Journal
CHEMICAL ENGINEERING JOURNAL
Volume 454, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.140158
Keywords
Photocatalytic nitrogen fixation; Ru single atom; EMSI; Active sites; Oxygen vacancy
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The sustainable production of NH3 via photocatalysis is challenging due to the difficulty in activating inert N-2. In this study, a photocatalyst based on electronic metal-support interactions (EMSI) was developed, and introducing Ru single atoms into TiO2 improved the N-2 fixation performance. The enhanced EMSI facilitated the transfer of photogenerated carriers and achieved efficient photocatalytic N-2 reduction.
The sustainable production of NH3 by fixing N-2 under mild conditions via photocatalysis is fascinating compared to current industrial processes operated at critical conditions. However, the inert N-2 is extremely difficult to adsorb and activate. And the transfer of photogenerated electrons to the NN bond is energetically challengeable. Herein, we presented a photocatalyst designed based on electronic metal-support interactions (EMSI), which proved to be a reliable strategy for improving the photocatalytic N-2 fixation performance. The introduction of Ru single atoms into TiO2 by a molten salt method can stabilize the oxygen vacancies, thus achieving an ammonia yield rate of 18.9 mu mol.g(-1).h(-1) under mild conditions without any sacrificial agent due to the significant enhancement of EMSI. The combination of experimental results with first-principles simulations confirmed that the EMSI can tune the local atomic structure and accelerate the transfer of photogenerated carriers between Ru single atoms and TiO2 carriers, thus effectively enhancing photocatalytic N-2 reduction activity. Additionally, the alternating pathway is more favored route for NH3 formation on the optimized single atom Ru/TiO2. Our atomic-level design and mechanistic studies provided a new reference for efficiently photocatalytic nitrogen fixation.
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