An experimental and theoretical study of binder and conductive additive free 3D-g-CCO/NF for electrocatalytic CO₂ conversion

Electrochemical conversion of CO₂ is a potentially viable approach to attain a carbon-neutral energy cycle and generate value-added hydrocarbons. Currently, binder and conductive additive free catalysts are required to reach industry-level CO₂ conversion rates. Here, we describe the production of a binder and conductive additive free three-dimensional grass-like CuCo₂O₄ spinel complex embedded in nickel foam (3D-g-CCO/NF) through a hydrothermal process followed by calcination. The 3D-g-CCO/NF achieved a maximum current density of −303.4 mA cm⁻² and exhibited high faradaic efficiency of 61.44% ± 3.5% for CO and 34.31% ± 3.5% for HCOOH. Density functional theory calculations indicate that the 3D-g-CCO/NF reduced the energy barrier of *COOH compared with *OCHO to form CO as a primary product. Further analysis revealed that the elemental and morphological structures of the 3D-g-CCO/NF were retained. This work emphasizes an impressive theoretical and experimental understanding for large-scale applications.