Photocatalytic oxidation of methane to value-added chemicals is a promising process under mild conditions, nevertheless confronting great challenges in efficiently activating C–H bonds and inhibiting over-oxidation. Herein, we propose a comprehensive strategy for the selective generation of reactive oxygen species (ROS) by regulating the sizes and facets of Au nanoparticles loaded on ZnO. For photocatalytic methane oxidation at ambient temperature, a high oxygenates yield of 36.4 mmol·g⁻¹·h⁻¹ with a nearly 100% selectivity has been achieved over the optimized 1.0% Au/ZnO-9.6 (1% Au with (111) facet and 9.6 nm size on ZnO) photocatalyst, exceeding most reported literatures. Mechanism investigations reveal that 1.0% Au/ZnO-9.6 with the medium size and Au (111) facet guarantees the favourable formation of superoxide radicals (·OOH) through mild oxygen reduction, ultimately leading to excellent photocatalytic methane oxidation performance. This work provides some guidance for the delicate design of photocatalysts for efficient photocatalytic methane oxidation and oxygen utilization.

The commercialization of lithium-sulfur (Li-S) batteries faces several bottlenecks, and the major two of which are the shuttle effect of polysulfides and the wild growth of Li dendrites, responsible for fast capacity decay and severe safety issues. As an essential component of Li-S batteries, the structure and properties of the separators are closely related to the above problems, and the exploration of multifunctional separators is highly sought-after. Herein, an integrated separator composited of defective graphene and polyimide (DG-PI) was innovatively fabricated by electrospinning combined with the laser-induced carbonization strategy. The all-in-one compact architecture with well-interconnected channels shows superior mechanical and thermal stability and wettability. More importantly, the PI nanofibers containing N–/O– functional groups can induce the uniform deposition of lithium on the anode surface, while the DG framework with abundant pentagonal/heptagonal rings and vacancies can strongly trap polysulfides and accelerate polysulfide transformation on the cathode side. The strong chemical interaction between the insulative PI layer and the conductive DG layer modulates the surface charge distribution of each other, leading to more prominent contributions to restraining lithium dendrites and shuttle effect. Therefore, the Li-S batteries based on the integrated DG-PI separators afford an excellent performance in protecting lithium anode (stable cycles of 200 h at 5 mA·cm⁻²) and good cycling stability with a low capacity decay of 0.05% per cycle after 700 cycles at 1 C. This work offers a new design concept of multifunctional Li-S battery separators and broadens the application scope of laser micro-nano fabrication technology.

The performance of lithium-sulfur battery is restricted by the lower value of electrode conductance and the sluggish LiPSs degradation kinetics. Unfortunately, the degradation rate of polysulfides was mostly attributed to the catalytic energy barrier in previous, which is unable to give accurate predictions on the performance of lithium-sulfur battery. Thereby, a quantitative framework relating the battery performance to catalytic energy barrier and electrical conductivity of the cathode host is developed here to quantitate the tendency. As the model compound, calculated-Ti₄O₇ (c-Ti₄O₇) has the highest comprehensive index with excellent electrical conductivity, although the catalytic energy barrier is not ideal. Through inputting the experimental properties such as impedance and charge/discharge data into the as-build model, the final conclusion is still in line with our prediction that Ti₄O₇ host shows the most excellent electrochemical performance. Therefore, the accurate model here would be attainable to design lithium-sulfur cathode materials with a bottom–up manner.

Carbonaceous materials represent the dominant choice of materials for anodic lithium storage in many energy storage devices. Nevertheless, the nonpolar carbonaceous materials offer weak adsorption toward Li⁺ that largely denies the high-rate Li⁺ storage. Herein, the atomic Fe sites decorated carbon nanofibers (AICNFs) facilely produced by electrospinning are reported for kinetically accelerated Li⁺ storage. Theoretical calculation reveals that the atomic Fe sites possess coordination unsaturated electronic configuration, enabling suitable bonding energy and facilitated diffusion path of Li⁺. As a result, the optimal structure displays a high capacitive contribution up to 95.9% at a scan rate of 2.0 mV·s⁻¹. In addition, ultrahigh capacity retention of 97% is afforded after 5,000 cycles at a current density of 3 A·g⁻¹. Moreover, the interlaced fiber structure enabled by electrospinning benefits structural stability and improved conductivity even at thick electrodes, thus allowing a high areal capacity of 1.76 mAh·cm⁻² at a loading of 8 mg·cm⁻². Because of these structure and performance merits, the lithium-ion capacitor containing the AICNF-based anode delivers a high energy density and large power density.