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The influence of phase purity on the stability of Pt/LaAlO3 catalysts in the aqueous phase reforming of glycerol
Aqueous phase reforming (APR) of waste oxygenates offers the potential for sustainable hydrogen production. However, catalyst stability remains elusive, due to the aggressive hydrothermal conditions employed. Herein, we show that the catalytic performance and stability of Pt supported on LaAlO3 cata...
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| Format: | Default Article |
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2022
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| Online Access: | https://hdl.handle.net/2134/21518064.v1 |
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| _version_ | 1818165688336908288 |
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| author | Donald Inns Xuetong Pei Zhaoxia Zhou Daniel J. M. Irving Simon Kondrat |
| author_facet | Donald Inns Xuetong Pei Zhaoxia Zhou Daniel J. M. Irving Simon Kondrat |
| author_sort | Donald Inns (5491154) |
| collection | Figshare |
| description | Aqueous phase reforming (APR) of waste oxygenates offers the potential for sustainable hydrogen production. However, catalyst stability remains elusive, due to the aggressive hydrothermal conditions employed. Herein, we show that the catalytic performance and stability of Pt supported on LaAlO3 catalysts for glycerol APR is strongly influenced by the phase purity of LaAlO3. Calcination of the support at 700 °C produces the LaAlO3 perovskite phase and an amorphous lanthanum carbonate phase, which can be removed by calcination at higher temperature. Catalysts comprised of phase pure LaAlO3 were notably more active, with a support calcination temperature of 1100 °C resulting in 20.4% glycerol conversion (TOF 686 h−1) in a 2 h batch reaction. Interestingly, all the catalysts, regardless of LaAlO3 phase purity, eventually transform into Pt/LaCO3OH-AlO(OH) during reaction, but only in the presence of evolved carbon dioxide, itself produced from glycerol reforming. Studies using simulated reaction products showed that organic acid products (lactic acid), in the absence of CO2, facilitated La leaching and loss of crystallinity. A carbonate source (CO2) is essential to limit La leaching and form stable Pt/LaCO3OH. Pt supported on LaCO3OH and AlO(OH) are stable and active catalysts during APR reactions. Yet, the rate of perovskite phase decomposition strongly influences the final catalyst performance, with the initially phase impure LaAlO3 decomposing too quickly to facilitate Pt redistribution. LaAlO3 calcined at higher temperatures evolved more slowly and consequently produced more active catalysts. |
| format | Default Article |
| id | rr-article-21518064 |
| institution | Loughborough University |
| publishDate | 2022 |
| record_format | Figshare |
| spelling | rr-article-215180642022-10-29T00:00:00Z The influence of phase purity on the stability of Pt/LaAlO3 catalysts in the aqueous phase reforming of glycerol Donald Inns (5491154) Xuetong Pei (9173159) Zhaoxia Zhou (1255245) Daniel J. M. Irving (14081599) Simon Kondrat (4394224) Macromolecular and materials chemistry Materials engineering Hydrogen production Catalyst stability Perovskite supported catalysts APR <p>Aqueous phase reforming (APR) of waste oxygenates offers the potential for sustainable hydrogen production. However, catalyst stability remains elusive, due to the aggressive hydrothermal conditions employed. Herein, we show that the catalytic performance and stability of Pt supported on LaAlO<sub>3</sub> catalysts for glycerol APR is strongly influenced by the phase purity of LaAlO<sub>3</sub>. Calcination of the support at 700 °C produces the LaAlO<sub>3</sub> perovskite phase and an amorphous lanthanum carbonate phase, which can be removed by calcination at higher temperature. Catalysts comprised of phase pure LaAlO<sub>3</sub> were notably more active, with a support calcination temperature of 1100 °C resulting in 20.4% glycerol conversion (TOF 686 h−1) in a 2 h batch reaction. Interestingly, all the catalysts, regardless of LaAlO<sub>3</sub> phase purity, eventually transform into Pt/LaCO<sub>3</sub>OH-AlO(OH) during reaction, but only in the presence of evolved carbon dioxide, itself produced from glycerol reforming. Studies using simulated reaction products showed that organic acid products (lactic acid), in the absence of CO<sub>2</sub>, facilitated La leaching and loss of crystallinity. A carbonate source (CO<sub>2</sub>) is essential to limit La leaching and form stable Pt/LaCO<sub>3</sub>OH. Pt supported on LaCO<sub>3</sub>OH and AlO(OH) are stable and active catalysts during APR reactions. Yet, the rate of perovskite phase decomposition strongly influences the final catalyst performance, with the initially phase impure LaAlO<sub>3</sub> decomposing too quickly to facilitate Pt redistribution. LaAlO<sub>3</sub> calcined at higher temperatures evolved more slowly and consequently produced more active catalysts.</p> 2022-10-29T00:00:00Z Text Journal contribution 2134/21518064.v1 https://figshare.com/articles/journal_contribution/The_influence_of_phase_purity_on_the_stability_of_Pt_LaAlO3_catalysts_in_the_aqueous_phase_reforming_of_glycerol/21518064 CC BY 4.0 |
| spellingShingle | Macromolecular and materials chemistry Materials engineering Hydrogen production Catalyst stability Perovskite supported catalysts APR Donald Inns Xuetong Pei Zhaoxia Zhou Daniel J. M. Irving Simon Kondrat The influence of phase purity on the stability of Pt/LaAlO3 catalysts in the aqueous phase reforming of glycerol |
| title | The influence of phase purity on the stability of Pt/LaAlO3 catalysts in the aqueous phase reforming of glycerol |
| title_full | The influence of phase purity on the stability of Pt/LaAlO3 catalysts in the aqueous phase reforming of glycerol |
| title_fullStr | The influence of phase purity on the stability of Pt/LaAlO3 catalysts in the aqueous phase reforming of glycerol |
| title_full_unstemmed | The influence of phase purity on the stability of Pt/LaAlO3 catalysts in the aqueous phase reforming of glycerol |
| title_short | The influence of phase purity on the stability of Pt/LaAlO3 catalysts in the aqueous phase reforming of glycerol |
| title_sort | influence of phase purity on the stability of pt/laalo3 catalysts in the aqueous phase reforming of glycerol |
| topic | Macromolecular and materials chemistry Materials engineering Hydrogen production Catalyst stability Perovskite supported catalysts APR |
| url | https://hdl.handle.net/2134/21518064.v1 |