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Atomically dispersed Ir confined in amorphous MoO3 (Ir1/a-MoO3) was designed as a high-efficiency catalyst for electrochemical reduction reaction of NO to NH3 (NORR). Atomic precise characterizations reveal that isolated Ir atoms are immobilized in O-vacancies of amorphous MoO3 to form Ir1-O5 moieties. Theoretical computations demonstrate that single-site Ir1-O5 can not only powerfully activate and hydrogenate NO with a near-zero energy barrier, but also exhibit a higher affinity to NO over H adatoms to suppress the competing hydrogen evolution and promote both NORR activity and selectivity. Consequently, Ir1/a-MoO3 shows the maximum NH3 yield rate of 438.8 μmol∙h−1∙cm−2 and NH3-Faradaic efficiency of 93.2%, representing one of the most efficient NORR catalysts to date.
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