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

Silicon monoxide (SiO) is an attractive anode material for next-generation lithium-ion batteries for its ultra-high theoretical capacity of 2680 mAh g(−1). The studies to date have been limited to electrodes with a relatively 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 practical technologies. Herein, we report a monolithic three-dimensional (3D) large-sheet holey graphene 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. Additionally, 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. [Image: see text] SUPPLEMENTARY INFORMATION: The online version contains supplementary material available at 10.1007/s40820-022-00790-z.