Electrosynthesized CuMgAl Layered Double Hydroxides as New Catalysts for the Electrochemical Reduction of CO2

In this study, new nanostructured CuMgAl Layered Double Hydroxide (LDH) based materials are synthesized on a 4 cm² sized carbonaceous gas diffusion membrane. By means of microscopic and spectroscopic techniques, the catalysts are thoroughly investigated, revealing the presence of several species within the same material. By a one-step, reproducible potentiodynamic deposition it is possible to obtain a composite with an intimate contact between a ternary CuMgAl LDH and Cu⁰/Cu₂O species. The catalyst compositions are investigated by varying: the molar ratio between the total amount of bivalent cations and Al³⁺, the amount of loading, and the molar ratios among the three cations in the electrolyte. Each electrocatalyst has been evaluated based on the catalytic performances toward the electrochemical CO₂ reduction to CH₃COOH at −0.4 V versus reversible hydrogen electrode  in liquid phase. The optimized catalyst, that is, CuMgAl 2:1:1 LDH exhibits a productivity of 2.0 mmol_CH3COOH g_cat⁻¹ h⁻¹. This result shows the beneficial effects of combining a material like the LDHs, alkaline in nature, and thus with a great affinity to CO₂, with Cu⁰/Cu⁺ species, which couples the increase of carbon sources availability at the electrode with a redox mediator capable to convert CO₂ into a C₂ product.