Chen Tsung-Yi, Thang Ho Viet, Yi Tien-Yu, Huang Shao-Chu, Lin Chia-Ching, Chang Yu-Ming, Chen Pei-Lin, Lin Ming-Hsien, Lee Jyh-Fu, Chen Hsin-Yi Tiffany, Hu Chi-Chang, Chen Han-Yi
Department of Materials Science and Engineering, National Tsing Hua University, 101, Sec. 2, Kuang-Fu Road, Hsinchu300044, Taiwan.
High Entropy Materials Center, 101, Sec. 2, Kuang-Fu Road, Hsinchu300044, Taiwan.
ACS Appl Mater Interfaces. 2022 Nov 23;14(46):52035-52045. doi: 10.1021/acsami.2c16777. Epub 2022 Nov 8.
Ni-containing heteropolyvanadate, Na[NiVO], was synthesized for the first time to be applied in high-energy lithium storage applications as a negative electrode material. Na[NiVO] can be prepared via a facile solution process that is suitable for low-cost mass production. The as-prepared electrode provided a high capacity of approximately 700 mAh g without degradation for 400 cycles, indicating excellent cycling stability. The mechanism of charge storage was investigated using operando X-ray absorption spectroscopy (XAS), X-ray diffraction (XRD), transition X-ray microscopy (TXM), and density functional theory (DFT) calculations. The results showed that V was reduced to V during lithiation, indicating that Na[NiVO] is an insertion-type material. In addition, Na[NiVO] maintained its amorphous structure with negligible volume expansion/contraction during cycling. Employed as the negative electrode in a lithium-ion battery (LIB), the Na[NiVO]//LiFePO full cell had a high energy density of 300 W h kg. When applied in a lithium-ion capacitor, the Na[NiVO]//expanded mesocarbon microbead full cell displayed energy densities of 218.5 and 47.9 W h kg at power densities of 175.7 and 7774.2 W kg, respectively. These findings reveal that the negative electrode material Na[NiVO] is a promising candidate for Li-ion storage applications.
首次合成了含镍杂多钒酸盐Na[NiVO]，以作为负极材料应用于高能储能领域。Na[NiVO]可通过一种简便的溶液法制备，该方法适用于低成本大规模生产。所制备的电极提供了约700 mAh g的高容量，在400次循环中无降解，表明具有优异的循环稳定性。使用原位X射线吸收光谱（XAS）、X射线衍射（XRD）、过渡X射线显微镜（TXM）和密度泛函理论（DFT）计算研究了电荷存储机制。结果表明，在锂化过程中V被还原为V，这表明Na[NiVO]是一种插入型材料。此外，Na[NiVO]在循环过程中保持其非晶结构，体积膨胀/收缩可忽略不计。作为锂离子电池（LIB）的负极，Na[NiVO]//LiFePO全电池具有300 W h kg的高能量密度。当应用于锂离子电容器时，Na[NiVO]//膨胀中碳微珠全电池在功率密度分别为175.7和7774.2 W kg时，能量密度分别为218.5和47.9 W h kg。这些发现表明，负极材料Na[NiVO]是锂离子存储应用的一个有前途的候选材料。
