Zhang Qiaoyu, Yuan Ming, Liu Lina, Li Shiyun, Chen Xuecheng, Liu Jie, Pang Xueyong, Wang Xiaojing
School of Materials Science and Engineering, Jiangsu University of Science and Technology, Zhenjiang 212003, China.
Faculty of Chemical Technology and Engineering, West Pomeranian University of Technology, Szczecin, Piastów Ave. 42, 71-065 Szczecin, Poland.
Langmuir. 2024 Mar 12;40(10):5326-5337. doi: 10.1021/acs.langmuir.3c03790. Epub 2024 Feb 26.
Capacitors with zinc ions, with excellent stabilities, low cost, and high energy density, are expected to be promising energy storage devices. However, the development of zinc-ion capacitors is quietly restricted by low specific capacity and cycling stability. Herein, to overcome these limitations, honeycomb-structured S, N-codoped carbon (SNPC) is constructed by one-pot calcination of waste corn bracts and thiourea. The honeycomb structure of SNPC is demonstrated to provide abundant active sites that can enhance the extron/ion transport, conductivity for high power export, and ion adsorption capacity in energy storage applications, leading to a higher electrochemical performance achieved. The electrolytes of zinc salt have also been studied. It reveals that the SNPC electrode presents the best electrochemical performance in a 2 M ZnSO and 0.5 M ZnCl electrolyte mixture because in the electrolyte mixture, Cl can replace the existing bound water in the solvation structure to form an anion-type water-free solvation structure ZnCl. The SNPC-800 electrode with a highly improved surface area (∼909.0 m g) is proved to be more suitable as the electrode than other materials. Aqueous zinc-ion capacitors (ZICs) have been assembled by the honeycomb-structured SNPC-800 as the cathode, which can achieve a relatively wide working voltage range of 0.1-1.8 V. The SNPC-800 ZICs exhibit a superior specific capacity of 179.1 mA h g at 0.1 A g. The energy density of SNPC-800 ZICs reaches an impressive value of 89.6 Wh kg at 53.8 W kg, and it sustains 28.3 Wh kg at 1997.6 W kg. In addition, there is 99.8% capacity retention in the SNPC-800 ZICs over 5000 cycles. The absorption energy in SPNC is much higher than that in undoped CPC, as confirmed by density functional theory, which reveals that introducing of heteroatoms (S, N) has a comparatively active advantage at increasing the Zn-ion storage capacity. This work proposes a practical strategy for the effective recycling of waste biomass materials into honeycomb carbon electrode materials. Moreover, the honeycomb carbon-based ZICs with excellent electrochemical performance and long-term cycling stability possess great potential to be a superior cathode in practical applications.
具有锌离子的电容器具有出色的稳定性、低成本和高能量密度,有望成为有前景的储能装置。然而,锌离子电容器的发展受到低比容量和循环稳定性的限制。在此,为克服这些限制,通过对废弃玉米苞叶和硫脲进行一锅煅烧构建了蜂窝状结构的硫、氮共掺杂碳(SNPC)。SNPC的蜂窝结构被证明能提供丰富的活性位点,可增强电子/离子传输、提高高功率输出的导电性以及储能应用中的离子吸附能力,从而实现更高的电化学性能。还对锌盐电解质进行了研究。结果表明,SNPC电极在2M硫酸锌和0.5M氯化锌的混合电解质中表现出最佳的电化学性能,因为在该混合电解质中,氯离子可取代溶剂化结构中现有的结合水,形成阴离子型无水溶剂化结构氯化锌。具有高度改善的表面积(约909.0平方米/克)的SNPC - 800电极被证明比其他材料更适合作为电极。以蜂窝状结构的SNPC - 800作为阴极组装了水系锌离子电容器(ZICs),其可实现0.1 - 1.8V相对较宽的工作电压范围。SNPC - 800 ZICs在0.1A/克时表现出179.1毫安时/克的优异比容量。SNPC - 800 ZICs的能量密度在53.8瓦/千克时达到令人印象深刻的89.6瓦时/千克,在1997.6瓦/千克时维持在28.3瓦时/千克。此外,SNPC - 800 ZICs在5000次循环中容量保持率为99.8%。密度泛函理论证实,SPNC中的吸收能量远高于未掺杂的CPC中的吸收能量,这表明引入杂原子(S、N)在提高锌离子存储容量方面具有相对积极的优势。这项工作提出了一种将废弃生物质材料有效回收为蜂窝状碳电极材料的实用策略。此外,具有优异电化学性能和长期循环稳定性的蜂窝状碳基ZICs在实际应用中极具潜力成为优异的阴极。