The development of efficient and affordable electrode materials is key to the construction of clean energy storage systems. Transition-metal chalcogenophosphates (TMPX₃, where TM represents Ni, Fe, Zn, V, Mn, Co, etc., and X denotes S, Se, or Te) are a promising class of two-dimensional (2D) layered materials with great potential for energy storage, photoelectrocatalysis, and electronic devices due to their unique electronic structure and tunable bandgap. In this review, we systematically summarise the latest research progress on TMPX₃ materials, adopting a pioneering multidimensional analysis framework to overcome the limitations of a unified single perspective. Firstly, we reveal the mechanisms of P–S bond anisotropy and TM coordination on the energy band structure from the atomic scale; secondly, through the comparative analysis of the existing preparation methods and regulation strategies, the optimised pathways for precise control of the number of layers and large-scale production are proposed. On this basis, we focus on the applications of TMPX₃ in photoelectrocatalysis and metal batteries, and elucidate the cross-scale correlation mechanism between its electronic/interfacial properties and macroscopic performance. Finally, the challenges and future opportunities of the material are presented, with the aim of providing valuable insights into the multi-field, precisely coupled design and energy storage applications of TMPX₃ materials.

The leakage of liquid electrolyte and the formation of lithium dendrites pose challenges to safety and stability of lithium metal batteries (LMBs). The appearance of gel polymer electrolyte (GPE) has obviously improved the safety of traditional LMBs. However, the limited inhibition of GPE on lithium dendrites is detrimental to the safety of LMBs. Herein, a kind of poly (vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)/gelatin (GN) GPE with high ionic conductivity, high-temperature resistance, and flame-retardancy, was prepared by electrospinning and soaking method. Utilizing the electrospinning network of PVDF-HFP, its affinity to liquid electrolytes, makes this GPE more beneficial to ions transport and the formation of gel. And, the GN with sol–gel properties, enhances the mechanical property (13.5 MPa) of HFP-GN GPE. Meanwhile, X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) suggest that the attraction of polar groups of GN to Li⁺ can regulate the distribution of Li⁺ and protect Li anodes. Consequently, the application of HFP-GN GPEs to LMBs with cathodes of LiFePO₄ and LiCoO₂ deliver excellent electrochemical performances: after 300 cycles, the LiFePO₄/HFP-GN GPE/Li battery keeps a low capacity decay rate of 0.09% at 5 C; after 400 cycles at 2 C, the LiCoO₂/HFP-GN GPE/Li cell retains a high capacity retention of 74%. This GPE is demonstrated for the application prospect of safe LMBs.

Proper regulation of metal-nitrogen carbon (M-N-C) materials derived from zeolitic imidazolate frameworks (ZIFs) is essential to enhance the oxygen reduction reaction (ORR) performance. However, most of the reports focus on the component regulation, and the structure regulation of ZIFs-derived M-N-C materials by a simple preparation method has been barely reported. Herein, using a one-step electrospinning method with subsequent pyrolysis, we have prepared a bead-like cobalt-nitrogen co-doped carbon nanocage/carbon nanofiber (Co-N-C/CNF) composite electrocatalyst with the porous carbon nanocages arranged one by one in the highly conductive carbon nanofibers. Profiting from the fully exposed active sites and improved conductivity, the Co-N-C/CNF catalyst exhibits an excellent ORR performance even surpassing the commercial Pt/C catalyst. Density functional theory (DFT) results demonstrate that the Co_NP-N₁-C₂ active sites on Co-N-C/CNF make the core contribution to the improvement of ORR properties. Moreover, the zinc-air battery (ZAB) based on the Co-N-C/CNF catalyst also shows outstanding discharge performance. This study provides a new strategy for the preparation and structural design for ZIFs-derived M-N-C materials as efficient ORR catalysts.

Harvesting solar energy to drive the semiconductor photocatalysis offers a promising tactic to address ever-growing challenges of both energy shortage and environmental pollution. Design and synthesis of nano-heterostructure photocatalysts with controllable components and morphologies are the key factors for achieving highly efficient photocatalytic processes. One-dimensional (1D) semiconductor nanofibers produced by electrospinning possess a large ratio of length to diameter, high ratio of surface to volume, small grain sizes, and high porosity, which are ideally suited for photocatalytic reactions from the viewpoint of structure advantage. After the secondary treatment of these nanofibers through the solvothermal, gas reduction, in situ doping, or assembly methods, the multi-component nanofibers with hierarchical nano-heterostructures can be obtained to further enhance their light absorption and charge carrier separation during the photocatalytic processes. In recent years, the electrospun semiconductor-based nano-heterostructures have become a “hot topic” in the fields of photocatalytic energy conversion and environmental remediation. This review article summarizes the recent progress in electrospinning synthesis of various kinds of high-performance semiconductor-based nano-heterostructure photocatalysts for H₂ production, CO₂ reduction, and decomposition of pollutants. The future perspectives of these materials are also discussed.

Li-S batteries are considered as a highly promising candidate for the next-generation energy storage system, attributing to their tremendous energy density. However, the two-dimensional island nucleation-growth process of lithium sulfide leads to a thick insulating film covering the electrode, inducing slow electrons transfer and mass-transfer of ions and liquid sulfur species in working Li-S cells. Here, we demonstrate a bio-inspired strategy of constructing ant-nest-like hierarchical porous ultrathin carbon nanosheet networks with the implants of metallic nanoparticles electrocatalysts (HPC-MEC) as efficient nanoreactors enabling rapid mass transfer, via a simple and green NaCl template. Such nanoreactors with a large active surface area could effectively anchor polysulfides for mitigating the shuttle effect, facilitating uniformly thin Li₂S film, and promoting the mass transfer for fast sulfur species conversions. This helps contribute to a continuously high sulfur utilization in Li-S batteries with the HPC-MEC reactors. As a typical exhibition, cobalt embedded hierarchical porous carbon (HPC-Co) could realize to deliver a remarkably high specific capacity of 1, 540.6 mAh·g^-1, an excellent rate performance of 878.8 mAh·g^-1 at 2 C, and high area capacity of 11.6 mAh·cm^-2 at a high sulfur load of 10 mg·cm^-2 and low electrolyte/sulfur ratio of 5 μL·mg^-1.