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We report here the first purely organometallic  fac ‐[Mn I (CO) 3 (bis‐ Me NHC)Br] complex with unprecedented activity for the selective electrocatalytic reduction of CO 2  to CO, exceeding 100 turnovers with excellent faradaic yields ( η  CO ≈95 %) in anhydrous CH 3 CN. Under the same conditions, a maximum turnover frequency (TOF max ) of 2100 s −1  was measured by cyclic voltammetry, which clearly exceeds the values reported for other manganese‐based catalysts. Moreover, the addition of water leads to the highest TOF max  value (ca. 320 000 s −1 ) ever reported for a manganese‐based catalyst. A Mn I  tetracarbonyl intermediate was detected under catalytic conditions for the first time.

A Highly Active N‐Heterocyclic Carbene Manganese(I) Complex for Selective Electrocatalytic CO 2 Reduction to CO