Interfacial Control for Enhanced Cycling Performance of Li-Ion Battery with Silicon-Based Anode and High-Voltage Layered Oxide Cathode
Authors: Nguyen Dan Thien , Nam Kyoung-Mo , Song Seung-Wan 
Published: February 2020

Advanced portable electronics, electric vehicles and energy storage systems need more than doubled energy density lithium-ion battery than current one consisting of graphite anode and LiCoO2 cathode. High-capacity silicon-based anode materials and high-voltage three-components layered oxide cathode materials have been actively researched for higher energy density batteries. Various methods for improving the cycling performance of silicon-based anode have been developed but mostly evaluated using a half-cell configuration.1,2 Just few reports on the performance of high-energy full-cells with silicon-based anode together with high-voltage cathode have been reported.3–5 This is associated with poor cycling ability of silicon-based anodes and continuous oxidative electrolyte decomposition above 4.3 V vs. Li/Li+. Nonetheless, interfacial reaction mechanisms for performance fade or enhancement of full-cells have not been studied in depth. Interfacial control with electrolyte components and surface structural stabilization of both anode and cathode are promising approaches for enhancement of full-cell performance.6,7 In this presentation, we report the enhanced cycling performance of high-energy full-cell with silicon-carbon composite anode and high-voltage layered LiNi0.5Co0.2Mn0.3O2 cathode (NCM) by interfacial control and the role of electrolyte component in enhancing the performance.

The 2016 coin full-cells of NCM//silicon-carbon composite were assembled with different electrolyte compositions. Cycling performance of full-cells was tested between 3.0 and 4.55 V at the rate of C/3 (330 mAg-1) for 100 cycles. Impedance spectroscopy, Raman spectroscopy, FT infrared spectroscopy, X-ray photoelectron spectroscopy and scanning electron microscope have been used to analyze electrochemical behaviors depending on electrolyte composition and surface chemistry of both cathode and anode.

Figure 1a-b compare the cycling performance of NCM//silicon-carbon composite full-cells in the conventional electrolyte of 1M LiPF6/EC:EMC (3:7) and a new electrolyte consisting of new solvents and additives. With the conventional electrolyte, the full-cell shows a rapid capacity fade and a low coulombic efficiency over 100 cycles. In contrary, the full-cell with a new electrolyte exhibits a significant performance enhancement; capacity retention is 71 % at the 100th cycle, and coulombic efficiency is maintained as higher than 99 %. Surface analyses of cathode and anode reveal that with new electrolyte a stable solid electrolyte interphase (SEI) layer forms at both surfaces of cathode and anode and a metal dissolution event from cathode is inhibited. Further discussion on interfacial control-performance relationship would be presented in the meeting.

Acknowledgements

This research was supported partly by the Korean Ministry of Education (2012026203) and partly by the Korean Ministry of Trade, Industry & Energy (A0022-00725 & 10049609).

References

1. N. Dimov, S. Kugino, and M. Yoshio, J. Power Sources, 136, 108 (2004).

2. M. Gauthier, D. Mazouzi, D. Reyter, B. Lestriez, P. Moreau, D. Guyomard, and L. Roué, Energy Environ. Sci., 6, 2145 (2013).

3. S. J. Lee, J.G. Han, Y. Lee, M.H. Jeong, W. C. Shin, M. Ue, and N.S. Choi, Electrochim. Acta, 137, 1 (2014).

4. X. Zhao, M. Li, K.H. Chang, and Y.M. Lin, Nano Res., 7, 1429 (2014).

5. L. Ji, H. Zheng, A. Ismach, Z. Tan, S. Xun, E. Lin, V. Battaglia, V. Srinivasan, and Y. Zhang, Nano Energy, 1, 164 (2012).

6. J.S. Kim, C.C. Nguyen, H.J. Kim, and S.W. Song, RSC Adv., 4, 12878 (2014).

7. Y.M. Lee, K. M. Nam, E.H. Hwang, Y. K. Kwon, D. H. Kang, S.S. Kim, and S.W. Song, J. Phys. Chem. C, 118, 10631(2014).

Figure 1