The efficient hydrogenation of 1-butene is an industrially significant reaction for producing fuels and value-added chemicals. However, achieving high catalytic efficiency and stability remains challenging, particularly for cost-effective materials, such as Ni. In this study, we developed a porous Ni-coated Ni foam catalyst by electrostatic spray deposition to address these challenges. The catalyst exhibited a turnover frequency approximately 10 times higher than that of either porous Ni or Ni foam alone. This enhancement was attributed to the formation of interfacial active sites, which facilitated improved reactant adsorption and activation during hydrogenation. The electrostatic spray deposition technique ensured a uniform and controlled coating, enabling precise engineering of the catalyst structure and interface. The post-deposition heat treatment was further optimized to enhance structural integrity and catalytic performance. This study highlights the importance of interface engineering and structural optimization in catalyst design and provides valuable insights into the development of efficient Ni-based catalysts for industrial hydrogenation applications. These findings emphasize the potential of electrostatic spray deposition as a versatile method for fabricating advanced catalytic systems.

Molybdenum oxide catalysts have been widely investigated as cost‐effective electrocatalysts for water electrocatalysis due to their easily tunable electronic structures. However, their oxygen evolution reaction (OER) activities remain limited by their low electrical conductivities and electronically inactive oxidation states, thereby prompting the development of various alternative strategies. Herein, Fe‐substituted MoO _x catalysts with controlled lattice distortion and oxygen vacancy concentrations are proposed. Fe‐substituted MoO _x is synthesized via aerosol spray pyrolysis and subsequent postannealing to control its interfacial properties. Fe substitution induces spatial segregation from Mo, leading to the formation of a yolk–shell structure that exposes abundant active sites. Furthermore, Mo orbital hybridization improves the electronic structure and greatly enhances electrical conductivity. The optimized yolk–shell‐structured FeMoO _x catalyst exhibits excellent performance at a high current density of 100 mA cm ⁻² , delivering a low overpotential of 294 mV and maintaining stable performance over 100 h. In situ electrochemical analyses reveal that temperature control of the charge distribution enhances oxygen intermediate adsorption and promotes OO bond formation through lattice oxygen species, thereby activating the lattice oxygen mechanism. This study provides mechanistic insights and a practical design strategy toward developing cost‐effective, high‐performance OER electrocatalysts based on transition‐metal‐modified molybdenum oxides.

The efficient hydrogenation of 1-butene is an industrially significant reaction for producing fuels and value-added chemicals. However, achieving high catalytic efficiency and stability remains challenging, particularly for cost-effective materials, such as Ni. In this study, we developed a porous Ni-coated Ni foam catalyst by electrostatic spray deposition to address these challenges. The catalyst exhibited a turnover frequency approximately ten times higher than that of either porous Ni or Ni foam alone. This enhancement was attributed to the formation of interfacial active sites, which facilitated improved reactant adsorption and activation during hydrogenation. The electrostatic spray deposition technique ensured a uniform and controlled coating, enabling pre-cise engineering of the catalyst structure and interface. The post-deposition heat treatment was further optimized to enhance structural integrity and catalytic performance. This study highlights the importance of interface engineering and structural optimization in catalyst design and pro-vides valuable insights into the development of efficient Ni-based catalysts for industrial hy-drogenation applications. These findings emphasize the potential of electrostatic spray deposition as a versatile method for fabricating advanced catalytic systems.

The Front Cover depicts Fe-substituted MoO_x yolk–shell catalyst spheres anchored on a conductive substrate under alkaline conditions. Mo atoms (yellow) form the oxide framework, while Fe dopants (blue) induce lattice distortion and oxygen vacancy formation within the structure. These defects promote efficient charge redistribution and activate lattice oxygen species (white) for O–O bond formation, with adsorbed and desorbed oxygen intermediates highlighted by subtle red outlines. The porous yolk–shell architecture exposes abundant active sites, while continuous oxygen bubble evolution indicates improved oxygen evolution performance and durability. More information can be found in the Research Article by D. Park and co-workers (DOI: 10.1002/cssc.202502390).

Nickel salts with different counter-anions were used as a model system to examine how precursor chemistry affects aerosol conversion and alkaline hydrogen evolution. Acetate, nitrate, chloride, and sulfate precursors were processed under the same spray-pyrolysis and reduction conditions. Thermogravimetric analysis showed separated dehydration and decomposition steps for acetate and distinct thermal responses for the inorganic salts. Ni_acetate showed the highest geometric HER activity among the tested electrodes, requiring overpotentials of 280.0 and 346.1 mV at 5 and 10 mA cm⁻², respectively, with a Tafel slope of 136.8 mV dec⁻¹. The comparison links precursor-dependent thermal and structural evolution with electrode performance and indicates that physical surface area alone does not account for the activity differences.