Hard‐Sphere Random Close‐Packed Au47Cd2(TBBT)31 Nanoclusters with a Faradaic Efficiency of Up to 96 % for Electrocatalytic CO2 Reduction to CO

Metal nanoclusters have recently attracted considerable attention, not only because of their special size range but also because of their well‐defined compositions and structures. However, subtly tailoring the compositions and structures of metal nanoclusters for potential applications remains challenging. Now, a two‐phase anti‐galvanic reduction (AGR) method is presented for precisely tailoring Au44(TBBT)28 to produce Au47Cd2(TBBT)31 nanoclusters with a hard‐sphere random close‐packed structure, exhibiting Faradaic efficiencies of up to 96 % at −0.57 V for the electrocatalytic reduction of CO2 to CO. A two‐phase anti‐galvanic reduction method is used to synthesize novel bimetallic Au47Cd2(TBBT)31 nanoclusters with kernel atoms having hard‐sphere random close‐packings. Au47Cd2(TBBT)31 nanoclusters not only exhibit unique structures but also have higher Faradaic efficiencies for electrocatalytically reducing CO2 to CO (96 % at −0.57 V).