Synthesis of silver and gold nanoparticles-enzyme-polymer conjugate hybrids as dual-activity catalysts for chemoenzymatic cascade reactions
Novel hybrids containing silver or gold nanoparticles have been synthesized in aqueous media and at room temperature using enzymes or tailor-made enzyme-polymer conjugates, which directly induced the formation of inorganic silver or gold species. The choice of pH, protein, or bioconjugate strongly a...
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Royal Society of Chemistry
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ftunivhelsihelda:oai:helda.helsinki.fi:10138/357129 2024-01-07T09:38:33+01:00 Synthesis of silver and gold nanoparticles-enzyme-polymer conjugate hybrids as dual-activity catalysts for chemoenzymatic cascade reactions Naapuri, Janne M. Losada-Garcia, Noelia Deska, Jan Palomo, Jose M. Department of Chemistry 2023-04-19T21:37:12Z 15 application/pdf http://hdl.handle.net/10138/357129 eng eng Royal Society of Chemistry 10.1039/d2nr00361a The authors thank the support of the Spanish National Research Council (CSIC). We gratefully acknowledge financial support by the Suomen Akatemia (grant numbers 298250 & 324976, J. D.), the COST action CA15106 (CHAOS) and Finnish Foundation for Technology Promotion. We also thank Ramiro Martinez from Novozymes. Naapuri , J M , Losada-Garcia , N , Deska , J & Palomo , J M 2022 , ' Synthesis of silver and gold nanoparticles-enzyme-polymer conjugate hybrids as dual-activity catalysts for chemoenzymatic cascade reactions ' , Nanoscale , vol. 14 , no. 15 , pp. 5701-5715 . https://doi.org/10.1039/d2nr00361a abb58b06-8142-42c9-9f9e-e3344f46e106 http://hdl.handle.net/10138/357129 000773657700001 cc_by_nc openAccess info:eu-repo/semantics/openAccess 116 Chemical sciences Article publishedVersion 2023 ftunivhelsihelda 2023-12-14T00:02:31Z Novel hybrids containing silver or gold nanoparticles have been synthesized in aqueous media and at room temperature using enzymes or tailor-made enzyme-polymer conjugates, which directly induced the formation of inorganic silver or gold species. The choice of pH, protein, or bioconjugate strongly affected the final metallic nanoparticles hybrid formation. Using Candida antarctica lipase (CALB) in a solution, nanobiohybrids containing Ag2O nanoparticles of 9 nm average diameter were obtained. The use of tailor-made bioconjugates, for example, the CALB modified with dextran-aspartic acid polymer (Dext6kDa), resulted in a nanobiohybrid containing smaller Ag(0)/Ag2O nanoparticles. In the case of nanobiohybrids based on gold, Au(0) species were found in all cases. The Au-CALB hybrid contained spherical nanoparticles with 18 nm average diameter size, with a minor range of larger ones (>100 nm) while the AuNPs-CALB-Dext6kDa hybrid was formed by much smaller nanoparticles (9 nm, minor range of 22 nm), and also nanorods of 20-30/40-50 nm length. Using Thermomyces lanuginosus lipase (TLL), apart from the nanoparticle formation, nanoflowers with a diameter range of 100-200 nm were obtained. All nanobiohybrids maintained (dual) enzymatic and metallic activities. For instance, these nanobiohybrids exhibited exquisite dual-activity for hydrolysis/cycloisomerization cascades starting from allenic acetates. By merging the transition metal reactivity with the inherent lipase catalysis, allenic acetates directly converted to the corresponding O-heterocycles in enantiopure form catalysed by AgNPs-CALB-Dext6kDa, taking advantage of a kinetic resolution/cyclization pathway. These results showed the high applicability of these novel hybrids, offering new opportunities for the design of novel reaction cascades. Peer reviewed Article in Journal/Newspaper Antarc* Antarctica HELDA – University of Helsinki Open Repository Nanoscale 14 15 5701 5715 |
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HELDA – University of Helsinki Open Repository |
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ftunivhelsihelda |
language |
English |
topic |
116 Chemical sciences |
spellingShingle |
116 Chemical sciences Naapuri, Janne M. Losada-Garcia, Noelia Deska, Jan Palomo, Jose M. Synthesis of silver and gold nanoparticles-enzyme-polymer conjugate hybrids as dual-activity catalysts for chemoenzymatic cascade reactions |
topic_facet |
116 Chemical sciences |
