 01062, Dresden, Germany.
Chair of Bioanalytical Chemistry, Technische Universität Dresden, 01062, Dresden, Germany.
Adv Mater. 2019 Jul;31(28):e1901478. doi: 10.1002/adma.201901478. Epub 2019 May 17.
Organic electrode materials are of long-standing interest for next-generation sustainable lithium-ion batteries (LIBs). As a promising cathode candidate, imide compounds have attracted extensive attention due to their low cost, high theoretical capacity, high working voltage, and fast redox reaction. However, the redox active site utilization of imide electrodes remains challenging for them to fulfill their potential applications. Herein, the synthesis of a highly stable, crystalline 2D polyarylimide (2D-PAI) integrated with carbon nanotube (CNT) is demonstrated for the use as cathode material in LIBs. The synthesized polyarylimide hybrid (2D-PAI@CNT) is featured with abundant π-conjugated redox-active naphthalene diimide units, a robust cyclic imide linkage, high surface area, and well-defined accessible pores, which render the efficient utilization of redox active sites (82.9%), excellent structural stability, and fast ion diffusion. As a consequence, high rate capability and ultrastable cycle stability (100% capacity retention after 8000 cycles) are achieved in the 2D-PAI@CNT cathode, which far exceeds the state-of-the-art polyimide electrodes. This work may inspire the development of novel organic electrodes for sustainable and durable rechargeable batteries.
有机电极材料长期以来一直是下一代可持续锂离子电池（LIBs）的研究热点。作为一种有前景的正极候选材料，酰亚胺化合物因其低成本、高理论容量、高工作电压和快速氧化还原反应而受到广泛关注。然而，酰亚胺电极的氧化还原活性位点利用率仍然具有挑战性，难以实现其潜在应用。在此，展示了一种与碳纳米管（CNT）集成的高度稳定的结晶二维聚芳酰亚胺（2D-PAI）的合成，用作LIBs的正极材料。合成的聚芳酰亚胺杂化物（2D-PAI@CNT）具有丰富的π共轭氧化还原活性萘二酰亚胺单元、强大的环状酰亚胺键、高比表面积和明确的可及孔隙，这使得氧化还原活性位点能够有效利用（82.9%），具有出色的结构稳定性和快速的离子扩散。因此，2D-PAI@CNT正极实现了高倍率性能和超稳定的循环稳定性（8000次循环后容量保持率为100%），远远超过了目前最先进的聚酰亚胺电极。这项工作可能会激发用于可持续和耐用可充电电池的新型有机电极的开发。
