RESUMO
Electrochemical carbon dioxide (CO2) conversion has enormous potential for reducing high atmospheric CO2 levels and producing valuable products simultaneously; however the development of inexpensive catalysts remains a great challenge. In this work, we successfully synthesised a 1D Cu-based metal-organic framework [Cu(PyDC)(H2O)], which crystallizes in an orthorhombic system with the Pccn space group, by the hydrothermal method. Among the different catalysts utilized, the heterostructures of cathodized Cu-Cu2O@CC demonstrate increased efficiency in producing CH3OH and C2H4, achieving maximum FE values of 37.4% and 40.53%, respectively. Also, the product formation rates of CH3OH and C2H4 reach up to 667 and 1921 µmol h-1 cm-2. On the other side, Cu-Cu2O/NC-700 carbon composites simultaneously produced C1-C3 products with a total FE of 23.27%. Furthermore, a comprehensive study involving detailed DFT simulations is used to calculate the energetic stability and catalytic activity towards the CO2 reduction of Cu(111), Cu2O(111), and Cu@Cu2O(111) surfaces. During the early phase of electrochemical treatment, Cu(II) carboxylate nodes (Cu-O) in the Cu(PyDC)(H2O) MOF were reduced to Cu and Cu2O, with a possible synergistic enhancement from the PyDC ligands. Thus, the improved activity and product enhancement are closely associated with the cathodized reconstruction of Cu-Cu2O@CC heterostructures on carbon cloth. Hence, this study provides efficient derivatives of Cu-based MOFs for notable electrocatalytic activity in CO2 reduction and gives valuable insights towards the advancement of practical CO2 conversion technology.