Sunlight-Powered Reverse Water Gas Shift Reaction Catalysed by Plasmonic Au/TiO<sub>2</sub> Nanocatalysts: Effects of Au Particle Size on the Activity and Selectivity
This study reports the low temperature and low pressure conversion (up to 160 °C, <i>p</i> = 3.5 bar) of CO<sub>2</sub> and H<sub>2</sub> to CO using plasmonic Au/TiO<sub>2</sub> nanocatalysts and mildly concentrated artificial sunlight as the sole ene...
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| Format: | Article |
| Language: | English |
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MDPI AG
2022-11-01
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| Series: | Nanomaterials |
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| Online Access: | https://www.mdpi.com/2079-4991/12/23/4153 |
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| author | Jordi Volders Ken Elen Arno Raes Rajeshreddy Ninakanti An-Sofie Kelchtermans Francesc Sastre An Hardy Pegie Cool Sammy W. Verbruggen Pascal Buskens Marlies K. Van Bael |
| author_facet | Jordi Volders Ken Elen Arno Raes Rajeshreddy Ninakanti An-Sofie Kelchtermans Francesc Sastre An Hardy Pegie Cool Sammy W. Verbruggen Pascal Buskens Marlies K. Van Bael |
| author_sort | Jordi Volders |
| collection | DOAJ |
| description | This study reports the low temperature and low pressure conversion (up to 160 °C, <i>p</i> = 3.5 bar) of CO<sub>2</sub> and H<sub>2</sub> to CO using plasmonic Au/TiO<sub>2</sub> nanocatalysts and mildly concentrated artificial sunlight as the sole energy source (up to 13.9 kW·m<sup>−2</sup> = 13.9 suns). To distinguish between photothermal and non-thermal contributors, we investigated the impact of the Au nanoparticle size and light intensity on the activity and selectivity of the catalyst. A comparative study between P25 TiO<sub>2</sub>-supported Au nanocatalysts of a size of 6 nm and 16 nm displayed a 15 times higher activity for the smaller particles, which can only partially be attributed to the higher Au surface area. Other factors that may play a role are e.g., the electronic contact between Au and TiO<sub>2</sub> and the ratio between plasmonic absorption and scattering. Both catalysts displayed ≥84% selectivity for CO (side product is CH<sub>4</sub>). Furthermore, we demonstrated that the catalytic activity of Au/TiO<sub>2</sub> increases exponentially with increasing light intensity, which indicated the presence of a photothermal contributor. In dark, however, both Au/TiO<sub>2</sub> catalysts solely produced CH<sub>4</sub> at the same catalyst bed temperature (160 °C). We propose that the difference in selectivity is caused by the promotion of CO desorption through charge transfer of plasmon generated charges (as a non-thermal contributor). |
| first_indexed | 2024-03-09T17:38:30Z |
| format | Article |
| id | doaj.art-345529dd340f489995cef6cc976fac4e |
| institution | Directory Open Access Journal |
| issn | 2079-4991 |
| language | English |
| last_indexed | 2024-03-09T17:38:30Z |
| publishDate | 2022-11-01 |
| publisher | MDPI AG |
| record_format | Article |
| series | Nanomaterials |
| spelling | doaj.art-345529dd340f489995cef6cc976fac4e2023-11-24T11:46:20ZengMDPI AGNanomaterials2079-49912022-11-011223415310.3390/nano12234153Sunlight-Powered Reverse Water Gas Shift Reaction Catalysed by Plasmonic Au/TiO<sub>2</sub> Nanocatalysts: Effects of Au Particle Size on the Activity and SelectivityJordi Volders0Ken Elen1Arno Raes2Rajeshreddy Ninakanti3An-Sofie Kelchtermans4Francesc Sastre5An Hardy6Pegie Cool7Sammy W. Verbruggen8Pascal Buskens9Marlies K. Van Bael10Design and Synthesis of Inorganic Materials (DESINe), Institute for Materials Research, Hasselt University, Agoralaan Building D, 3590 Diepenbeek, BelgiumDesign and Synthesis of Inorganic Materials (DESINe), Institute for Materials Research, Hasselt University, Agoralaan Building D, 3590 Diepenbeek, BelgiumSustainable Energy, Air & Water Technology (DuEL), University of Antwerp, Groenenborgerlaan 171, 2020 Antwerp, BelgiumSustainable Energy, Air & Water Technology (DuEL), University of Antwerp, Groenenborgerlaan 171, 2020 Antwerp, BelgiumDesign and Synthesis of Inorganic Materials (DESINe), Institute for Materials Research, Hasselt University, Agoralaan Building D, 3590 Diepenbeek, BelgiumThe Netherlands Organisation for Applied Scientific Research (TNO), High Tech Campus 25, 5656 AE Eindhoven, The NetherlandsDesign and Synthesis of Inorganic Materials (DESINe), Institute for Materials Research, Hasselt University, Agoralaan Building D, 3590 Diepenbeek, BelgiumLaboratory of Adsorption and Catalysis, University of Antwerp, Universiteitsplein 1, 2610 Wilrijk, BelgiumSustainable Energy, Air & Water Technology (DuEL), University of Antwerp, Groenenborgerlaan 171, 2020 Antwerp, BelgiumDesign and Synthesis of Inorganic Materials (DESINe), Institute for Materials Research, Hasselt University, Agoralaan Building D, 3590 Diepenbeek, BelgiumDesign and Synthesis of Inorganic Materials (DESINe), Institute for Materials Research, Hasselt University, Agoralaan Building D, 3590 Diepenbeek, BelgiumThis study reports the low temperature and low pressure conversion (up to 160 °C, <i>p</i> = 3.5 bar) of CO<sub>2</sub> and H<sub>2</sub> to CO using plasmonic Au/TiO<sub>2</sub> nanocatalysts and mildly concentrated artificial sunlight as the sole energy source (up to 13.9 kW·m<sup>−2</sup> = 13.9 suns). To distinguish between photothermal and non-thermal contributors, we investigated the impact of the Au nanoparticle size and light intensity on the activity and selectivity of the catalyst. A comparative study between P25 TiO<sub>2</sub>-supported Au nanocatalysts of a size of 6 nm and 16 nm displayed a 15 times higher activity for the smaller particles, which can only partially be attributed to the higher Au surface area. Other factors that may play a role are e.g., the electronic contact between Au and TiO<sub>2</sub> and the ratio between plasmonic absorption and scattering. Both catalysts displayed ≥84% selectivity for CO (side product is CH<sub>4</sub>). Furthermore, we demonstrated that the catalytic activity of Au/TiO<sub>2</sub> increases exponentially with increasing light intensity, which indicated the presence of a photothermal contributor. In dark, however, both Au/TiO<sub>2</sub> catalysts solely produced CH<sub>4</sub> at the same catalyst bed temperature (160 °C). We propose that the difference in selectivity is caused by the promotion of CO desorption through charge transfer of plasmon generated charges (as a non-thermal contributor).https://www.mdpi.com/2079-4991/12/23/4153plasmonicnanoparticlegoldtitaniacatalysisCCU |
| spellingShingle | Jordi Volders Ken Elen Arno Raes Rajeshreddy Ninakanti An-Sofie Kelchtermans Francesc Sastre An Hardy Pegie Cool Sammy W. Verbruggen Pascal Buskens Marlies K. Van Bael Sunlight-Powered Reverse Water Gas Shift Reaction Catalysed by Plasmonic Au/TiO<sub>2</sub> Nanocatalysts: Effects of Au Particle Size on the Activity and Selectivity Nanomaterials plasmonic nanoparticle gold titania catalysis CCU |
| title | Sunlight-Powered Reverse Water Gas Shift Reaction Catalysed by Plasmonic Au/TiO<sub>2</sub> Nanocatalysts: Effects of Au Particle Size on the Activity and Selectivity |
| title_full | Sunlight-Powered Reverse Water Gas Shift Reaction Catalysed by Plasmonic Au/TiO<sub>2</sub> Nanocatalysts: Effects of Au Particle Size on the Activity and Selectivity |
| title_fullStr | Sunlight-Powered Reverse Water Gas Shift Reaction Catalysed by Plasmonic Au/TiO<sub>2</sub> Nanocatalysts: Effects of Au Particle Size on the Activity and Selectivity |
| title_full_unstemmed | Sunlight-Powered Reverse Water Gas Shift Reaction Catalysed by Plasmonic Au/TiO<sub>2</sub> Nanocatalysts: Effects of Au Particle Size on the Activity and Selectivity |
| title_short | Sunlight-Powered Reverse Water Gas Shift Reaction Catalysed by Plasmonic Au/TiO<sub>2</sub> Nanocatalysts: Effects of Au Particle Size on the Activity and Selectivity |
| title_sort | sunlight powered reverse water gas shift reaction catalysed by plasmonic au tio sub 2 sub nanocatalysts effects of au particle size on the activity and selectivity |
| topic | plasmonic nanoparticle gold titania catalysis CCU |
| url | https://www.mdpi.com/2079-4991/12/23/4153 |
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