To overcome the shuttle effect in Li–S batteries, novel biomimetic molecule catalysts are synthesized by grafting hemin molecules to three functionalized carbon nanotube systems (CNTs–COOH, CNTs–OH, and CNTs–NH2). The Li–S battery using the CNTs–COOH@hemin cathode exhibits the optimal initial specific capacity (1637.8 mAh g−1) and cycle durability (up to 1800 cycles). Various in situ characterization techniques, such as Raman spectroscopy, Fourier‐transform infrared reflection absorption spectroscopy, and UV–vis spectroscopy, combined with density functional theory computations are used to investigate the structure–reactivity correlation and the working mechanism in the Li–S system. It is demonstrated that the unique structure of the CNTs‐COOH@hemin composite with good conductivity and adequate active sites resulting from molecule catalyst as well as the strong absorption to polysulfides entrapped by the coordinated Fe(III) complex with FeO bond enables the homogeneous dispersion of S, facilitates the catalysis and conversion of polysulfides, and improves the battery's performance.

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.

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 (Li2S x , 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.

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.

Lithium–sulfur (Li–S) batteries are receiving intense interest owing to their high energy densities, cost effectiveness, and the natural abundance of sulfur.