Manufacturing Single‐Atom Alloy Catalysts for Selective CO2 Hydrogenation via Refinement of Isolated‐Alloy‐Islands

Abstract Single‐atom alloy (SAA) catalysts exhibit huge potential in heterogeneous catalysis. Manufacturing SAAs requires complex and expensive synthesis methods to precisely control the atomic scale dispersion to form diluted alloys with less active sites and easy sintering of host metal, which is still in the early stages of development. Here, we address these limitations with a straightforward strategy from a brand‐new perspective involving the ‘islanding effect’ for manufacturing SAAs without dilution: homogeneous RuNi alloys were continuously refined to highly dispersed alloy‐islands (~1 nm) with completely single‐atom sites where the relative metal loading was as high as 40 %. Characterized by advanced atomic‐resolution techniques, single Ru atoms were bonded with Ni as SAAs with extraordinary long‐term stability and no sintering of the host metal. The SAAs exhibited 100 % CO selectivity, over 55 times reverse water‐gas shift (RWGS) rate than the alloys with Ru cluster sites, and over 3–4 times higher than SAAs by the dilution strategy. This study reports a one‐step manufacturing strategy for SAA's using the wetness impregnation method with durable high atomic efficiency and holds promise for large‐scale industrial applications.