Efficient hydrogen (H ₂ ) generation from electrochemical overall water splitting (OWS) is key to a sustainable H ₂ economy. Low‐cost transition metal‐based catalysts, such as Ni‐ and Co‐based phosphides, have gained attention for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) due to their excellent corrosion resistance and high electrical conductivity. In particular, bimetallic Ni and Co‐based phosphide catalysts are considered highly efficient electrocatalysts for OWS due to their abundant adsorption sites and low adsorption energy for hydrogen species. However, improving their stability and activity remains challenging. Herein, a Ce doping NiCo phosphide catalyst is presented with vary Ce amount (Ce _x ‐NiCoP) supported on nickel foam (NF) with multi‐site functionality, achieving highly efficient HER performance comparable to benchmark platinum catalysts support carbon fiber or NF (Pt/C or Pt/NF). Comprehensive characterization results show that the optimal amount of Ce doping significantly influences the electronic structure of the catalyst, preventing the formation of Ni ₅ P ₄ and CeO ₂ , promoting the dominant NiCoP phase. This modification enhances the catalyst's hydrophilicity, improving the HER activity significantly. Remarkably, the catalyst also demonstrates exceptional OER performance, making it a highly active and stable bifunctional catalyst for OWS, with the highest energy efficiency of 96.7%.

Carbon aerogels synthesized via the polymerization of resorcinol (R) and formaldehyde (F) exhibit remarkable physiochemical properties, such as high thermal stability and excellent electrical conductivity. However, their limited specific surface area and porosity restrict their application potential. Herein, we developed hierarchical porous carbon aerogels using a one-step carbonization and activation method, directly converting the resin into carbon aerogel material by adding KOH as an activating agent. In contrast to conventional carbon aerogels with an irregular block ground structure, our hierarchical porous carbon aerogels exhibit substantially enhanced specific surface area, total pore volume, and surface oxygen content. In addition, this straightforward one-step fabrication approach holds significant promise for energy storage applications. Notably, the hierarchical porous carbon aerogel C1, with a KOH/RF mass ratio of 1, was proven to be the most effective electrode candidates, achieving a specific capacitance of 261.9 F·g⁻¹ at 1 A·g⁻¹ and 208.2 F·g⁻¹ at 20 A·g⁻¹. Moreover, it exhibited an outstanding rate capability of 79.5% and excellent capacity retention of approximately 97.5% after 10,000 cycles (7 A·g⁻¹). This work highlights a promising approach for synthesizing commercial-grade carbon aerogels with hierarchical porosity, enabling high-performance energy storage applications.

Developing efficient, low‐cost electrocatalysts for overall water splitting (OWS) is critical for advancing hydrogen energy technologies. Here, we fabricate Mo‐incorporated N‐rich‐CoMoCN electrocatalyst from ZIF‐67 (CoCN material), ammonium molybdate, and melamine precursors. This catalyst, featuring the predominant Co/Co ₆ Mo ₆ C ₂ heterojunction and abundant surface‐layered architecture, collectively provides an ideal microenvironment for catalytic reactions and facilitates charge transfer. In alkaline media, it exhibits outstanding bifunctional activity, delivering overpotentials of only 107 and 256 mV for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), respectively, at a current density of 10 mA cm ⁻² , far surpassing the performance of CoCN and CoMoCN. Notably, the N‐rich‐CoMoCN‐based electrolyzer requires only 1.52 V to achieve 10 mA cm ⁻² in a two‐electrode system with 1.0 M KOH. The comprehensive structural and electrochemical characterizations reveal that the incorporation of Mo and N modulates the catalyst's morphology as well as lattice and electronic configurations, resulting in the strong electronic interaction between Co, Mo, and N, thereby accelerating the intrinsic reaction kinetics. Density functional theory (DFT) calculation further uncovers that N enrichment can effectively modulate the electronic state distribution of Co and Mo, thereby promoting interfacial charge rearrangement and regulating the d ‐band center of the catalyst. The synergistic effect between heterostructure construction and N enrichment optimizes the electronic structure and surface energy of the N‐rich‐CoMoCN catalyst, which facilitates charge transfer, ultimately leading to enhanced electrocatalytic activity in OWS performance. This work highlights an efficient strategy for designing high‐performance bifunctional catalysts from MOF‐derived heterostructures for sustainable hydrogen production.

Traditional oxidative dehydrogenation of n-butene has typically required relatively high operating temperatures (400–500 °C), which has driven increasing interest in the development of catalysts capable of delivering high activity at lower temperatures. In this study, zinc ferrite (ZnFe₂O₄-ST) was successfully synthesized via hydrothermal hydrolysis of Zn–Fe oleate and demonstrated remarkable catalytic performance for the oxidative dehydrogenation of n-butene under mild conditions. At 300 °C, ZnFe₂O₄-ST achieved a conversion of 72.9% with 92.1% selectivity toward 1,3-butadiene, a result that, to the best of our knowledge, ranks among the best reported in the literature. By contrast, ZnFe₂O₄ prepared by conventional coprecipitation (17.2% conversion with 91.3% selectivity) and sol-gel (10.1% conversion with 86.4% selectivity) methods showed much lower activities, highlighting the critical influence of synthesis strategy on catalytic performance. To better understand the origin of these differences, a detailed structural and physicochemical characterization was undertaken using X-ray diffraction (XRD), thermogravimetric analysis (TGA), transmission electron microscopy (TEM), N₂ adsorption–desorption, X-ray photoelectron spectroscopy (XPS), H₂-temperature-programmed reduction (H₂-TPR), temperature-programmed re-oxidation (TPRO), and NH₃-temperature-programmed desorption (NH₃-TPD). These analyses revealed that the as-synthesized ZnFe₂O₄-ST possessed a significantly smaller average particle size, a larger specific surface area, and superior reducibility compared with the other samples. These properties are believed to be the key factors underpinning its outstanding catalytic behavior and provide important insights into the design of efficient low-temperature catalysts for selective oxidative dehydrogenation.