期刊
CHEMICAL ENGINEERING JOURNAL
卷 428, 期 -, 页码 -出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2021.132648
关键词
Li metal anodes; Ni2P nanoparticles; Hollow carbon spheres; Homogeneous Li deposition; Large-scale production
资金
- National Natural Science Foundation of China [51874361, 52034011]
- Science and Technology program of Hunan Province [2019RS3002, 2020GK2074]
- Fundamental Research Funds for the Central Universities of Central South University [2020zzts086]
The study demonstrates a large-scale production method for three-dimensional interconnected stacked hollow carbon spheres modified with evenly dispersed Ni2P nanoparticles, which improves ion/electron conductivity. Density functional theory calculations show that Li+ adsorbs onto Ni2P nanoparticles with higher binding energy, leading to lower nucleation overpotential and better electrochemical performance. These findings have significant potential for practical applications in high-performance Li metal anodes.
Porous carbon is a promising host for stable lithium (Li) metal composite anodes. However, homogeneous lithiophilicity modification and large-scale production of these material are difficult to address simultaneously, leading to poor electrochemical performance and limiting practical application of Li metal anode. Herein, we display a large-scale productive three-dimensional (3D) interconnected stacked hollow carbon spheres modified with evenly dispersed Ni2P nanoparticles (Ni2P@ISHCP). Interestingly, the interconnected hollow carbon skeletons are further graphitized during the simple and scalable preparation process of Ni2P nanoparticles, which is favorable for the higher ion/electron conductivity. Impressively, density functional theory calculations (DFT) demonstrate Li+ adsorbs Ni2P nanoparticle presenting the stronger binding energy and a mass of charge transfer compared with pure carbon. It benefits a lower nucleation overpotential and the homogeneous Li selective deposition into the 3D interconnected hollow spheres. As expected, a superior average Coulombic efficiency (CE) of 98.4% near 400 cycles at 1 mA cm-2 and a long cycling life over 1000 h cycling with a low overpotential of 12 mV are successfully achieved. Coupled with a LiFePO4 cathode, the fabricated full-cell exhibits a capacity retention of 99.3% with 135 mAh g-1 over 200 cycles at 1C and outstanding rate capability, presenting the tremendous practical application potential.
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