Silica‐Protected Ultrathin Ni3FeN Nanocatalyst for the Efficient Hydrolytic Dehydrogenation of NH3BH3

Abstract Transition metal nitrides (TMNs) inevitably aggregate in the high‐temperature thermal ammonolysis process, resulting in blocking of the active catalytic sites and serious decreases in their corresponding catalytic performance. Therefore, how to synthesize ultrasmall TMNs with higher exposed unsaturated coordination sites is still a challenge. Herein, ultrathin Ni 3 FeN (Ni 3 FeN@SiO 2 ) with the size of ≈ 20 nm and thickness of ≈ 3.0 nm is fabricated by SiO 2 protection strategy. The obtained Ni 3 FeN@SiO 2 displays outstanding performance in NH 3 BH 3 hydrolytic dehydrogenation due to the high specific surface area, intrinsic metal‐vacancies, and hydrophilic SiO 2 layer.