Atomically Fe-doped MoS_2−x with Fe-Mo dual sites for efficient electrocatalytic NO reduction to NH₃

Electrocatalytic NO-to-NH₃ conversion (NORR) provides an appealing route for both sustainable NH₃ production and harmful NO abatement. Herein, we combine the strategies of atomic doping and vacancy engineering to design atomically Fe-doped and S-vacancy-rich MoS₂ (Fe₁/MoS_2−x) as a highly efficient NORR catalyst, showing the maximum NH₃-Faradaic efficiency of 82.5% and NH₃ yield of 288.2 μmol h⁻¹ cm⁻² at − 0.6 V vs. RHE. Theoretical calculations unveil that Fe-Mo dual sites created on Fe₁/MoS_2−x can cooperatively activate NO and dissociate the N[dbnd]O bond, boost the protonation energetics and simultaneously suppress the competing hydrogen evolution, resulting in the significantly expedited NORR activity and selectivity.