As one important component of sulfur cathodes, the carbon host plays a key role in the electrochemical performance of lithium‐sulfur (Li‐S) batteries. In this paper, a mesoporous nitrogen‐doped carbon (MPNC)‐sulfur nanocomposite is reported as a novel cathode for advanced Li‐S batteries. The nitrogen doping in the MPNC material can effectively promote chemical adsorption between sulfur atoms and oxygen functional groups on the carbon, as verified by X‐ray absorption near edge structure spectroscopy, and the mechanism by which nitrogen enables the behavior is further revealed by density functional theory calculations. Based on the advantages of the porous structure and nitrogen doping, the MPNC‐sulfur cathodes show excellent cycling stability (95% retention within 100 cycles) at a high current density of 0.7 mAh cm‐2 with a high sulfur loading (4.2 mg S cm‐2) and a sulfur content (70 wt%). A high areal capacity (≈3.3 mAh cm‐2) is demonstrated by using the novel cathode, which is crucial for the practical application of Li‐S batteries. It is believed that the important role of nitrogen doping promoted chemical adsorption can be extended for development of other high performance carbon‐sulfur composite cathodes for Li‐S batteries.
Silicon has attracted ever‐increasing attention as a high‐capacity anode material in Li‐ion batteries owing to its extremely high theoretical capacity. However, practical application of silicon anodes is seriously hindered by its fast capacity fading as a result of huge volume changes during the charge/discharge process. Here, an interpenetrated gel polymer binder for high‐performance silicon anodes is created through in‐situ crosslinking of water‐soluble poly(acrylic acid) (PAA) and polyvinyl alcohol (PVA) precursors. This gel polymer binder with deformable polymer network and strong adhesion on silicon particles can effectively accommodate the large volume change of silicon anodes upon lithiation/delithiation, leading to an excellent cycling stability and high Coulombic efficiency even at high current densities. Moreover, high areal capacity of ∼4.3 mAh/cm2 is achieved based on the silicon anode using the gel PAA–PVA polymer binder with a high mass loading. In view of simplicity in using the water soluble gel polymer binder, it is believed that this novel binder has a great potential to be used for high capacity silicon anodes in next generation Li‐ion batteries, as well as for other electrode materials with large volume change during cycling.
Despite the high theoretical capacity of lithium-sulfur batteries, their practical applications are severely hindered by a fast capacity decay, stemming from the dissolution and diffusion of lithium polysulfides in the electrolyte. A novel functional carbon composite (carbon-nanotube-interpenetrated mesoporous nitrogen-doped carbon spheres, MNCS/CNT), which can strongly adsorb lithium polysulfides, is now reported to act as a sulfur host. The nitrogen functional groups of this composite enable the effective trapping of lithium polysulfides on electroactive sites within the cathode, leading to a much improved electrochemical performance (1200 mAh g(-1) after 200 cycles). The enhancement in adsorption can be attributed to the chemical bonding of lithium ions by nitrogen functional groups in the MNCS/CNT framework. Furthermore, the micrometer-sized spherical structure of the material yields a high areal capacity (ca. 6 mAh cm(-2)) with a high sulfur loading of approximately 5 mg cm(-2), which is ideal for practical applications of the lithium-sulfur batteries.
Electroactive polymers are a new generation of "green" cathode materials for rechargeable lithium batteries. We have developed nanocomposites combining graphene with two promising polymer cathode materials, poly(anthraquinonyl sulfide) and polyimide, to improve their high-rate performance. The polymer-graphene nanocomposites were synthesized through a simple in situ polymerization in the presence of graphene sheets. The highly dispersed graphene sheets in the nanocomposite drastically enhanced the electronic conductivity and allowed the electrochemical activity of the polymer cathode to be efficiently utilized. This allows for ultrafast charging and discharging; the composite can deliver more than 100 mAh/g within just a few seconds.
