Li2O-Based Cathode Additives Enabling Prelithiation of Si Anodes

Low first-cycle Coulombic efficiency is especially poor for silicon (Si)-based anodes due to the high surface area of the Si-active material and extensive electrolyte decomposition during the initial cycles forming the solid electrolyte interphase (SEI). Therefore, developing successful prelithiation methods will greatly benefit the development of lithium-ion batteries (LiBs) utilizing Si anodes. In pursuit of this goal, in this study, lithium oxide (Li2O) was added to a LiNi0.6Mn0.2Co0.2O2 (NMC622) cathode using a scalable ball-milling approach to compensate for the initial Li loss at the anode. Different milling conditions were tested to evaluate the impact of particle morphology on the additive performance. In addition, Co3O4, a well-known oxygen evolution reaction catalyst, was introduced to facilitate the activation of Li2O. The Li2O + Co3O4 additives successfully delivered an additional capacity of 1116 mAh/gLi2O when charged up to 4.3 V in half cells and 1035 mAh/gLi2O when charged up to 4.1 V in full cells using Si anodes.

A Strategic Approach to Use Upcycled Si Nanomaterials for Stable Operation of Lithium-Ion Batteries

Silicon, as a promising next-generation anode material, has drawn special attention from industries due to its high theoretical capacity (around 3600 mAh g−1) in comparison with conventional electrodes, e.g., graphite. However, the fast capacity fading resulted by a large volume change hinders the pragmatic use of Si anodes for lithium ion batteries. In this work, we propose an efficient strategy to improve the cyclability of upcycled Si nanomaterials through a simple battery operation protocol. When the utilization degree of Si electrodes was decreased, the electrode deformation was significantly alleviated. This directly led to an excellent electrochemical performance over 100 cycles. In addition, the average charge (delithation) voltage was shifted to a lower voltage, when the utilization degree of electrodes was controlled. These results demonstrated that our strategic approach would be an effective way to enhance the electrochemical performance of Si anodes and improve the cost-effectiveness of scaling-up the decent nanostructured Si material.

Water-Soluble Elastomeric Carboxymethyl Chitosan as an Efficient Binder for Si Anodes of Lithium Ion Batteries

The binder acts a pivotal part in determining the mechanical and electrochemical performances of lithium-ion battery electrodes. Herein, a series of water-soluble Si anode binders based on carboxymethyl chitosan (C-Cs) and styrene-butadiene rubber (SBR) is developed. Water-soluble C-Cs and aqueous emulsion SBR solution are mixed to form C-Cs/SBR binders. The physical properties of the modified Si electrode are investigated through electrolyte swelling test, peeling test, and scanning electron microscopy. The mechanical strength provided to Cu foils and active substances by the C-Cs/SBR binder is higher than that produced by C-Cs. This performance can effectively reduce the stress/strain caused by the drastic volume change of the Si anodes during repeated uses and improve the electrochemical property of lithium-ion batteries. The initial thicknesses of the Si electrodes with polyvinylidene fluoride, C-Cs, and C-Cs/SBR20 binders are approximately 7.1, 7.2, and 6.9 µm, respectively. After 100 cycles, their initial thicknesses increase to 11.2, 12.4, and 7.2 µm and correspond to expansions of 57.8%, 72.2%, and 4.3%, respectively. The discharge capacity of Si electrodes containing C-Cs/SBR20 binder reaches to 1340 mAh·g−1 when the current density is 4 A·g−1, and reserves to be 1020 mAh·g−1 after undergoing 400 cycles of repeated use at 500 mA·g−1.