Interface Catalysts of In Situ-Grown TiO2/MXenes for High-Faraday-Efficiency CO2 Reduction

Climate change and the global energy crisis have led to an increasing need for greenhouse gas remediation and clean energy sources. The electrochemical CO₂ reduction reaction (CO₂RR) is a promising solution for both issues as it harvests waste CO₂ and chemically reduces it to more useful forms. However, the high overpotential required for the reaction makes it electrochemically unfavorable. Here, we fabricate a novel electrode composed of TiO₂ nanoparticles grown in situ on MXene charge acceptor 2D sheets with excellent CO₂RR characteristics. A straightforward solvothermal method was used to grow the nanoparticles on the Ti₃C₂T<i>_x</i> MXene flakes. The electrochemical performance of the TiO₂/MXene electrodes was analyzed. The Faradaic efficiencies of the TiO₂/MXene electrodes were determined, with a value of 99.41% at -1.9 V (vs. Ag/AgCl). Density functional theory mechanistic analysis was used to reveal the most likely mechanism resulting in the production of one CO molecule along with a carbonate anion through ∗CO, ∗O, and activated CO₂^2- intermediates. Bader charge analysis corroborated this pathway, showing that CO₂ gains a greater negative charge when TiO₂/MXene serves as a catalyst compared to MXene or TiO₂ alone. These results show that TiO₂/MXene nanocomposite electrodes may be very useful in the conversion of CO₂ while still being efficient in both time and cost.