Direct conversion of CO and H2O to hydrocarbons at atmospheric pressure using a TiO2−x/Ni photothermal catalyst
摘要
Hydrocarbon fuels can be synthesized from CO and water via Kölbel–Engelhardt synthesis, a thermocatalytic process in which temperatures of ≥200 °C and elevated pressures are typically needed. While light-driven hydrocarbon production by CO hydrogenation has been demonstrated under milder conditions, for this reaction H2 must first be sourced. Here we report the direct production of hydrocarbons from CO and water at atmospheric pressure via light-driven Kölbel–Engelhardt synthesis without external heating or the addition of H2. Using a TiO2-supported Ni catalyst, we obtain an activity of 8.83 mol−CH2− molNi−1 h−1 and C2+ selectivity higher than 55%. In situ spectroscopy and density functional theory calculations suggest that the migration of photogenerated electrons from TiO2 to Ni facilitates carbon–carbon coupling at the interface of the TiO2−x/Ni catalyst, which accounts for the observed high selectivity towards multi-carbon products.