Two-dimensional Si nanosheets have been studied as a promising candidate for lithium-ion battery anode materials. However, Si nanosheets reported so far showed poor cycling performances and required further improvements. In this work, we utilize inexpensive natural clays for preparing high quality Si nanosheets via a one-step simultaneous molten salt-induced exfoliation and chemical reduction process. This approach produces high purity mesoporous Si nanosheets in high yield. As a control experiment, two-step process (pre-exfoliated silicate sheets and subsequent chemical reduction) cannot sustain their original two-dimensional structure. In contrast, one-step method results in a production of 5 nm-thick highly porous Si nanosheets. Carbon-coated Si nanosheet anodes exhibit a high reversible capacity of 865 mAh g(-1) at 1.0 A g(-1) with an outstanding capacity retention of 92.3% after 500 cycles. It also delivers high rate capability, corresponding to a capacity of 60% at 20 A g(-1) compared to that of 2.0 A g(-1). Furthermore, the Si nanosheet electrodes show volume expansion of only 42% after 200 cycles.

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We show that a high energy density can be achieved in a practical manner with freestanding electrodes without using conductive carbon, binders, and current collectors. We made and used a folded graphene composite electrode designed for a high areal capacity anode. The traditional thick graphene composite electrode, such as made by filtering graphene oxide to create a thin film and reducing it such as through chemical or thermal methods, has sluggish reaction kinetics. Instead, we have made and tested a thin composite film electrode that was folded several times using a water-assisted method; it provides a continuous electron transport path in the fold regions and introduces more channels between the folded layers, which significantly enhances the electron/ion transport kinetics. A fold electrode consisting of SnO/graphene with high areal loading of 5 mg cm has a high areal capacity of 4.15 mAh cm, well above commercial graphite anodes (2.50-3.50 mAh cm), while the thickness is maintained as low as ∼20 μm. The fold electrode shows stable cycling over 500 cycles at 1.70 mA cm and improved rate capability compared to thick electrodes with the same mass loading but without folds. A full cell of fold electrode coupled with LiCoO cathode was assembled and delivered an areal capacity of 2.84 mAh cm after 300 cycles. This folding strategy can be extended to other electrode materials and rechargeable batteries.

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Three-dimensional (3D) hyperporous silicon flakes (HPSFs) are prepared via the chemical reduction of natural clay minerals bearing metal oxides. Natural clays generally have 2D flake-like structures with broad size distributions in the lateral dimension and varied thicknesses depending on the first processing condition from nature. They have repeating layers of silicate and metal oxides in various ratios. When the clay mineral is subjected to a reduction reaction, metal oxide layers can perform a negative catalyst for absorbing large amounts of exothermic heat from the reduction reaction of the silicate layers with metal reductant. Selectively etching out metal oxides shows a hyperporous nanoflake structure containing 100 nm macropores and meso-/micropores on its framework. The resultant HPSFs are demonstrated as anode materials for lithium-ion batteries. Compared to conventional micro-Si anodes, HPSFs exhibit exceptionally high initial Coulombic efficiency over 92%. Furthermore, HPSF anodes show outstanding cycling performance (reversible capacity of 1619 mAh g at a rate of 0.5 C after 200 cycles, 95.2% retention) and rate performance (∼580 mAh g at a rate of 10 C) owing to their distinctive structure.