It is still a grand challenge to exploit efficient catalysts to achieve sustainable photocatalytic N reduction under ambient conditions. Here, we developed a ruthenium-based single-atom catalyst anchored on defect-rich TiO nanotubes (denoted Ru-SAs/Def-TNs) as a model system for N fixation. The constructed Ru-SAs/Def-TNs exhibited a catalytic efficiency of 125.2 μmol g h, roughly 6 and 13 times higher than those of the supported Ru nanoparticles and Def-TNs, respectively. Through ultrafast transient absorption and photoluminescence spectroscopy, we revealed the relationship between catalytic activity and photoexcited electron dynamics in such a model SA catalytic system. The unique ligand-to-metal charge-transfer state formed in Ru-SAs/Def-TNs was found to be responsible for its high catalytic activity because it can greatly promote the transfer of photoelectrons from Def-TNs to the Ru-SAs center and the subsequent capture by Ru-SAs. This work sheds light on the origin of the high performance of SA catalysts from the perspective of photoexcited electron dynamics and hence enriches the mechanistic understanding of SA catalysis.
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