1 research outputs found
Hydroxyl-Bonded Ru on Metallic TiN Surface Catalyzing CO<sub>2</sub> Reduction with H<sub>2</sub>O by Infrared Light
Synchronized conversion of CO2 and H2O into
hydrocarbons and oxygen via infrared-ignited photocatalysis remains
a challenge. Herein, the hydroxyl-coordinated single-site Ru is anchored
precisely on the metallic TiN surface by a NaBH4/NaOH reforming
method to construct an infrared-responsive HO-Ru/TiN photocatalyst.
Aberration-corrected high-angle annular dark-field scanning transmission
electron microscopy (ac-HAADF-STEM) and X-ray absorption spectroscopy
(XAS) confirm the atomic distribution of the Ru species. XAS and density
functional theory (DFT) calculations unveil the formation of surface
HO-RuN5–Ti Lewis pair sites, which achieves efficient
CO2 polarization/activation via dual coordination with
the C and O atoms of CO2 on HO-Ru/TiN. Also, implanting
the Ru species on the TiN surface powerfully boosts the separation
and transfer of photoinduced charges. Under infrared irradiation,
the HO-Ru/TiN catalyst shows a superior CO2-to-CO transformation
activity coupled with H2O oxidation to release O2, and the CO2 reduction rate can further be promoted by
about 3-fold under simulated sunlight. With the key reaction intermediates
determined by in situ diffuse reflectance infrared Fourier transform
spectroscopy (DRIFTS) and predicted by DFT simulations, a possible
photoredox mechanism of the CO2 reduction system is proposed