Several critical issues, such as the shuttling effect and the sluggish reaction kinetics, exist in the design of high‐performance lithium–sulfur (Li‐S) batteries. Here, it is reported that nitrogen doping can simultaneously and significantly improve both the immobilization and catalyzation effects of Co9S8 nanoparticles in Li‐S batteries. Combining the theoretical calculations with experimental investigations, it is revealed that nitrogen atoms can increase the binding energies between LiPSs and Co9S8, and as well as alleviate the sluggish kinetics of Li‐S chemistry in the Li2S6 cathode. The same effects are also observed when adding N‐Co9S8 nanoparticles into the commercial Li2S cathode (which has various intrinsic advantages, but unfortunately a high overpotential). A remarkable improvement in the battery performances in both cases is observed. The work brings heteroatom‐doped Co9S8 to the attention of designing high‐performance Li‐S batteries. A fundamental understanding of the inhibition of LiPSs shuttle and the catalytic effect of Li2S in the newly developed system may encourage more effort along this interesting direction.
Lithium-sulfur (Li-S) batteries have attracted widespread attention due to their high theoretical energy density. However, their practical application is still hindered by the shuttle effect and the sluggish conversion of lithium polysulfides (LiPSs). Herein, monodisperse molybdenum (Mo) nanoparticles embedded onto nitrogen-doped graphene (Mo@N-G) were developed and used as a highly efficient electrocatalyst to enhance LiPS conversion. The weight ratio of the electrocatalyst in the catalyst/sulfur cathode is only 9%. The unfilled d orbitals of oxidized Mo can attract the electrons of LiPS anions and form Mo–S bonds during the electrochemical process, thus facilitating fast conversion of LiPSs. Li-S batteries based on the Mo@N-G/S cathode can exhibit excellent rate performance, large capacity, and superior cycling stability. Moreover, Mo@N-G also plays an important role in room-temperature quasi-solid-state Li-S batteries. These interesting findings suggest the great potential of Mo nanoparticles in building high-performance Li-S batteries.
To unlock the great potential of lithium metal anodes for high‐performance batteries, a number of critical challenges must be addressed. The uncontrolled dendrite growth and volume changes during cycling (especially, at high rates) will lead to short lifespan, low Coulombic efficiency (CE), and security risks of the batteries. Here it is reported that Li metal anodes, employing the monodisperse, lithiophilic, robust, and large‐cavity N‐doped hollow carbon nanospheres (NHCNSs) as the host, show remarkable performances—high areal capacity (10 mAh cm−2), high CE (up to 99.25% over 500 cycles), complete suppression of dendrite growth, dense packing of Li anode, and an extremely smooth electrode surface during repeated Li plating/stripping. In symmetric cells, a highly stable voltage hysteresis over a long cycling life >1200 h is achieved, and a low and stable voltage hysteresis can be realized even at an ultrahigh current density of 64 mA cm−2. Furthermore, the NHCNSs‐based anodes, when paired with a LiFePO4 (LFP) cathode in full cells, give rise to highly improved rate capability (104 mAh g−1 at 10 C) and cycling stability (91.4% capacity retention for 200 cycles), enabling a promising candidate for the next‐generation high energy/power density batteries.
Room-temperature sodium-sulfur (RT Na-S) batteries are arousing great interest in recent years. Their practical applications, however, are hindered by several intrinsic problems, such as the sluggish kinetic, shuttle effect, and the incomplete conversion of sodium polysulfides (NaPSs). Here a sulfur host material that is based on tungsten nanoparticles embedded in nitrogen-doped graphene is reported. The incorporation of tungsten nanoparticles significantly accelerates the polysulfides conversion (especially the reduction of Na 2 S 4 to Na 2 S, which contributes to 75% of the full capacity) and completely suppresses the shuttle effect, en route to a fully reversible reaction of NaPSs. With a host weight ratio of only 9.1% (about 3-6 times lower than that in recent reports), the cathode shows unprecedented electrochemical performances even at high sulfur mass loadings. The experimental findings, which are corroborated by the first-principles calculations, highlight the so far unexplored role of tungsten nanoparticles in sulfur hosts, thus pointing to a viable route toward stable Na-S batteries at room temperatures.
Lithium-sulfur (Li-S) batteries, as part of the post-lithium-ion batteries (post-LIBs), are expected to deliver significantly higher energy densities. Their power densities, however, are today considerably worse than that of the LIBs, limiting the Li-S batteries to very few specific applications that need low power and long working time. With the rapid development of single cell components (cathode, anode, or electrolyte) in the last few years, it is expected that an integrated approach can maximize the power density without compromising the energy density in a Li-S full cell. Here, this goal is achieved by using a novel biomass porous carbon matrix (PCM) in the anode, as well as N-Co 9 S 8 nanoparticles and carbon nanotubes (CNTs) in the cathode. The authors' approach unlocks the potential of the electrodes and enables the Li-S full pouch cells with unprecedented power densities and energy densities (325 Wh kg −1 and 1412 W kg −1 , respectively). This work addresses the problem of low power densities in the current Li-S technology, thus making the Li-S batteries a strong candidate in more application scenarios.
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