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Phase-selective active sites on ordered/disordered titanium dioxide enable exceptional photocatalytic ammonia synthesis.

ABSTRACT: Photocatalytic N₂ fixation to NH₃ via defect creation on TiO₂ to activate ultra-stable N[triple bond, length as m-dash]N has drawn enormous scientific attention, but poor selectivity and low yield rate are the major bottlenecks. Additionally, whether N₂ preferentially adsorbs on phase-selective defect sites on TiO₂ in correlation with appropriate band alignment has yet to be explored. Herein, theoretical predictions reveal that the defect sites on disordered anatase (A_d) preferentially exhibit higher N₂ adsorption ability with a reduced energy barrier for a potential-determining-step (*N₂ to NNH*) than the disordered rutile (R_d) phase of TiO₂. Motivated by theoretical simulations, we synthesize a phase-selective disordered-anatase/ordered-rutile TiO₂ photocatalyst (Na-A_d/R_o) by sodium-amine treatment of P25-TiO₂ under ambient conditions, which exhibits an efficient NH₃ formation rate of 432 μmol g^-1 h^-1, which is superior to that of any other defect-rich disordered TiO₂ under solar illumination with a high apparent quantum efficiency of 13.6% at 340 nm. The multi-synergistic effects including selective N₂ chemisorption on the defect sites of Na-A_d with enhanced visible-light absorption, suitable band alignment, and rapid interfacial charge separation with R_o enable substantially enhanced N₂ fixation.

SUBMITTER: Lee J

PROVIDER: S-EPMC8293799 | biostudies-literature |

REPOSITORIES: biostudies-literature

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