Abstract Lithium–sulfur batteries are regarded as one of the most promising candidates for next‐generation rechargeable batteries. However, the practical application of lithium–sulfur (Li–S) batteries is seriously impeded by the notorious shuttling of soluble polysulfide intermediates, inducing a low utilization of active materials, severe self‐discharge, and thus a poor cycling life, which is particularly severe in high‐sulfur‐loading cathodes. Herein, a polysulfide‐immobilizing polymer is reported to address the shuttling issues. A natural polymer of Gum Arabic (GA) with precise oxygen‐containing functional groups that can induce a strong binding interaction toward lithium polysulfides is deposited onto a conductive support of a carbon nanofiber (CNF) film as a polysulfide shielding interlayer. The as‐obtained CNF–GA composite interlayer can achieve an outstanding performance of a high specific capacity of 880 mA h g −1 and a maintained specific capacity of 827 mA h g −1 after 250 cycles under a sulfur loading of 1.1 mg cm −2 . More importantly, high reversible areal capacities of 4.77 and 10.8 mA h cm −2 can be obtained at high sulfur loadings of 6 and even 12 mg cm −2 , respectively. The results offer a facile and promising approach to develop viable lithium–sulfur batteries with high sulfur loading and high reversible capacities.
Potassium (K) metal is a promising anode for potential low-cost and high-energy-density K-ion batteries. However, its application is hampered by serious dendrite growth and large volume change. Herein, a Co nanoparticle-embedded nitrogen-doped nanoporous carbon nanofiber paper is prepared by carbonizing the electrospun fiber paper of metal–organic framework (MOF) nanoparticles and polyacrylonitrile, which displays a high potassiophilicity due to the incorporation of Co nanoparticles and N doping. As a three-dimensional host, excellent electrochemical performance is demonstrated for the K metal anode with a high average Coulombic efficiency of 98.75% for 400 cycles and a long lifespan of 1300 h in symmetric cells. Furthermore, enhanced electrochemical performance with good cycling stability and rate capability is achieved in full cells that are paired with organic cathodes. Our findings highlight a promising strategy for fabricating high-performance K metal anodes using MOF-based materials.
Potassium–metal batteries are attractive candidates for low-cost and large-scale energy storage systems due to the abundance of potassium. However, K metal dendrite growth as well as volume expansion of K metal anodes on cycling have significantly hindered its practical applications. Although enhanced performance has been reported using carbon hosts with complicated structure engineering, they are not suitable for mass production. Herein, a highly potassiophilic carbon nanofiber paper with abundant oxygen-containing functional groups on the surface and a 3D interconnected network architecture is fabricated through a facile, scalable, and environmental-friendly biosynthesis method. As a host for K metal anode, uniform K nucleation and stable plating/stripping performance are demonstrated, with a stable cycling of 1400 h and a low overpotential of 45 mV, which are much better than all carbon hosts without complicated structure engineering. Moreover, full cells pairing the carbon nanofiber paper/K composite anodes with K4Fe(CN)6 cathodes exhibit excellent cycle stability and rate capability. The results provide a promising way for realizing dendrite-free K metal anodes and high-performance potassium–ion batteries.
Organic electrode materials free of rare transition metal elements are promising for sustainable, cost-effective, and environmentally benign battery chemistries. However, severe shuttling effect caused by the dissolution of active materials in liquid electrolytes results in fast capacity decay, limiting their practical applications. Here, using a gel polymer electrolyte (GPE) that is in situ formed on Nafion-coated separators, the shuttle reaction of organic electrodes is eliminated while maintaining the electrochemical performance. The synergy of physical confinement by GPE with tunable polymer structure and charge repulsion of the Nafion-coated separator substantially prevents the soluble organic electrode materials with different molecular sizes from shuttling. A soluble small-molecule organic electrode material of 1,3,5-tri(9,10-anthraquinonyl)benzene demonstrates exceptional electrochemical performance with an ultra-long cycle life of 10 000 cycles, excellent rate capability of 203 mAh g-1 at 100 C, and a wide working temperature range from -70 to 100 °C based on the solid-liquid conversion chemistry, which outperforms all previously reported organic cathode materials. The shielding capability of GPE can be designed and tailored toward organic electrodes with different molecular sizes, thus providing a universal resolution to the shuttling effect that all soluble electrode materials suffer.
A porous N-doped carbon-coated manganese oxide/zinc manganate (MZM@N-C) composite was successfully prepared as advanced cathode material for aqueous ZIBs.
Lithium (Li) metal is regarded as an ideal anode for the next-generation high-energy-density Li-ion batteries. However, its practical application has been seriously hindered by the dendrite growth and volume change during charge/discharge cycling. Herein, a three-dimensional (3D) hollow carbon tube (HCT) mat is fabricated from natural willow catkins to form HCT/Li composite through a scalable molten infusion method. The intrinsic heteroatoms endow the HCTs with excellent lithiophilicity, and molten Li can be impregnated into the 3D HCT mat easily via capillary driving force. As a result, a uniform Li plating/stripping and stable Li composite anode were demonstrated, delivering 500 stable cycles at 2 mA cm–2. Furthermore, a full cell using a commercial lithium iron phosphate cathode achieves excellent cycling stability above 250 cycles at a high rate of 5 C (1 C = 170 mAh g–1). This work sheds light on a facile and practical method to construct a stable Li metal anode for remarkable Li metal rechargeable batteries.
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