Manipulating bimetal structure of CuCo at mesoscale via topological transformation of layered double hydroxides

Abstract Topological transformation of layered double hydroxides (LDHs) containing bimetal components is a powerful method for producing bimetal catalysts, but suffers from uncontrollable bimetal structures and catalytically active sites due to the indistinct mechanism. This work demonstrates the manipulation of CuCo structure by simply changing the aspect ratio or Cu/Co distribution (one in layer and the other in interlayer) of LDHs, affording (i) exclusive Janus Cu‐Co particles or well‐alloyed CuCo particles and (ii) CuCo alloy with Janus Cu‐Co, monometallic Co, or monometallic Cu coexisting. The mesoscale key factor in the topological transformation is revealed. In the syngas conversion, the selectivity to alcohol reaches 49.3% and 43.2% with C 2+ alcohol fraction of >94% on well‐alloyed CuCo and Janus Cu‐Co particles with good affinity of Cu‐Co sites. But the presence of monometallic Co or Cu suppresses alcohol selectivity or C 2+ alcohol fraction by facilitating the production of hydrocarbons or methanol, respectively.