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Nuclear Waste and Biocatalysis: A Sustainable Liaison?

[Image: see text] It is well-known that energy-rich radiation induces water splitting, eventually yielding hydrogen peroxide. Synthetic applications, however, are scarce and to the best of our knowledge, the combination of radioactivity with enzyme-catalysis has not been considered yet. Peroxygenase...

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Autores principales: Zhang, Wuyuan, Liu, Huanhuan, van Schie, Morten M. C. H., Hagedoorn, Peter-Leon, Alcalde, Miguel, Denkova, Antonia G., Djanashvili, Kristina, Hollmann, Frank
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2020
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7723303/
https://www.ncbi.nlm.nih.gov/pubmed/33312749
http://dx.doi.org/10.1021/acscatal.0c03059
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author Zhang, Wuyuan
Liu, Huanhuan
van Schie, Morten M. C. H.
Hagedoorn, Peter-Leon
Alcalde, Miguel
Denkova, Antonia G.
Djanashvili, Kristina
Hollmann, Frank
author_facet Zhang, Wuyuan
Liu, Huanhuan
van Schie, Morten M. C. H.
Hagedoorn, Peter-Leon
Alcalde, Miguel
Denkova, Antonia G.
Djanashvili, Kristina
Hollmann, Frank
author_sort Zhang, Wuyuan
collection PubMed
description [Image: see text] It is well-known that energy-rich radiation induces water splitting, eventually yielding hydrogen peroxide. Synthetic applications, however, are scarce and to the best of our knowledge, the combination of radioactivity with enzyme-catalysis has not been considered yet. Peroxygenases utilize H(2)O(2) as an oxidant to promote highly selective oxyfunctionalization reactions but are also irreversibly inactivated in the presence of too high H(2)O(2) concentrations. Therefore, there is a need for efficient in situ H(2)O(2) generation methods. Here, we show that radiolytic water splitting can be used to promote specific biocatalytic oxyfunctionalization reactions. Parameters influencing the efficiency of the reaction and current limitations are shown. Particularly, oxidative inactivation of the biocatalyst by hydroxyl radicals influences the robustness of the overall reaction. Radical scavengers can alleviate this issue, but eventually, physical separation of the enzymes from the ionizing radiation will be necessary to achieve robust reaction schemes. We demonstrate that nuclear waste can also be used to drive selective, peroxygenase-catalyzed oxyfunctionalization reactions, challenging our view on nuclear waste in terms of sustainability.
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spelling pubmed-77233032020-12-09 Nuclear Waste and Biocatalysis: A Sustainable Liaison? Zhang, Wuyuan Liu, Huanhuan van Schie, Morten M. C. H. Hagedoorn, Peter-Leon Alcalde, Miguel Denkova, Antonia G. Djanashvili, Kristina Hollmann, Frank ACS Catal [Image: see text] It is well-known that energy-rich radiation induces water splitting, eventually yielding hydrogen peroxide. Synthetic applications, however, are scarce and to the best of our knowledge, the combination of radioactivity with enzyme-catalysis has not been considered yet. Peroxygenases utilize H(2)O(2) as an oxidant to promote highly selective oxyfunctionalization reactions but are also irreversibly inactivated in the presence of too high H(2)O(2) concentrations. Therefore, there is a need for efficient in situ H(2)O(2) generation methods. Here, we show that radiolytic water splitting can be used to promote specific biocatalytic oxyfunctionalization reactions. Parameters influencing the efficiency of the reaction and current limitations are shown. Particularly, oxidative inactivation of the biocatalyst by hydroxyl radicals influences the robustness of the overall reaction. Radical scavengers can alleviate this issue, but eventually, physical separation of the enzymes from the ionizing radiation will be necessary to achieve robust reaction schemes. We demonstrate that nuclear waste can also be used to drive selective, peroxygenase-catalyzed oxyfunctionalization reactions, challenging our view on nuclear waste in terms of sustainability. American Chemical Society 2020-11-20 2020-12-04 /pmc/articles/PMC7723303/ /pubmed/33312749 http://dx.doi.org/10.1021/acscatal.0c03059 Text en © 2020 American Chemical Society This is an open access article published under a Creative Commons Non-Commercial No Derivative Works (CC-BY-NC-ND) Attribution License (http://pubs.acs.org/page/policy/authorchoice_ccbyncnd_termsofuse.html) , which permits copying and redistribution of the article, and creation of adaptations, all for non-commercial purposes.
spellingShingle Zhang, Wuyuan
Liu, Huanhuan
van Schie, Morten M. C. H.
Hagedoorn, Peter-Leon
Alcalde, Miguel
Denkova, Antonia G.
Djanashvili, Kristina
Hollmann, Frank
Nuclear Waste and Biocatalysis: A Sustainable Liaison?
title Nuclear Waste and Biocatalysis: A Sustainable Liaison?
title_full Nuclear Waste and Biocatalysis: A Sustainable Liaison?
title_fullStr Nuclear Waste and Biocatalysis: A Sustainable Liaison?
title_full_unstemmed Nuclear Waste and Biocatalysis: A Sustainable Liaison?
title_short Nuclear Waste and Biocatalysis: A Sustainable Liaison?
title_sort nuclear waste and biocatalysis: a sustainable liaison?
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7723303/
https://www.ncbi.nlm.nih.gov/pubmed/33312749
http://dx.doi.org/10.1021/acscatal.0c03059
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