Fu Qishan, Yang Muzi, Liu Zhongfei, Yang Hao, She Fengquan, Zhang Xiaoqi, Xie Fangyan, Hu Yuwen, Chen Jian
School of Materials Science and Engineering, Sun Yat-sen University, Guangzhou 510725, China.
Instrumental Analysis and Research Centre, Sun Yat-sen University, Guangzhou 510275, China.
J Colloid Interface Sci. 2022 Jul 15;618:161-172. doi: 10.1016/j.jcis.2022.03.060. Epub 2022 Mar 16.
Two-dimensional (2D) transition metal carbides (MXene) have shown great advantages as electrode materials in the new generation of energy storage, especially in supercapacitors. However, the inherent low specific capacitance and restacking layers of nanosheets that occur during electrode preparation further reduce the electrochemical performance of the materials. Based on this, we design a N, S co-doping electrode with a three-dimensional (3D) structure, which not only improves the specific capacitance through fundamentally modifying the electronic structure of the electrode materials, but also effectively improves the rate performance of the electrode by preventing the restacking of 2D materials. The N, S co-doping 3D architecture TiCT electrode (TC/NS-3D) exhibits an excellent capacitance value of 440 F g at 5 mV s and 64% capacitance retention rate at a high scan rate of 1000 mV s in 3 mol L HSO electrolyte. The TC/NS-3D electrode also shows excellent capacitance retention of 97.2% after the 10,000 cycles stability test. The density functional theory (DFT) analysis reveals the enhanced performance is attributed to accelerated intermediates transport kinetics promoted by 3D structure engineering and N, S co-doping for TiCT. This study is promising in designing heteroatomic doping 3D structure MXene-based materials for electrochemical energy storage systems.
二维(2D)过渡金属碳化物(MXene)在新一代储能领域,尤其是超级电容器中,作为电极材料展现出了巨大优势。然而,电极制备过程中纳米片固有的低比电容和重新堆叠现象进一步降低了材料的电化学性能。基于此,我们设计了一种具有三维(3D)结构的氮、硫共掺杂电极,它不仅通过从根本上改变电极材料的电子结构来提高比电容,还通过防止二维材料的重新堆叠有效地提高了电极的倍率性能。氮、硫共掺杂三维结构TiCT电极(TC/NS-3D)在3 mol·L HSO电解质中,扫描速率为5 mV·s时展现出440 F·g的优异电容值,在1000 mV·s的高扫描速率下电容保持率为64%。在进行10000次循环稳定性测试后,TC/NS-3D电极也显示出97.2%的优异电容保持率。密度泛函理论(DFT)分析表明,性能增强归因于三维结构工程以及对TiCT进行氮、硫共掺杂所促进的中间体传输动力学加速。这项研究对于设计用于电化学储能系统的杂原子掺杂三维结构MXene基材料具有重要意义。