Simplified Preparation of BaAl2O4−ye−y/C Oxy‐Electrides Using Pechini Approach for Ammonia Synthesis

Electride‐based materials are among the most active catalysts for ammonia synthesis, with a strong potential for application in the development of green ammonia synthesis; however, their synthesis often requires complicated reaction conditions limiting their scalability. Herein, a straightforward and scalable synthesis method for a BaAl2O4−ye−y/C oxy‐electride composite via carboxylic acid complexation (pseudo‐Pechini) followed by carbothermal reduction is presented. The resulting composite exhibits significant surface area, of ≈41 m2 g−1, which is considerably higher than the electrides prepared by solid‐state synthesis. Upon loading with ruthenium, the BaAl2O4−ye−y/C composite demonstrates excellent catalytic activity for ammonia synthesis, achieving rates of 3090 μmol g−1catalyst h−1 with 0.6Ru/BaAl2O4−ye−y/C, and 3737 μmol g−1catalyst h−1 with 1.1Ru/BaAl2O4−ye−y/C at mild reaction conditions (400 °C and 1 bar). Comprehensive characterization through X‐ray diffraction, Raman spectroscopy, scanning electron microscopy, and scanning transmission electron microscopy‐energy dispersive X‐ray spectroscopy confirms the textural and structural properties of the catalyst, while iodometric titration method and electron paramagnetic resonance analysis confirm the electride‐like nature of the resulting composite. The results reported in this work highlight a straightforward approach for the design of electride‐based composite material displaying superior catalytic properties for green ammonia synthesis.