Electronic Modulation of the Interaction between Fe Single Atoms and WO2.72-x for Photocatalytic N2 Reduction

In the design of photocatalysts for ammonia synthesis, the construction of effective nitrogen (N-2) adsorption and activation sites is critical. Herein, Fe single atoms were effectively fixed on the surfaces of WO2.72-x nanowires. Electronic interactions between single Fe atoms and WO2.72-x resulted in a d-band center shift toward the Fermi level and thus enhancement of N-2 bonding with the catalyst surface. The studies of differential charge density and electron localization reveal that there is enhanced electron transfer from Fe-SA/WO2.72-x to the adsorbed N-2, signifying that Fe single atoms are active centers for N-2 activation. Benefiting from electronic interactions, the optimized catalyst shows a NH(4)( )(+)generation rate of 186.5 mu mol g(-1 )h(-1) during photocatalytic N-2 reduction.

Automated summary

In the design of photocatalysts for ammonia synthesis, the fixation of single Fe atoms effectively provides sites for nitrogen adsorption and activation, leading to enhanced interaction between the catalyst surface and nitrogen molecules. The optimized catalyst shows a high NH(4)( )(+) generation rate during photocatalytic N-2 reduction.