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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Main Authors: Jelle Rohlfs, Koen W. Bossers, Nicole Meulendijks, Fidel Valega Mackenzie, Man Xu, Marcel A. Verheijen, Pascal Buskens, Francesc Sastre
Format: Article
Language:English
Published: MDPI AG 2022-01-01
Series:Catalysts
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Online Access:https://www.mdpi.com/2073-4344/12/2/126
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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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