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Dual Active Centers Bridged by Oxygen Vacancies of Ruthenium Single-Atom Hybrids Supported on Molybdenum Oxide for Photocatalytic Ammonia Synthesis.

Haibo YinZhen ChenYue PengShangchao XiongYadong LiHiromi YamashitaJunhua Li
Published in: Angewandte Chemie (International ed. in English) (2022)
Photocatalytic synthesis of ammonia (NH 3 ) holds significant potential compared with the Haber-Bosch process. However, the reported photocatalysts suffer from low efficiency owing to localized electron deficiency. Herein, Ru-SA (single atoms)/H x MoO 3-y hybrids with abundant of Mo n+ (4<n<6) species neighboring oxygen vacancies (O V ) are synthesized via a H-spillover process. Detailed characterizations demonstrate that Ru-SA/H x MoO 3-y hybrids can quantitatively produce NH 3 from N 2 and H 2 through the presence of dual active centers (Ru SA and Mo n+ ). The Ru SA boost the activation and migration of H 2 , and Mo n+ species act as the trapping sites of localized electrons and the adsorption and dissociation sites of N 2 , finally leading to NH 3 synthesis on Mo n+ -OH. The NH 3 generation rate is up to 4.0 mmol h -1  g -1 , accompanied by an apparent quantum efficiency over 6.0 % at 650 nm.
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