Rational Design and Validation of CuO/Cu Heterogeneous Interface Catalyst for CO Electroreduction to C Products.

Rapid construction of highly active non-precious metal catalysts for electrochemical CO reduction reaction (CORR) to C products is still challenging. Under the guidance of theoretical calculation, the CuO(200)/Cu(111) is screened heterogeneous catalyst which is favorable for arduous CO activation and unstable CO adsorption during the electrochemical CORR. Then, a novel CuO(200)/Cu(111) heterogeneous interface is fabricated by an ambient precipitation coupled chemical reduction strategy. Notably, the obtained CuO/Cu exhibits excellent activity for CORR, which FE is 82.98% under the industrial current density of 450 mA cm in membrane electrode assembly cell. In situ X-ray photoelectron spectroscopy combined with spherical aberration correction electron microscope reveals CuO/Cu interface exhibits the excellent structural durability. Furthermore, in situ Raman and in situ attenuated total reflection-surface-enhanced IR absorption spectroscopy directly capture COOH, CHO, and COCHO intermediates, disclosing the formation of the C products involves in the COCHO pathway. Mechanism studies demonstrate the presence of charge aggregation at CuO/Cu interface directly reduces the energy barrier for C─C coupling (rate-determining step) to 0.76 eV. This work developed a highly active heterogeneous interface for CORR, which provides a novel insight for the fabrication of Cu-based catalysts.