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Metal-Free N-Doped Carbons for Solvent-Less CO(2) Fixation Reactions: A Shrimp Shell Valorization Opportunity

[Image: see text] High anthropogenic CO(2) emissions are among the main causes of climate change. Herein, we investigate the use of CO(2) for the synthesis of organic cyclic carbonates on metal-free nitrogen-doped carbon catalysts obtained from chitosan, chitin, and shrimp shell wastes, both in batc...

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Autores principales: Polidoro, Daniele, Perosa, Alvise, Rodríguez-Castellón, Enrique, Canton, Patrizia, Castoldi, Lidia, Rodríguez-Padrón, Daily, Selva, Maurizio
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2022
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9942530/
https://www.ncbi.nlm.nih.gov/pubmed/36845462
http://dx.doi.org/10.1021/acssuschemeng.2c04443
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author Polidoro, Daniele
Perosa, Alvise
Rodríguez-Castellón, Enrique
Canton, Patrizia
Castoldi, Lidia
Rodríguez-Padrón, Daily
Selva, Maurizio
author_facet Polidoro, Daniele
Perosa, Alvise
Rodríguez-Castellón, Enrique
Canton, Patrizia
Castoldi, Lidia
Rodríguez-Padrón, Daily
Selva, Maurizio
author_sort Polidoro, Daniele
collection PubMed
description [Image: see text] High anthropogenic CO(2) emissions are among the main causes of climate change. Herein, we investigate the use of CO(2) for the synthesis of organic cyclic carbonates on metal-free nitrogen-doped carbon catalysts obtained from chitosan, chitin, and shrimp shell wastes, both in batch and in continuous flow (CF). The catalysts were characterized by N(2) physisorption, CO(2)-temperature-programmed desorption, X-ray photoelectron spectroscopy, scanning electron microscopy, and CNHS elemental analysis, and all reactivity tests were run in the absence of solvents. Under batch conditions, the catalyst obtained by calcination of chitin exhibited excellent performance in the conversion of epichlorohydrin (selected as a model epoxide), resulting in the corresponding cyclic carbonate with 96% selectivity at complete conversion, at 150 °C and 30 bar CO(2), for 4 h. On the other hand, in a CF regime, a quantitative conversion and a carbonate selectivity >99% were achieved at 150 °C, by using the catalyst obtained from shrimp waste. Remarkably, the material displayed an outstanding stability over a reaction run time of 180 min. The robustness of the synthetized catalysts was confirmed by their good operational stability and reusability: ca. (75 ± 3)% of the initial conversion was achieved/retained by all systems, after six recycles. Also, additional batch experiments proved that the catalysts were successful on different terminal and internal epoxides.
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spelling pubmed-99425302023-02-22 Metal-Free N-Doped Carbons for Solvent-Less CO(2) Fixation Reactions: A Shrimp Shell Valorization Opportunity Polidoro, Daniele Perosa, Alvise Rodríguez-Castellón, Enrique Canton, Patrizia Castoldi, Lidia Rodríguez-Padrón, Daily Selva, Maurizio ACS Sustain Chem Eng [Image: see text] High anthropogenic CO(2) emissions are among the main causes of climate change. Herein, we investigate the use of CO(2) for the synthesis of organic cyclic carbonates on metal-free nitrogen-doped carbon catalysts obtained from chitosan, chitin, and shrimp shell wastes, both in batch and in continuous flow (CF). The catalysts were characterized by N(2) physisorption, CO(2)-temperature-programmed desorption, X-ray photoelectron spectroscopy, scanning electron microscopy, and CNHS elemental analysis, and all reactivity tests were run in the absence of solvents. Under batch conditions, the catalyst obtained by calcination of chitin exhibited excellent performance in the conversion of epichlorohydrin (selected as a model epoxide), resulting in the corresponding cyclic carbonate with 96% selectivity at complete conversion, at 150 °C and 30 bar CO(2), for 4 h. On the other hand, in a CF regime, a quantitative conversion and a carbonate selectivity >99% were achieved at 150 °C, by using the catalyst obtained from shrimp waste. Remarkably, the material displayed an outstanding stability over a reaction run time of 180 min. The robustness of the synthetized catalysts was confirmed by their good operational stability and reusability: ca. (75 ± 3)% of the initial conversion was achieved/retained by all systems, after six recycles. Also, additional batch experiments proved that the catalysts were successful on different terminal and internal epoxides. American Chemical Society 2022-09-29 /pmc/articles/PMC9942530/ /pubmed/36845462 http://dx.doi.org/10.1021/acssuschemeng.2c04443 Text en © 2022 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 Polidoro, Daniele
Perosa, Alvise
Rodríguez-Castellón, Enrique
Canton, Patrizia
Castoldi, Lidia
Rodríguez-Padrón, Daily
Selva, Maurizio
Metal-Free N-Doped Carbons for Solvent-Less CO(2) Fixation Reactions: A Shrimp Shell Valorization Opportunity
title Metal-Free N-Doped Carbons for Solvent-Less CO(2) Fixation Reactions: A Shrimp Shell Valorization Opportunity
title_full Metal-Free N-Doped Carbons for Solvent-Less CO(2) Fixation Reactions: A Shrimp Shell Valorization Opportunity
title_fullStr Metal-Free N-Doped Carbons for Solvent-Less CO(2) Fixation Reactions: A Shrimp Shell Valorization Opportunity
title_full_unstemmed Metal-Free N-Doped Carbons for Solvent-Less CO(2) Fixation Reactions: A Shrimp Shell Valorization Opportunity
title_short Metal-Free N-Doped Carbons for Solvent-Less CO(2) Fixation Reactions: A Shrimp Shell Valorization Opportunity
title_sort metal-free n-doped carbons for solvent-less co(2) fixation reactions: a shrimp shell valorization opportunity
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9942530/
https://www.ncbi.nlm.nih.gov/pubmed/36845462
http://dx.doi.org/10.1021/acssuschemeng.2c04443
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