Firstly, this research focused on determining appropriate temperature for the elevated temperature test. Serious capacity fading and polarization of the electrode was found with the increased temperature. To balance the safety operation and necessary temperature effect on the LIB, optimum temperature for testing the cell was selected.
Secondly, a novel method for the electrode modification is developed using the plasma enhanced chemical vapor deposition (PECVD) process. This process successfully deposited Teflon thin film on the LrMNO based electrodes. Coin cells were assembled using the pristine/modified electrodes and tested both at room temperature and 55 oC. Since Teflon layer has the anti-corrosion property and thermal stability, the Teflon coated electrodes have prevented the attacks from the electrolyte byproducts and their performance was also improved at the elevated temperature. Polarization of the modified electrodes during cycling apparently reduced and cycling performance of the electrode enhanced, subsequently.
Thirdly, instead of modifying on the electrode surface, the functional polymers was directly coated on the NCM particles by environmental friendly less power consuming water-based coating process. In the first part, single polymer PSSNa modification was made on the NCM particles. This has obtained improved performance, particularly high-rate capability due to the possible interaction between the electron lone pairs present in the anionic polymer and the Li+. Besides, the organic compounds of the polymer could have facilitated the de-solvation and solvation process of the Li-ion. The relative higher charge transfer resistance in the early stage of polymer modified cells was solved by the addition of Super P, in which, the electrostatic self-assembling technique by the cationic and anionic polymer (PDDA-PSSNa) have been employed for the Super P attachment. By this technique, the Super P showed good adhesion on
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the NCM particles. In addition, the modified samples also demonstrated the enhancement in the cycle performance at 55 oC. After the electrochemical operation, in terms of the reduced electrolyte decomposition and SEI formation can strongly relative to the contribution of the polymer-physical-barrier layer on the material surface.
Furthermore, the inhibition of the phase transformation in the surface structure of polymer-coated particles could be also examined. In the second part of polymer modification, the Li-type PSS has been prepared and used to replace the Na-type PSS onto the NCM material. The result demonstrated the better rate capability in the Li-type PSS than that of the Na-type modified sample. It could be attributed to the Li-ion migrating that is more kinetics favor in the lithium-containing polymer film. The 1 % CNT as the conductive agent has also participated in the polymer coating. With the PSSLi and concomitant CNT networks modification, the considerable improvement in the reversible capacity, rate capability, and cycle stability can be simultaneously achieved.
Finally, the elevated high cut-off operating potential (4.6 V) of the NCM has been investigated. The intense electrolyte decomposition was come up in the non-treated NCM cell, causing the serious capacity fading during the cycling. In contrast, the polymer and CNT-polymer modified cells could maintain the well capacity retention (>
90 %) after cycling at such the high operating potential. Additionally, the more cation mixing appeared in the pristine cell may associate with the exposing of materials to the electrolyte. By comparison, the polymeric A-SEI we constructed on the NCM particle surface could show the capability to stabilize the electrode-electrolyte interface further gives the substantial promotions in the electrochemical performance.
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