Angewandte Chemie International Edition · 2023 · 28 citations · 35 references
The ambient ammonia synthesis coupled with distributed green hydrogen production technology can provide promising solutions for low-carbon NH<sub>3</sub> production and H<sub>2</sub> storage. Herein, we reported Ru-loaded defective pyrochlore K<sub>2</sub> Ta<sub>2</sub> O<sub>6-x</sub> with remarkable visible-light absorption and a very low work function, enabling effective visible-light-driven ammonia synthesis from N<sub>2</sub> and H<sub>2</sub> at low pressure down to 0.2 atm. The photocatalytic rate was 2.8 times higher than that of the best previously reported photocatalyst and the photo-thermal rate at 425 K was similar to that of Ru-loaded black TiO<sub>2</sub> at 633 K. Compared to perovskite-type KTaO<sub>3-x</sub> with the same composition, the pyrochlore exhibited a 3.7-fold increase in intrinsic activity due to a higher photoexcited charge separation efficiency and a higher conduction band position. The interfacial Schottky barrier and spontaneous electron transfer between K<sub>2</sub> Ta<sub>2</sub> O<sub>6-x</sub> and Ru further improve photoexcited charge separation and accumulate energetic electrons to facilitate N<sub>2</sub> activation.
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How a century of ammonia synthesis changed the world
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