Silicon is a promising material for lithium-ion batteries due to its super high capacity.1 However, the volume expansion and the pulverization of Si limit its perforamce.2 This study investigates the effect of a polymer brush core-shell structure of Si as an anode material. The polymer brush is designed through Si-C covalent bond of vinyl monomers by thermal hydrosilylation reaction. According to the results, the PBCS structure provides three significant functions on Si particles because of the intramolecular effect of hydrogen bonding with PBCS and binder delivers a good dispersion in the slurry, a mechanical protection during cycling, and excellent ionic conductivity for high-rate tests. Compared with the unmodified electrode (SiNP), the modified electrodes (SiNP-M1 and SiNP-M2) incorporating the PBCS provides better initial columbic efficiency of 87.1% with the first discharge capacity of 1988.9 mAh g-1. The TEM and operando TXM results display that the PBCS structure significantly protects the nano Si from cracking owing to the high elastic function and intramolecular hydrogen bonding effect of the PBCS. Operando X-ray diffraction is also used to provide the phase information of the Si electrodes. With this novel PBCS-Si material, a high energy density lithium-ion battery contains pure Si can be expected. Reference Li, C.; Shi, T.; Li, D.; Yoshitake, H.; Wang, H., Effect of surface modification on electrochemical performance of nano-sized Si as an anode material for Li-ion batteries. RSC Advances 2016, 6 (41), 34715-34723.Gao, Y.; Yi, R.; Li, Y. C.; Song, J.; Chen, S.; Huang, Q.; Mallouk, T. E.; Wang, D., General Method of Manipulating Formation, Composition, and Morphology of Solid-Electrolyte Interphases for Stable Li-Alloy Anodes. J Am Chem Soc 2017, 139 (48), 17359-17367. Figure 1
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