<p>Solar-driven conversion of CO<sub>2</sub> into hydrocarbons offers a sustainable route to carbon-neutral fuels, yet efficient C-C coupling under photo-thermal conditions remains challenging. Here, we report a potassium-promoted Cu<sub>2</sub>Fe<sub>1</sub> tandem catalyst for selective photo-thermal CO<sub>2</sub> hydrogenation under industrially relevant conditions. Under illumination at 250 °C and 20 bar, the catalyst achieves 77.4% selectivity towards C<sub>2</sub><sup>+</sup> hydrocarbons, with a C<sub>2-5</sub> hydrocarbon yield of 5.04 mmol g<sup>−1</sup> h<sup>−1</sup>, representing highly competitive performance among reported photo-thermal CO<sub>2</sub> hydrogenation systems. Mechanistic studies reveal a tandem pathway in which Cu promotes the reverse water-gas shift reaction to generate CO, followed by Fischer-Tropsch-type hydrocarbon formation over in situ-formed <i>χ</i>-Fe<sub>5</sub>C<sub>2</sub>. In situ DRIFTS, in situ XRD and CO-TPR analyses further show that light-induced non-thermal effects, together with localized heating at the Cu-Fe interface, facilitate carbide formation and accelerate key intermediate evolution.</p>

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Unlocking solar-derived CO2 conversion to hydrocarbons over plasmonic Cu-Fe tandem catalysts under industrially relevant conditions

  • Xinhuilan Wang,
  • Alejandra Rendón-Patiño,
  • Diego Mateo,
  • Jorge Gascon

摘要

Solar-driven conversion of CO2 into hydrocarbons offers a sustainable route to carbon-neutral fuels, yet efficient C-C coupling under photo-thermal conditions remains challenging. Here, we report a potassium-promoted Cu2Fe1 tandem catalyst for selective photo-thermal CO2 hydrogenation under industrially relevant conditions. Under illumination at 250 °C and 20 bar, the catalyst achieves 77.4% selectivity towards C2+ hydrocarbons, with a C2-5 hydrocarbon yield of 5.04 mmol g−1 h−1, representing highly competitive performance among reported photo-thermal CO2 hydrogenation systems. Mechanistic studies reveal a tandem pathway in which Cu promotes the reverse water-gas shift reaction to generate CO, followed by Fischer-Tropsch-type hydrocarbon formation over in situ-formed χ-Fe5C2. In situ DRIFTS, in situ XRD and CO-TPR analyses further show that light-induced non-thermal effects, together with localized heating at the Cu-Fe interface, facilitate carbide formation and accelerate key intermediate evolution.