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Pulsed Photothermal Heterogeneous Catalysis
[Image: see text] Anthropogenic climate change urgently calls for the greening and intensification of the chemical industry. Most chemical reactors make use of catalysts to increase their conversion yields, but their operation at steady-state temperatures limits their rate, selectivity, and energy e...
Autores principales: | , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Chemical Society
2023
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Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9990069/ https://www.ncbi.nlm.nih.gov/pubmed/36910867 http://dx.doi.org/10.1021/acscatal.2c05435 |
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author | Baldi, Andrea Askes, Sven H. C. |
author_facet | Baldi, Andrea Askes, Sven H. C. |
author_sort | Baldi, Andrea |
collection | PubMed |
description | [Image: see text] Anthropogenic climate change urgently calls for the greening and intensification of the chemical industry. Most chemical reactors make use of catalysts to increase their conversion yields, but their operation at steady-state temperatures limits their rate, selectivity, and energy efficiency. Here, we show how to break such a steady-state paradigm using ultrashort light pulses and photothermal nanoparticle arrays to modulate the temperature of catalytic sites at timescales typical of chemical processes. Using heat dissipation and time-dependent microkinetic modeling for a number of catalytic landscapes, we numerically demonstrate that pulsed photothermal catalysis can result in a favorable, dynamic mode of operation with higher energy efficiency, higher catalyst activity than for any steady-state temperature, reactor operation at room temperature, resilience against catalyst poisons, and access to adsorbed reagent distributions that are normally out of reach. Our work identifies the key experimental parameters controlling reaction rates in pulsed heterogeneous catalysis and provides specific recommendations to explore its potential in real experiments, paving the way to a more energy-efficient and process-intensive operation of catalytic reactors. |
format | Online Article Text |
id | pubmed-9990069 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2023 |
publisher | American Chemical Society |
record_format | MEDLINE/PubMed |
spelling | pubmed-99900692023-03-08 Pulsed Photothermal Heterogeneous Catalysis Baldi, Andrea Askes, Sven H. C. ACS Catal [Image: see text] Anthropogenic climate change urgently calls for the greening and intensification of the chemical industry. Most chemical reactors make use of catalysts to increase their conversion yields, but their operation at steady-state temperatures limits their rate, selectivity, and energy efficiency. Here, we show how to break such a steady-state paradigm using ultrashort light pulses and photothermal nanoparticle arrays to modulate the temperature of catalytic sites at timescales typical of chemical processes. Using heat dissipation and time-dependent microkinetic modeling for a number of catalytic landscapes, we numerically demonstrate that pulsed photothermal catalysis can result in a favorable, dynamic mode of operation with higher energy efficiency, higher catalyst activity than for any steady-state temperature, reactor operation at room temperature, resilience against catalyst poisons, and access to adsorbed reagent distributions that are normally out of reach. Our work identifies the key experimental parameters controlling reaction rates in pulsed heterogeneous catalysis and provides specific recommendations to explore its potential in real experiments, paving the way to a more energy-efficient and process-intensive operation of catalytic reactors. American Chemical Society 2023-02-22 /pmc/articles/PMC9990069/ /pubmed/36910867 http://dx.doi.org/10.1021/acscatal.2c05435 Text en © 2023 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/). |
spellingShingle | Baldi, Andrea Askes, Sven H. C. Pulsed Photothermal Heterogeneous Catalysis |
title | Pulsed Photothermal
Heterogeneous Catalysis |
title_full | Pulsed Photothermal
Heterogeneous Catalysis |
title_fullStr | Pulsed Photothermal
Heterogeneous Catalysis |
title_full_unstemmed | Pulsed Photothermal
Heterogeneous Catalysis |
title_short | Pulsed Photothermal
Heterogeneous Catalysis |
title_sort | pulsed photothermal
heterogeneous catalysis |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9990069/ https://www.ncbi.nlm.nih.gov/pubmed/36910867 http://dx.doi.org/10.1021/acscatal.2c05435 |
work_keys_str_mv | AT baldiandrea pulsedphotothermalheterogeneouscatalysis AT askessvenhc pulsedphotothermalheterogeneouscatalysis |