Direct-Contact Prelithiation of Si-C Anode Study as a Function of Time, Pressure, Temperature, and the Cell Ideal...

Direct-contact prelithiation (PL) is a facile, practical, and scalable method to overcome the first-cycle loss and large volume expansion issues for silicon anode (with 30 wt % Si loading) material, and a detailed study is absent. Here, an understanding of direct-contact PL as a function of the PL time, and the effects of externally applied pressure (weight), microstructure, and operating temperature have been studied. The impact of PL on the Si-C electrode surfaces has been analyzed by electrochemical techniques and different microstructural analyses. The solid electrolyte interface (SEI) layer thickness increases with the increase in PL time and decreases after 2 min of PL time. The ideal PL time was found to be between 15 (PL-15) and 30 (PL-30) min with 83.5 and 97.3% initial Coulombic efficiency (ICE), respectively, for 20 g of externally applied weight. The PL-15 and PL-30 cells showed better cyclic stability than PL-0 (without prelithiation), with more than 90% capacity retention after 500 cycles at 1 A g^-1 current density. The discharge capacities for PL-15 and PL-30 have been observed as highest at 45 °C operating temperature with limited cyclability. We propose here a synchronization strategy in prelithiation time, pressure, and temperature to achieve excellent cell performance.