Silicon-based materials are considered as strong candidates to next-generation lithium ion battery anodes because of their ultrahigh specific capacities. However, the pulverization and delamination of electrochemical active materials originated from the huge volume expansion (>300%) of silicon during the lithiation process results in rapid capacity fade, especially in high mass loading electrodes. Here we demonstrate that direct chemical vapor deposition (CVD) growth of vertical graphene nanosheets on commercial SiO microparticles can provide a stable conducting network via interconnected vertical graphene encapsulation during lithiation, thus remarkably improving the cycling stability in high mass loading SiO anodes. The vertical graphene encapsulated SiO (d-SiO@vG) anode exhibits a high capacity of 1600 mA h/g and a retention up to 93% after 100 cycles at a high areal mass loading of 1.5 mg/cm. Furthermore, 5 wt % d-SiO@vG as additives increased the energy density of traditional graphite/NCA 18650 cell by ∼15%. We believe that the results strongly imply the important role of CVD-grown vertical graphene encapsulation in promoting the commercial application of silicon-based anodes.
If the flexible transparent and free-standing paper-like materials that would be expected to meet emerging technological demands, such as components of transparent electrical batteries, flexible solar cells, bendable electronics, paper displays, wearable computers, and so on, could be achieved in silicon, it is no doubt that the traditional semiconductor materials would be rejuvenated. Bulk silicon cannot provide a solution because it usually exhibits brittleness at below their melting point temperature due to high Peierls stress. Fortunately, when the silicon's size goes down to nanoscale, it possesses the ultralarge straining ability, which results in the possibility to design flexible transparent and self-standing silicon nanowires paper (FTS-SiNWsP). However, realization of the FTS-SiNWsP is still a challenging task due largely to the subtlety in the preparation of a unique interlocking alignment with free-catalyst controllable growth. Herein, we present a simple synthetic strategy by gas flow directed assembly of a unique interlocking alignment of the Si nanowires (SiNWs) to produce, for the first time, the FTS-SiNWsP, which consisted of interconnected SiNWs with the diameter of ~10 nm via simply free-catalyst thermal evaporation in a vertical high-frequency induction furnace. This approach opens up the possibility for creating various flexible transparent functional devices based on the FTS-SiNWsP.
Silicon/carbon (Si/C) composites have rightfully earned the attention as anode candidates for high-energy-density lithium-ion batteries (LIBs) owing to their advantageous capacity and superior cycling stability, yet their practical application remains a significant challenge. In this study, we report the large-scale synthesis of an intriguing micro/nanostructured pore-rich Si/C microsphere consisting of Si nanoparticles tightly immobilized onto a micron-sized cross-linked C matrix that is coated by a thin C layer (denoted P-Si/C@C) using a low-cost spray-drying approach and a chemical vapor deposition process with inorganic salts as pore-forming agents. The as-obtained P-Si/C@C composite has high porosity that provides sufficient inner voids to alleviate the huge volume expansion of Si. The outer smooth and robust C shells strengthen the stability of the entire structure and the solid−electrolyte interphase. Si nanoparticles embedded in a microsized cross-linked C matrix show excellent electrical conductivity and superior structural stability. By virtue of structural advantages, the asfabricated P-Si/C@C anode displays a high initial Coulombic efficiency of 89.8%, a high reversible capacity of 1269.6 mAh g −1 at 100 mA g −1 , and excellent cycle performance with a capacity of 708.6 mAh g −1 and 87.1% capacity retention after 820 cycles at 1000 mA g −1 , outperforming the reported results of Si/C composite anodes. Furthermore, a low electrode swelling of 18.1% at a high areal capacity of 3.8 mAh cm −2 can be obtained. When assembled into a practical 3.2 Ah cylindrical cell, extraordinary long cycling life with a capacity retention of 81.4% even after 1200 cycles at 1C (3.2 A) and excellent rate performance are achieved, indicating significant advantages for long-life power batteries in electric vehicles.
Si with high theoretical capacity has long suffered from its large volume variation and low electrical transport linked to poor cycling stability and rate performance.
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