Endothermic Dehydrogenation-Driven Preventive Magnesiation of Sio by Magnesium Hydride for High-Performance Sio-Based Lithium Storage Materials

Abstract

Silicon monoxide (SiO)-based materials have gained much attention as high-capacity lithium storage materials because of their superior cycle performance. However, low initial Coulombic efficiency (ICE) of SiO derived from the irreversible electrochemical reaction of the amorphous SiO2 phase in SiO makes wide use of the SiO-based anode materials in lithium-ion batteries challenging. Magnesiation of SiO is one of the promising solutions to improve ICE of SiO-based anode materials. Here, we propose an endothermic dehydrogenation-driven magnesiation of SiO by employing MgH2 to improve both ICE and cycle performance. The resulting Si/Mg2SiO4 nanocomposite material showed much-improved ICE of 89.5% and long-term cycle performance for over 300 cycles compared to the homologue prepared by the magnesiation of SiO using Mg and pristine SiO. High-resolution transmission electron microscopy with thermogravimetry−differential scanning calorimetry revealed that the endothermic dehydrogenation of MgH2 mitigates the rapid temperature rise during magnesiation of SiO, thereby inhibiting the increase of Si domain size in the resulting Si/Mg2SiO4 nanocomposite. Detailed material characterization and electrochemical analysis of Si/Mg2SiO4 nanocomposite materials will be discussed in this presentation.