Continuous-Flow Sunlight-Powered CO<sub>2</sub> Methanation Catalyzed by γ-Al<sub>2</sub>O<sub>3</sub>-Supported Plasmonic Ru Nanorods

oleh: Jelle Rohlfs, Koen W. Bossers, Nicole Meulendijks, Fidel Valega Mackenzie, Man Xu, Marcel A. Verheijen, Pascal Buskens, Francesc Sastre

Format: Article
Diterbitkan: MDPI AG 2022-01-01

Deskripsi

Plasmonic CO<sub>2</sub> methanation using γ-Al<sub>2</sub>O<sub>3</sub>-supported Ru nanorods was carried out under continuous-flow conditions without conventional heating, using mildly concentrated sunlight as the sole and sustainable energy source (AM 1.5, irradiance 5.5–14.4 kW·m<sup>−2</sup> = 5.5–14.4 suns). Under 12.5 suns, a CO<sub>2</sub> conversion exceeding 97% was achieved with complete selectivity towards CH<sub>4</sub> and a stable production rate (261.9 <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><mi>mmol</mi><mo>·</mo><msubsup><mi mathvariant="normal">g</mi><mrow><mi>Ru</mi></mrow><mrow><mo>−</mo><mn>1</mn></mrow></msubsup><mo>·</mo><msup><mi mathvariant="normal">h</mi><mrow><mo>−</mo><mn>1</mn></mrow></msup></mrow></semantics></math></inline-formula>) for at least 12 h. The CH<sub>4</sub> production rate showed an exponential increase with increasing light intensity, suggesting that the process was mainly promoted by photothermal heating. This was confirmed by the apparent activation energy of 64.3 kJ·mol<sup>−1</sup>, which is very similar to the activation energy obtained for reference experiments in dark (67.3 kJ·mol<sup>−1</sup>). The flow rate influence was studied under 14.4 suns, achieving a CH<sub>4</sub> production plateau of 264 µmol min<sup>−1</sup> (792 <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><mi>mmol</mi><mo>·</mo><msubsup><mi mathvariant="normal">g</mi><mrow><mi>Ru</mi></mrow><mrow><mo>−</mo><mn>1</mn></mrow></msubsup><mo>·</mo><msup><mi mathvariant="normal">h</mi><mrow><mo>−</mo><mn>1</mn></mrow></msup></mrow></semantics></math></inline-formula>) with a constant catalyst bed temperature of approximately 204 °C.