Dual-modified LiNi0.8Co0.1Mn0.1O2 cathode materials with lithium conducting hybrid oligomer and single-walled carbon nanotube for improving electrochemical performance and thermal stability of lithium-ion batteries: A novel approach for high-power and high-safety applications

In this study, we investigated the synergetic effect of a novel lithium-ion conducting hybrid oligomer [N, N′-bismaleimide-4, 4′-diphenylmethane (BMI), lithiated trithiocyanuric acid (Li-TCA) and Jeffamine®-M1000 (JA®); Li-BTJ] coating layer on a nickel-rich LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode material wrapped with highly electron-conductive single-walled carbon nanotubes (SWCNTs) to enhance electrochemical performance and thermal stability for high-power and high-safety lithium-ion batteries (LIBs). Morphological analyses using scanning electron microscopy/energy dispersive spectroscopy and transmission electron microscopy showed that the NCM811 active material surface was uniformly coated with a hybrid oligomer to form NCM811@Li-BTJ, which was subsequently wrapped with SWCNTs (NCM@Li-BTJ/SWCNT composite cathode). CR2032 coin-type cells with optimized NCM811@1 wt% Li-BTJ/0.2 wt% SWCNT composite electrodes delivered a significantly enhanced capacity retention (CR) of 90.1 % relative to that of bare NCM811 electrodes (CR: 82.1 %) at 1C for 200 cycles from 2.8 to 4.3 V (vs. Li/Li+). Electrochemical impedance spectroscopy and cyclic voltammetry revealed that this superior cycling performance resulted from a lower charge transfer resistance (Rct: 96.2 vs. 324.3 Ω) and a lower polarization voltage (∆V: 0.243 vs. 0.411 V vs. Li/Li+). The in-situ micro-calorimetric results presented the total heat generation (Qt) values of the coin cells with the delithiated NCM811@Li-BTJ and NCM@Li-BTJ/SWCNT electrodes at 5C and 35 °C were substantially lower by ~9.3 % and ~ 14.6 %, respectively, compared to the bare NCM811 counterpart, indicating that the surface modifications on the NCM811 active materials could prevent the LIBs' thermal instability. Furthermore, X-ray photoelectron spectroscopy studies revealed that the Li-BTJ hybrid oligomer coating layer effectively suppressed the formation of residual Li side products such as Li2CO3 evidently on the surface of the NCM811 active material particles, thereby inhibiting undesirable side reactions. Post-mortem analyses of the dual-modified NCM811 electrode after cycling revealed that the microstructure and particle morphology of the NCM composite cathode material were extensively maintained through the synergistic effects of the Li-BTJ ion-conductive and SWCNTs electron-conductive agents.