The specific capacity of commercially available cathode carbon-coated lithium iron phosphate is typically 120-160 mAh g À 1 , which is lower than the theoretical value 170 mAh g À 1 . Here we report that the carbon-coated lithium iron phosphate, surface-modified with 2 wt% of the electrochemically exfoliated graphene layers, is able to reach 208 mAh g À 1 in specific capacity. The excess capacity is attributed to the reversible reduction-oxidation reaction between the lithium ions of the electrolyte and the exfoliated graphene flakes, where the graphene flakes exhibit a capacity higher than 2,000 mAh g À 1 . The highly conductive graphene flakes wrapping around carbon-coated lithium iron phosphate also assist the electron migration during the charge/discharge processes, diminishing the irreversible capacity at the first cycle and leading to B100% coulombic efficiency without fading at various C-rates. Such a simple and scalable approach may also be applied to other cathode systems, boosting up the capacity for various Li batteries.

Reconstructing carbon nanomaterials (e.g., fullerene, carbon nanotubes (CNTs), and graphene) to multidimensional networks with hierarchical structure is a critical step in exploring their applications. Herein, a sacrificial template method by casting strategy is developed to prepare highly flexible and free-standing carbon film consisting of CNTs, graphene, or both. The scalable size, ultralight and binder-free characteristics, as well as the tunable process/property are promising for their large-scale applications, such as utilizing as interlayers in lithium-sulfur battery. The capability of holding polysulfides (i.e., suppressing the sulfur diffusion) for the networks made from CNTs, graphene, or their mixture is pronounced, among which CNTs are the best. The diffusion process of polysulfides can be visualized in a specially designed glass tube battery. X-ray photoelectron spectroscopy analysis of discharged electrodes was performed to characterize the species in electrodes. A detailed analysis of lithium diffusion constant, electrochemical impedance, and elementary distribution of sulfur in electrodes has been performed to further illustrate the differences of different carbon interlayers for Li-S batteries. The proposed simple and enlargeable production of carbon-based networks may facilitate their applications in battery industry even as a flexible cathode directly. The versatile and reconstructive strategy is extendable to prepare other flexible films and/or membranes for wider applications.

In this study we prepared molybdenum trioxide (MoO3) nanorods having average lengths of 0.5-1.5 μm and widths of approximately 100-200 nm through a one-step mechanical break-down process involving favorable fracturing along the crystal direction. We controlled the dimensions of the as-prepared nanorods by applying various imposing times (15-90 min). The nanorods prepared over a reaction time of 90 min were, on average, much shorter and narrower relative to those obtained over 30 min. Evaluations of lithium-ion storage properties revealed that the electrochemical performance of these nanorods was much better than that of bulk materials. As cathodes, the nanorods could deliver a high specific capacity (>315 mA h g(-1)) with losses of less than 2% in the first cycle at a rate of 30 mA g(-1); as anodes, the specific capacity was 800 mA h g(-1) at a rate of 50 mA g(-1). Relative to α-MoO3 microparticles, these nanorods displayed significantly enhanced lithium-ion storage properties with higher reversible capacities and better rate performance, presumably because their much shorter diffusion lengths and higher specific surface areas allowed more-efficient insertion/deinsertion of lithium ions during the charge/discharge process. Accordingly, enhanced physical and/or chemical properties can be obtained through appropriate nanostructuring of materials.

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Elementary sulphur (S) has been shown to be an excellent cathode material in energy storage devices such as Li-S batteries owing to its very high capacity. The major challenges associated with the sulphur cathodes are structural degradation, poor cycling performance and instability of the solid-electrolyte interphase caused by the dissolution of polysulfides during cycling. Tremendous efforts made by others have demonstrated that encapsulation of S materials improves their cycling performance. To make this approach practical for large scale applications, the use of low-cost technology and materials has become a crucial and new focus of S-based Li-ion batteries. Herein, we propose to use a low temperature spraying process to fabricate graphene/S electrode material, where the ink is composed of graphene flakes and the micron-sized S particles prepared by grinding of low-cost S powders. The S particles are found to be well hosted by highly conductive graphene flakes and consequently superior cyclability (∼70% capacity retention after 250 cycles), good coulombic efficiency (∼98%) and high capacity (∼1500 mA h g(-1)) are obtained. The proposed approach does not require high temperature annealing or baking; hence, another great advantage is to make flexible Li-ion batteries. We have also demonstrated two types of flexible batteries using sprayed graphene/S electrodes.

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