In spite of recent progress, there is still a lack of reliable organic electrodes for Li storage with high comprehensive performance, especially in terms of long-term cycling stability. Herein, we report an ideal polymer electrode based on anthraquinone, namely, polyanthraquinone (PAQ), or specifically, poly(1,4-anthraquinone) (P14AQ) and poly(1,5-anthraquinone) (P15AQ). As a lithium-storage cathode, P14AQ showed exceptional performance, including reversible capacity almost equal to the theoretical value (260 mA h g(-1); >257 mA h g(-1) for AQ), a very small voltage gap between the charge and discharge curves (2.18-2.14=0.04 V), stable cycling performance (99.4% capacity retention after 1000 cycles), and fast-discharge/charge ability (release of 69% of the low-rate capacity or 64% of the energy in just 2 min). Exploration of the structure-performance relationship between P14AQ and related materials also provided us with deeper understanding for the design of organic electrodes.
Lithium-ion batteries suffer severe power loss at temperatures below zero degrees Celsius, limiting their use in applications such as electric cars in cold climates and high-altitude drones. The practical consequences of such power loss are the need for larger, more expensive battery packs to perform engine cold cranking, slow charging in cold weather, restricted regenerative braking, and reduction of vehicle cruise range by as much as 40 per cent. Previous attempts to improve the low-temperature performance of lithium-ion batteries have focused on developing additives to improve the low-temperature behaviour of electrolytes, and on externally heating and insulating the cells. Here we report a lithium-ion battery structure, the 'all-climate battery' cell, that heats itself up from below zero degrees Celsius without requiring external heating devices or electrolyte additives. The self-heating mechanism creates an electrochemical interface that is favourable for high discharge/charge power. We show that the internal warm-up of such a cell to zero degrees Celsius occurs within 20 seconds at minus 20 degrees Celsius and within 30 seconds at minus 30 degrees Celsius, consuming only 3.8 per cent and 5.5 per cent of cell capacity, respectively. The self-heated all-climate battery cell yields a discharge/regeneration power of 1,061/1,425 watts per kilogram at a 50 per cent state of charge and at minus 30 degrees Celsius, delivering 6.4-12.3 times the power of state-of-the-art lithium-ion cells. We expect the all-climate battery to enable engine stop-start technology capable of saving 5-10 per cent of the fuel for 80 million new vehicles manufactured every year. Given that only a small fraction of the battery energy is used for self-heating, we envisage that the all-climate battery cell may also prove useful for plug-in electric vehicles, robotics and space exploration applications.
Lithium-sulfur (Li-S) batteries offer theoretical energy density much higher than that of lithium-ion batteries, but their development faces significant challenges. Mesoporous carbon-sulfur composite microspheres are successfully synthesized by combining emulsion polymerization and the evaporation-induced self-assembly (EISA) process. Such materials not only exhibit high sulfur-specific capacity and excellent retention as Li-S cathodes but also afford much improved tap density, sulfur content, and areal capacity necessary for practical development of high-energy-density Li-S batteries. In addition, when incorporated with carbon nanotubes (CNTs) to form mesoporous carbon-CNT-sulfur composite microspheres, the material demonstrated superb battery performance even at a high current density of 2.8 mA/cm(2), with a reversible capacity over 700 mAh/g after 200 cycles.
Despite the high theoretical capacity of lithiumsulfur batteries,t heir practical applications are severely hindered by afast capacity decay, stemming from the dissolution and diffusion of lithium polysulfides in the electrolyte.Anovel functional carbon composite (carbon-nanotube-interpenetrated mesoporous nitrogen-doped carbon spheres,M NCS/ CNT), whichc an strongly adsorb lithium polysulfides,i sn ow reported to act as asulfur host. The nitrogen functional groups of this composite enable the effective trapping of lithium polysulfides on electroactive sites within the cathode,leading to amuchimproved electrochemical performance (1200 mAh g À1 after 200 cycles). The enhancement in adsorption can be attributed to the chemical bonding of lithium ions by nitrogen functional groups in the MNCS/CNT framework. Furthermore,t he micrometer-sized spherical structure of the material yields ahigh areal capacity (ca. 6mAh cm À2 )with ahigh sulfur loading of approximately 5mgcm À2 ,w hich is ideal for practical applications of the lithium-sulfur batteries.
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