Abstract
Recently, single-atom catalysts have aroused extensive attention in fields of clean energy and environmental protection due to their unique activity and efficient utilization of the active atoms. It is of great importance but still remains a great challenge to unveil the effect of single atoms on precise catalysis. Herein, it is reported that doping TiO2 hollow microspheres (TiO2 -HMSs) with single atomic Fe can boost the photoreactivity of TiO2 -HMSs towards NO oxidation due to the synergistic effects of atomically dispersed Fe and bonded Ti atom which act as dual active sites. The atomically dispersed Fe atoms occupy the subsurface Ti vacancies, and the interaction between Ti 3d and Fe 3d orbitals result in the formation of FeTi bond. Single atomic Fe modulates the electronic structure of the bonded Ti atoms by electron transfer, which facilitates the adsorption and activation of NO and O2 at Fe and bonded Ti sites, respectively. In addition, the introduction of single atomic Fe sharply suppresses the production of toxic NO2 byproduct. The synergistic effects of the dual active sites then cause a drastic promotion in photocatalytic oxidation of NO.
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