Spin Effect of Transition Metal Oxides on Ammonia Decomposition

The ammonia decomposition reaction serves as a critical model for understanding the spin effect due to the spin sensitivity of its intermediates. However, due to the challenges in characterizing the electronic structural changes influenced by spin in experiments, the spin interactions between active sites and reaction intermediates remain elusive. Herein, the differences in spin effects between 3d-5d orbital transition metal oxides and various intermediates were investigated through a combination of DFT calculations and experimental characterization. By constructing novel descriptors, we decouple how the spin-orbital coupling of the adsorbate and catalyst affects the magnetic exchange interaction. It has been proven that the better the intrinsic magnetic moment of the metal center matches the average magnetism of the reaction intermediates, the more favorable it is for enhancing the catalytic reaction rate.