A Silicon Monoxide Lithium?Ion Battery Anode with Ultrahigh Areal Capacity

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Silicon monoxide (SiO) is an attractive anode material for next-generation lithium-ion batteries for its ultra-high theoreti-cal capacity of 2680 mAh -g?1. The studies to date have been limited to electrodes with a rela-tively low mass loading (< 3.5 mg -cm?2), which has seriously restricted the areal capacity and its potential in practical devices. Maximizing areal capacity with such high-capacity materials is critical for capitalizing their potential in practi-cal technologies. Herein, we report a monolithic three-dimensional (3D) large-sheet holey gra-phene framework/SiO (LHGF/SiO) composite for high-mass-loading electrode. By specifically using large-sheet holey graphene building blocks, we construct LHGF with super-elasticity and exceptional mechanical robustness, which is essential for accommodating the large volume change of SiO and ensuring the structure integrity even at ultrahigh mass loading. Addi-tionally, the 3D porous graphene network structure in LHGF ensures excellent electron and ion transport. By systematically tailoring microstructure design, we show the LHGF/SiO anode with a mass loading of 44 mg -cm?2 delivers a high areal capacity of 35.4 mAh -cm?2 at a current of 8.8 mA -cm?2 and retains a capacity of 10.6 mAh -cm?2 at 17.6 mA -cm?2, greatly exceeding those of the state-of-the-art commercial or research devices. Furthermore, we show an LHGF/SiO anode with an ultra-high mass loading of 94 mg -cm?2 delivers an unprecedented areal capacity up to 140.8 mAh -cm?2. The achievement of such high areal capacities marks a critical step toward realizing the full potential of high-capacity alloy-type electrode materials in practical lithium-ion batteries.
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