RESUMEN
The sluggish reaction kinetics at the cathode/electrolyte interface of lithium-sulfur (Li-S) batteries limits their commercialization. Herein, we show that a dual-regulation system of iron phthalocyanine (FePc) and octafluoronaphthalene (OFN) decorated on graphene (Gh), denoted as Gh/FePc+OFN, accelerates the interfacial reaction kinetics of lithium polysulfides (LiPSs). Multiple in situ spectroscopy techniques and ex situ X-ray photoelectron spectroscopy combined with density functional theory calculations demonstrate that FePc acts as an efficient anchor and scissor for the LiPSs through Fe···S coordination, mainly facilitating their liquid-liquid transformation, whereas OFN enables Li-bond interaction with the LiPSs, accelerating the kinetics of the liquid-solid nucleation and growth of Li2S. This dual-regulation system promotes the smooth conversion reaction of sulfur, thereby improving the battery performance. A Gh/FePc+OFN-based Li-S cathode delivered an ultrahigh initial capacity of 1604 mAh g-1 at 0.2 C, with an ultralow capacity decay rate of 0.055% per cycle at 1 C over 1000 cycles.
RESUMEN
Lithium-sulfur (Li-S) batteries are receiving intense interest owing to their high energy densities, cost effectiveness, and the natural abundance of sulfur. However, practical applications are still limited by rapid capacity decay caused by multielectron redox reactions and complex phase transformations. Here, we include commercially available titanium silicalite-1 (TS-1) in carbon/sulfur cathodes, to introduce strong chemical interactions between the lithium polysulfides (LiPS) and TS-1 in a working Li-S battery. In situ UV-visible spectroscopy together with other experimental results confirm that incorporation of TS-1 mediators enables direct conversion between S82- and S3*- radicals during the discharge process, which effectively promotes the kinetic behaviors of soluble LiPS and regulates uniform nucleation and growth of solid sulfide precipitates. These features give our TS-1 engineered sulfur cathode an ultrahigh initial capacity of 1459 mA h g-1 at 0.1C. Moreover, the system has an impressively high areal capacity (3.84 mA h cm-2) and long cycling stability with a high sulfur loading of 4.9 mg cm-2. This novel and low-cost fabrication procedure is readily scalable and provides a promising avenue for potential industrial applications.
RESUMEN
The complicated reactions at the cathode-electrolyte interface in Li-S batteries are a large barrier for their successful commercialization. Herein, we developed a molecular design strategy and employed three small molecules acting as interfacial mediators to the cathodes of Li-S batteries. The theoretical calculation results show that the incorporation of tris(4-fluorophenyl)phosphine (TFPP) has a strong binding performance. The experimental results demonstrate that the strong chemical interactions between polysulfides and the F, P atoms in TFPP not only modify the kinetics of the electrochemical processes in the electrolyte but also promote the formation of short-chain clusters (Li2Sx, x = 1, 2, 3, and 4) at the interface during the charge-discharge process. As a result, an optimized electrode exhibits a low capacity decay rate of 0.042% per cycle when the current rate is increased to 5 C over 1000 cycles.
RESUMEN
Water splitting is considered to be a very promising alternative to greenly produce hydrogen, and the key to optimizing this process is the development of suitable electrocatalysts. Here, a sacrificial-counter-electrode method to synthesize a MoS x /carbon nanotubes/Pt catalyst (0.55 wt% Pt loading) is developed, which exhibits a low overpotential of 25 mV at a current density of 10 mA cm-2, a low Tafel slope of 27 mV dec-1, and excellent stability under acidic conditions. The theory calculations and experimental results confirm the high hydrogen evolution activity that is likely due to the fact that the S atoms in MoS x can be substituted with O atoms during a potential cycling process when using Pt as a counter-electrode, where the O atoms act as bridges between the catalytic PtO x particles and the MoS x support to generate a MoS x -O-PtO x structure, allowing the Pt atoms to donate more electrons thus facilitating the hydrogen evolution reaction process.