Yuan Min, Luo Feng, Wang Zeping, Li Hui, Rao Yifan, Yu Jiabing, Wang Ying, Xie Dingli, Chen Xianping, Wong Ching-Ping
Key Laboratory of Optoelectronic Technology & Systems, Education Ministry of China, Chongqing University and College of Optoelectronic Engineering, Chongqing University, Chongqing 400044, China.
State Key Laboratory of Power Transmission Equipment & System Security and New Technology and School of Electrical Engineering, Chongqing University, Chongqing 400044, China.
ACS Appl Mater Interfaces. 2021 May 19;13(19):22426-22437. doi: 10.1021/acsami.1c03219. Epub 2021 May 6.
This study proposes an efficient, facile, and scalable strategy to synthesize heteroatom-doped porous graphene via laser direct writing on the precursor-doped polyimide (PI) film, which is fabricated for the first time through incorporating PI powder and precursors with sodium carboxymethyl cellulose (CMC) binder by a drop-casting and low-temperature drying process. The resulting microsupercapacitors (MSCs) based on the as-prepared heteroatom-doped porous graphene exhibit remarkable capacitive performance. The typical boron-doped MSC prepared on borax-doped polyimide film possesses an ultrahigh areal capacitance of 60.6 mF cm at 0.08 mA cm, which is approximately 20 times larger than that of undoped MSC. Furthermore, the boron-doped MSC has impressive cycling stability (with the capacitance retention of 96.3% after 20 000 cycles), exceptional mechanical flexibility, tunable capacitance, and voltage output through arbitrary modular serial and parallel integration. Besides, the nitrogen-doped porous graphene with excellent capacitive performance is also prepared by laser direct scribing on the sulfonated melamine-doped polyimide film, demonstrating excellent scalability and generality of this strategy. Hence, one-step laser direct writing on precursor-doped polyimide films can realize heteroatom doping and generation of hierarchical porous graphene electrodes simultaneously, which opens a new avenue for the facile, cost-effective, and scalable fabrication of heteroatom-doped porous graphene, thus promising for MSCs and various flexible and wearable electronics at large-scale production.
本研究提出了一种高效、简便且可扩展的策略，通过在掺杂前驱体的聚酰亚胺（PI）薄膜上进行激光直写来合成杂原子掺杂的多孔石墨烯，该PI薄膜是首次通过将PI粉末和前驱体与羧甲基纤维素钠（CMC）粘合剂混合，采用滴铸和低温干燥工艺制备而成。基于所制备的杂原子掺杂多孔石墨烯的微型超级电容器（MSC）展现出卓越的电容性能。在硼砂掺杂的聚酰亚胺薄膜上制备的典型硼掺杂MSC在0.08 mA cm下具有60.6 mF cm的超高面积电容，约为未掺杂MSC的20倍。此外，硼掺杂MSC具有令人印象深刻的循环稳定性（20000次循环后电容保持率为96.3%）、出色的机械柔韧性、可调电容以及通过任意模块化串联和并联集成实现的电压输出。此外，通过在磺化三聚氰胺掺杂的聚酰亚胺薄膜上进行激光直写，还制备出了具有优异电容性能的氮掺杂多孔石墨烯，证明了该策略具有出色的可扩展性和通用性。因此，在前驱体掺杂的聚酰亚胺薄膜上进行一步激光直写可同时实现杂原子掺杂和分级多孔石墨烯电极的生成，这为简便、经济高效且可扩展地制备杂原子掺杂多孔石墨烯开辟了一条新途径，有望用于大规模生产的MSC以及各种柔性和可穿戴电子产品。
