Sodium-ion batteries (SIBs) are considered a top alternative to lithium-ion batteries (LIBs) for large-scale renewable energy storage units due to their low cost and the abundance of sodium-bearing precursors in the earth's mineral deposits. However, the development of anode materials for SIBs to date has been mainly limited to carbonaceous materials with minimal research devoted to high capacity alloy-based materials. In this study, an antimony (Sb)/carbon (C) electrode with ~30 nm Sb nanoparticles (NPs) uniformly encapsulated in interconnecting one-dimensional (1D) 400 nm carbon fibers (denoted as SbNP@C) was fabricated using a simple and scalable electrospinning method. This binder-free, current collector-free SbNP@C electrode demonstrated high capacity and stable long-term cycling performance at various current densities. The SbNP@C electrode showed an initial total capacity of 422 mAh/gelectrode and retained 350 mAh/gelectrode after 300 deep charge-discharge cycles under 100 mA/gSb. Moreover, because of the efficient 1D sodium-ion transport pathway and the highly conductive network of SbNP@C, the electrode preserved high overall capacities even when cycled at high currents, extending its usability to high power applications.
The electrochemical performance of mesoporous carbon (C)/tin (Sn) anodes in Na‐ion and Li‐ion batteries is systematically investigated. The mesoporous C/Sn anodes in a Na‐ion battery shows similar cycling stability but lower capacity and poorer rate capability than that in a Li‐ion battery. The desodiation potentials of Sn anodes are approximately 0.21 V lower than delithiation potentials. The low capacity and poor rate capability of C/Sn anode in Na‐ion batteries is mainly due to the large Na‐ion size, resulting in slow Na‐ion diffusion and large volume change of porous C/Sn composite anode during alloy/dealloy reactions. Understanding of the reaction mechanism between Sn and Na ions will provide insight towards exploring and designing new alloy‐based anode materials for Na‐ion batteries.
Selenium-impregnated carbon composites were synthesized by infusing Se into mesoporous carbon at a temperature of 600 °C under vacuum. Ring-structured Se8 was produced and confined in the mesoporous carbon, which acts as an electronic conductive matrix. During the electrochemical process in low-cost LiPF6/EC/DEC electrolyte, low-order polyselenide intermediates formed and were stabilized by mesoporous carbon, which avoided the shuttle reaction of polyselenides. Exceptional electrochemical performance of Se/mesoporous carbon composites was demonstrated in both Li-ion and Na-ion batteries. In lithium-ion batteries, Se8/mesoporous carbon composite cathodes delivered a reversible capacity of 480 mAh g(-1) for 1000 charge/discharge cycles without any capacity loss, while in Na-ion batteries, it provided initial capacity of 485 mAh g(-1) and retained 340 mAh g(-1) after 380 cycles. The Se8/mesoporous carbon composites also showed excellent rate capability. As the current density increased from 0.1 to 5 C, the capacity retained about 46% in Li-ion batteries and 34% in Na-ion batteries.
Nano-Sn/C composites are ideal anode materials for high energy and power density Li-ion batteries. However, because of the low melting point of Sn and the tendency of grain growth, especially during high temperature carbonization, it has been a significant challenge to create well-dispersed ultrasmall Sn nanoparticles within a carbon matrix. In this paper, we demonstrate an aerosol spray pyrolysis technique, as a facile and scalable method, to synthesize a nano-Sn/C composite with uniformly dispersed 10 nm nano-Sn within a spherical carbon matrix. The discharge capacity of nano-Sn/C composite sphere anodes maintains the initial capacity of 710 mAh/g after 130 cycles at 0.25 C. The nano-Sn/C composite sphere anodes can provide ~600 mAh/g even at a high rate of 20 C. To the best of our knowledge, such high rate performance for Sn anodes has not been reported previously. The exceptional performance of the nano-Sn/C composite is attributed to the unique nano-Sn/C structure: (1) carbon matrix offers mechanical support to accommodate the stress associated with the large volume change of nano-Sn, thus alleviating pulverization; (2) the carbon matrix prevents Sn nanoparticle agglomeration upon prolonged cycling; and (3) carbon network provides continuous path for Li ions and electrons inside the nano-Sn/C composite spheres.