description |
Novel hybrids containing silver or gold nanoparticles have been synthesized in aqueous media and at room temperature using enzymes or tailor-made enzyme-polymer conjugates, which directly induced the formation of inorganic silver or gold species. The choice of pH, protein, or bioconjugate strongly affected the final metallic nanoparticles hybrid formation. Using Candida antarctica lipase (CALB) in a solution, nanobiohybrids containing Ag2O nanoparticles of 9 nm average diameter were obtained. The use of tailor-made bioconjugates, for example, the CALB modified with dextran-aspartic acid polymer (Dext6kDa), resulted in a nanobiohybrid containing smaller Ag(0)/Ag2O nanoparticles. In the case of nanobiohybrids based on gold, Au(0) species were found in all cases. The Au-CALB hybrid contained spherical nanoparticles with 18 nm average diameter size, with a minor range of larger ones (>100 nm) while the AuNPs-CALB-Dext6kDa hybrid was formed by much smaller nanoparticles (9 nm, minor range of 22 nm), and also nanorods of 20-30/40-50 nm length. Using Thermomyces lanuginosus lipase (TLL), apart from the nanoparticle formation, nanoflowers with a diameter range of 100-200 nm were obtained. All nanobiohybrids maintained (dual) enzymatic and metallic activities. For instance, these nanobiohybrids exhibited exquisite dual-activity for hydrolysis/cycloisomerization cascades starting from allenic acetates. By merging the transition metal reactivity with the inherent lipase catalysis, allenic acetates directly converted to the corresponding O-heterocycles in enantiopure form catalysed by AgNPs-CALB-Dext6kDa, taking advantage of a kinetic resolution/cyclization pathway. These results showed the high applicability of these novel hybrids, offering new opportunities for the design of novel reaction cascades. Peer reviewed |
author2 |
Department of Chemistry |
format |
Article in Journal/Newspaper |
author |
Naapuri, Janne M. Losada-Garcia, Noelia Deska, Jan Palomo, Jose M. |
author_facet |
Naapuri, Janne M. Losada-Garcia, Noelia Deska, Jan Palomo, Jose M. |
author_sort |
Naapuri, Janne M. |
title |
Synthesis of silver and gold nanoparticles-enzyme-polymer conjugate hybrids as dual-activity catalysts for chemoenzymatic cascade reactions |
title_short |
Synthesis of silver and gold nanoparticles-enzyme-polymer conjugate hybrids as dual-activity catalysts for chemoenzymatic cascade reactions |
title_full |
Synthesis of silver and gold nanoparticles-enzyme-polymer conjugate hybrids as dual-activity catalysts for chemoenzymatic cascade reactions |
title_fullStr |
Synthesis of silver and gold nanoparticles-enzyme-polymer conjugate hybrids as dual-activity catalysts for chemoenzymatic cascade reactions |
title_full_unstemmed |
Synthesis of silver and gold nanoparticles-enzyme-polymer conjugate hybrids as dual-activity catalysts for chemoenzymatic cascade reactions |
title_sort |
synthesis of silver and gold nanoparticles-enzyme-polymer conjugate hybrids as dual-activity catalysts for chemoenzymatic cascade reactions |
publisher |
Royal Society of Chemistry |
publishDate |
2023 |
url |
http://hdl.handle.net/10138/357129 |
genre |
Antarc* Antarctica |
genre_facet |
Antarc* Antarctica |
op_relation |
10.1039/d2nr00361a The authors thank the support of the Spanish National Research Council (CSIC). We gratefully acknowledge financial support by the Suomen Akatemia (grant numbers 298250 & 324976, J. D.), the COST action CA15106 (CHAOS) and Finnish Foundation for Technology Promotion. We also thank Ramiro Martinez from Novozymes. Naapuri , J M , Losada-Garcia , N , Deska , J & Palomo , J M 2022 , ' Synthesis of silver and gold nanoparticles-enzyme-polymer conjugate hybrids as dual-activity catalysts for chemoenzymatic cascade reactions ' , Nanoscale , vol. 14 , no. 15 , pp. 5701-5715 . https://doi.org/10.1039/d2nr00361a abb58b06-8142-42c9-9f9e-e3344f46e106 http://hdl.handle.net/10138/357129 000773657700001 |
op_rights |
cc_by_nc openAccess info:eu-repo/semantics/openAccess |
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Nanoscale |
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14 |
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5701 |
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5715 |
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