Dai Juguo, Yang Chunying, Xu Yiting, Wang Xiaohong, Yang Siyu, Li Dongxu, Luo Lili, Xia Long, Li Junshan, Qi Xueqiang, Cabot Andreu, Dai Lizong
Fujian Provincial Key Laboratory of Fire Retardant Materials, College of Materials, Xiamen University, Xiamen, 361005, China.
Catalonia Institute for Energy Research (IREC), Sant Adrià de Besòs, Barcelona, Catalonia, 08930, Spain.
Adv Mater. 2023 Sep;35(39):e2303732. doi: 10.1002/adma.202303732. Epub 2023 Aug 7.
Ammonium-ion aqueous supercapacitors are raising notable attention owing to their cost, safety, and environmental advantages, but the development of optimized electrode materials for ammonium-ion storage still lacks behind expectations. To overcome current challenges, here, a sulfide-based composite electrode based on MoS and polyaniline (MoS @PANI) is proposed as an ammonium-ion host. The optimized composite possesses specific capacitances above 450 F g at 1 A g , and 86.3% capacitance retention after 5000 cycles in a three-electrode configuration. PANI not only contributes to the electrochemical performance but also plays a key role in defining the final MoS architecture. Symmetric supercapacitors assembled with such electrodes display energy densities above 60 Wh kg at a power density of 725 W kg . Compared with Li and K ions, the surface capacitive contribution in NH -based devices is lower at every scan rate, which points to an effective generation/breaking of H-bonds as the mechanism controlling the rate of NH insertion/de-insertion. This result is supported by density functional theory calculations, which also show that sulfur vacancies effectively enhance the NH adsorption energy and improve the electrical conductivity of the whole composite. Overall, this work demonstrates the great potential of composite engineering in optimizing the performance of ammonium-ion insertion electrodes.
铵离子水系超级电容器因其成本、安全性和环境优势而备受关注,但用于铵离子存储的优化电极材料的开发仍落后于预期。为了克服当前的挑战,本文提出了一种基于硫化钼(MoS)和聚苯胺(MoS@PANI)的硫化物基复合电极作为铵离子主体。优化后的复合材料在三电极配置下,在1 A g时的比电容高于450 F g,在5000次循环后电容保持率为86.3%。聚苯胺不仅有助于提高电化学性能,而且在确定最终的硫化钼结构中起着关键作用。用这种电极组装的对称超级电容器在功率密度为725 W kg时的能量密度高于60 Wh kg。与锂离子和钾离子相比,在每个扫描速率下,基于铵离子的器件中的表面电容贡献较低,这表明氢键的有效生成/断裂是控制铵离子插入/脱插速率的机制。密度泛函理论计算支持了这一结果,该计算还表明硫空位有效地提高了铵离子的吸附能量,并改善了整个复合材料的电导率。总体而言,这项工作证明了复合工程在优化铵离子插入电极性能方面的巨大潜力。