Carbon-coated olivine NaFePO(4) (C-NaFePO(4)) spherical particles with a uniform diameter of ∼80 nm are obtained by chemical delithiation and subsequent electrochemical sodiation of carbon-coated olivine LiFePO(4) (C-LiFePO(4)), which is synthesized by a solvothermal method. The C-NaFePO(4) electrodes are identical (particle size, particle size distribution, surface coating, and active material loading, etc.) to C-LiFePO(4) except that Li ions in C-LiFePO(4) are replaced by Na ions, making them ideal for comparison of thermodynamics and kinetics between C-NaFePO(4) cathode in sodium-ion (Na-ion) batteries and C-LiFePO(4) in lithium-ion (Li-ion) batteries. In this paper, the equilibrium potentials, reaction resistances, and diffusion coefficient of Na in C-NaFePO(4) are systematically investigated by using the galvanostatic intermittent titration technique (GITT), electrochemical impedance spectroscopy (EIS) and cyclic voltammetry (CV), and compared to those of the well-known LiFePO(4) cathodes in Li-ion batteries. Due to the lower diffusion coefficient of Na-ion and higher contact and charge transfer resistances in NaFePO(4) cathodes, the rate performance of C-NaFePO(4) in Na-ion batteries is much worse than that of C-LiFePO(4) in Li-ion batteries. However, the cycling stability of C-NaFePO(4) is almost comparable to C-LiFePO(4) by retaining 90% of its capacity even after 100 charge-discharge cycles at a charge-discharge rate of 0.1 C.
Designed as a high-capacity alloy host for Na-ion chemistry, a forest of Sn nanorods with a unique core-shell structure was synthesized on viral scaffolds, which were genetically engineered to ensure a nearly vertical alignment upon self-assembly onto a metal substrate. The interdigital spaces thus formed between individual rods effectively accommodated the volume expansion and contraction of the alloy upon sodiation/desodiation, while additional carbon-coating engineered over these nanorods further suppressed Sn aggregation during extended electrochemical cycling. Due to the unique nanohierarchy of multiple functional layers, the resultant 3D nanoforest of C/Sn/Ni/TMV1cys, binder-free composite electrode already and evenly assembled on a stainless steel current collector, exhibited supreme capacity utilization and cycling stability toward Na-ion storage and release. An initial capacity of 722 mA·h (g Sn)(-1) along with 405 mA·h (g Sn)(-1) retained after 150 deep cycles demonstrates the longest-cycling nano-Sn anode material for Na-ion batteries reported in the literature to date and marks a significant performance improvement for neat Sn material as alloy host for Na-ion chemistry.
Highly stable sulfur/microporous carbon (S/MC) composites are prepared by vacuum infusion of sulfur vapor into microporous carbon at 600 °C, and lithium sulfide/microporous carbon (Li2S/MC) cathodes are fabricated via a novel and facile in situ lithiation strategy, i.e., spraying commercial stabilized lithium metal powder (SLMP) onto a prepared S/MC film cathode prior to the routine compressing process in cell assembly. The in situ formed Li2S/MC film cathode shows high Coulombic efficiency and long cycling stability in a conventional commercial Li-ion battery electrolyte (1.0 M LiPF6 + EC/DEC (1:1 v/v)). The reversible capacities of Li2S/MC cathodes remain about 650 mAh/g even after 900 charge/discharge cycles, and the Coulombic efficiency is close to 100% at a current density of 0.1C, which demonstrates the best electrochemical performance of Li2S/MC cathodes reported to date. Furthermore, this Li2S/MC film cathode fabricated via our in situ lithiation strategy can be coupled with a Li-free anode, such as graphite, carbon/tin alloys, or Si nanowires to form a rechargeable Li-ion cell. As the Li2S/MC cathode is paired with a commercial graphite anode, the full cell of Li2S/MC-graphite (Li2S-G) shows a stable capacity of around 600 mAh/g in 150 cycles. The Li2S/MC cathodes prepared by high-temperate sulfur infusion and SLMP prelithiation before cell assembly are ready to fit into current Li-ion batteries manufacturing processes and will pave the way to commercialize low-cost Li2S-G Li-ion batteries.
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