Synergistic Effect of FeNi Bimetallic Clusters for the Catalytic of Hydrogen Dissociation and Desorption: A Density Functional Theory Study

Cognition to the metal-metal interactions is of vital importance for the catalytic process and would help exploring novel catalysts. In the present study, the model system of FexNiy (x + y = 6) bimetallic clusters was utilized to study how metal-metal interactions influence the catalytic performance. The formation energies of different FeNi clusters, the hydrogen chemisorption energies together with the maximum hydrogen capacity and the saturated hydrogen atoms desorption energies were calculated. Bimetallic clusters exhibit a superior performance than pure clusters. Especially, Fe2Ni4 cluster has the highest hydrogen loading capacity, the most facile hydrogen molecule dissociation activation energy barrier and the lowest hydrogen atom desorption energy, suggesting that it is easier to dissociate H2 and release the H atoms. As a consequence, by adjusting appropriate metal/metal ratios, it is possible to design bimetallic catalysts with excellent catalytic performance.