Continuous-Flow Sunlight-Powered CO<sub>2</sub> Methanation Catalyzed by γ-Al<sub>2</sub>O<sub>3</sub>-Supported Plasmonic Ru Nanorods
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, irra...
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author | Jelle Rohlfs Koen W. Bossers Nicole Meulendijks Fidel Valega Mackenzie Man Xu Marcel A. Verheijen Pascal Buskens Francesc Sastre |
author_facet | Jelle Rohlfs Koen W. Bossers Nicole Meulendijks Fidel Valega Mackenzie Man Xu Marcel A. Verheijen Pascal Buskens Francesc Sastre |
author_sort | Jelle Rohlfs |
collection | DOAJ |
description | 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. |
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spelling | doaj.art-662d92e9b46345028b0cb7b5a199023f2023-11-23T19:11:41ZengMDPI AGCatalysts2073-43442022-01-0112212610.3390/catal12020126Continuous-Flow Sunlight-Powered CO<sub>2</sub> Methanation Catalyzed by γ-Al<sub>2</sub>O<sub>3</sub>-Supported Plasmonic Ru NanorodsJelle Rohlfs0Koen W. Bossers1Nicole Meulendijks2Fidel Valega Mackenzie3Man Xu4Marcel A. Verheijen5Pascal Buskens6Francesc Sastre7The Netherlands Organisation for Applied Scientific Research (TNO), High Tech Campus 25, 5656AE Eindhoven, The NetherlandsThe Netherlands Organisation for Applied Scientific Research (TNO), High Tech Campus 25, 5656AE Eindhoven, The NetherlandsThe Netherlands Organisation for Applied Scientific Research (TNO), High Tech Campus 25, 5656AE Eindhoven, The NetherlandsThe Netherlands Organisation for Applied Scientific Research (TNO), High Tech Campus 25, 5656AE Eindhoven, The NetherlandsThe Netherlands Organisation for Applied Scientific Research (TNO), High Tech Campus 25, 5656AE Eindhoven, The NetherlandsEurofins Materials Science, High Tech Campus 11, 5656AE Eindhoven, The NetherlandsThe Netherlands Organisation for Applied Scientific Research (TNO), High Tech Campus 25, 5656AE Eindhoven, The NetherlandsThe Netherlands Organisation for Applied Scientific Research (TNO), High Tech Campus 25, 5656AE Eindhoven, The NetherlandsPlasmonic 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.https://www.mdpi.com/2073-4344/12/2/126carbon dioxideSabatier reactionsolar lightsurface plasmon resonancephotochemistry |
spellingShingle | Jelle Rohlfs Koen W. Bossers Nicole Meulendijks Fidel Valega Mackenzie Man Xu Marcel A. Verheijen Pascal Buskens Francesc Sastre Continuous-Flow Sunlight-Powered CO<sub>2</sub> Methanation Catalyzed by γ-Al<sub>2</sub>O<sub>3</sub>-Supported Plasmonic Ru Nanorods Catalysts carbon dioxide Sabatier reaction solar light surface plasmon resonance photochemistry |
title | Continuous-Flow Sunlight-Powered CO<sub>2</sub> Methanation Catalyzed by γ-Al<sub>2</sub>O<sub>3</sub>-Supported Plasmonic Ru Nanorods |
title_full | Continuous-Flow Sunlight-Powered CO<sub>2</sub> Methanation Catalyzed by γ-Al<sub>2</sub>O<sub>3</sub>-Supported Plasmonic Ru Nanorods |
title_fullStr | Continuous-Flow Sunlight-Powered CO<sub>2</sub> Methanation Catalyzed by γ-Al<sub>2</sub>O<sub>3</sub>-Supported Plasmonic Ru Nanorods |
title_full_unstemmed | Continuous-Flow Sunlight-Powered CO<sub>2</sub> Methanation Catalyzed by γ-Al<sub>2</sub>O<sub>3</sub>-Supported Plasmonic Ru Nanorods |
title_short | Continuous-Flow Sunlight-Powered CO<sub>2</sub> Methanation Catalyzed by γ-Al<sub>2</sub>O<sub>3</sub>-Supported Plasmonic Ru Nanorods |
title_sort | continuous flow sunlight powered co sub 2 sub methanation catalyzed by γ al sub 2 sub o sub 3 sub supported plasmonic ru nanorods |
topic | carbon dioxide Sabatier reaction solar light surface plasmon resonance photochemistry |
url | https://www.mdpi.com/2073-4344/12/2/126 |
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