Unveiling the magnetic ordering effect in La-doped Ti3C2O2 MXenes on electrocatalytic CO2 reduction

Abstract

In the pursuit of sustainable energy solutions, the carbon dioxide reduction reaction (CO₂RR) holds immense promise for converting CO₂ into valuable chemicals and fuels. In this view, the exploration of magnetic MXene catalysts is crucial for understanding their reactivity and performance in electrochemical reactions to improve the CO₂ conversion process. Herein, two distinct magnetic configurations, ferromagnetic (FM) and antiferromagnetic (AFM), were considered for La-doped Ti₃C₂O₂ (La-Ti₃C₂O₂). Using density functional theory (DFT) calculations, the first principles simulation was carried out to evaluate the electronic properties, magnetic properties, and CO₂RR potential of these configurations. Our findings reveal an enhancement in semiconductivity and surface reactivity of the La-Ti₃C₂O₂ catalyst, resulting in improved electron transfer characteristics. This facilitates CO₂ adsorption and decreases the formation energy barrier of intermediate species towards the CO₂ hydrogenations. The La-Ti₃C₂O₂ catalyst showed a better performance than the parent molecule Ti₃C₂O₂, which suffers from an insufficiency of reactivity on its surface. Furthermore, the study demonstrates the AFM structure of La-Ti₃C₂O₂ to be the soundest, which thereby displays a better efficiency than the FM structure. Considering our findings, during the current CO₂ conversion process, the reaction pathway with a less energy consumption must be preferred over others.