Facile Fabrication of Ethoxy-Functional Polysiloxane Wrapped LiNi0.6Co0.2Mn0.2O2 Cathode with Improved Cycling...

Dealing with the water molecule on the surface of LiNi0.6Co0.2Mn0.2O2 (NCM) cathode and hydrogen fluoride in the electrolyte is one of the most difficult challenges in Li-ion battery research. In this paper, the surface polymerization of tetraethyl orthosilicate (TEOS) on NCM to generate ethoxy-functional polysiloxane (EPS) wrapped NCM (E-NCM) cathode under mild conditions and without any additions is utilized to solve this intractable problem. The differential scanning calorimetry, transmission electron microscopy, and X-ray photoelectron spectroscopy results show that the formed amorphous coating can provide a protective shell to improve the NCM thermal stability, suppress the thickening of the solid electrolyte interphase (SEI) layer, and scavenge HF in the electrolyte. The E-NCM composite with 2 mol % EPS delivers a high discharge capacity retention of 84.9% after 100 cycles at a 1 C discharge rate in the 2.8-4.3 V potential range at 55 °C. Moreover, electrochemical impedance spectroscopy measurements reveal that the EPS coating could alleviate the impedance rise during cycling especially at an elevated temperature. Therefore, the fabricated E-NCM cathode with long-term cycling and thermal stability is a promising candidate for use in a high-energy Li-ion battery.