Not One, Not Two, But at Least Three: Activity Origin of Copper Single-Atom Catalysts toward CO 2 /CO Electroreduction to C 2+ Products

Copper (Cu) single-atom catalysts (SACs) exhibit great potential for generating multicarbon (C2+) products, but the intrinsic activity of single-atom Cu (Cu1) under realistic conditions remains controversial. Herein, we perform extensive calculations with explicit solvation to investigate the underlying mechanism of Cu SACs, disclosing the absence of C2+ activity in Cu1 sites regardless of the different substrates. The original Cu1 sites (first taking Cu1 stably anchored on carbon nitride as an example) cannot facilitate *CO hydrogenation and CO–CO coupling due to the lack of active sites nearby, and they are unstable under operation, causing leaching and aggregation to form small Cu clusters. The derived Cu…

• NN
  National Natural Science Foundation of China

  Awards: 22203044, 22173048
• PA
  Priority Academic Program Development of Jiangsu Higher Education Institutions
• NK
  National Key Research and Development Program of China