Electrodeposited Ni-rich Ni-Pt mesoporous nanowires for selective and efficient formic acid-assisted hydrogenation of levulinic acid to γ-valerolactone
In pursuit of friendlier conditions for the preparation of high-value biochemicals, we developed a catalytic synthesis of -valerolactone by levulinic acid hydrogenation with formic acid as the hydrogen source. Both levulinic and formic acid are intermediate products in the biomass transformation pr...
| Autores: | , , , |
|---|---|
| Tipo de documento: | artigo |
| Estado: | Versión aceptada para publicación |
| Data de publicação: | 2021 |
| País: | España |
| Recursos: | Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya) |
| Repositório: | Recercat. Dipósit de la Recerca de Catalunya |
| OAI Identifier: | oai:recercat.cat:2445/176706 |
| Acesso em linha: | https://hdl.handle.net/2445/176706 |
| Access Level: | Acceso aberto |
| Palavra-chave: | Platí Catàlisi Hidrogenació Platinum Catalysis Hydrogenation |
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Electrodeposited Ni-rich Ni-Pt mesoporous nanowires for selective and efficient formic acid-assisted hydrogenation of levulinic acid to γ-valerolactoneSerrà i Ramos, AlbertArtal López, RaúlPhilippe, LaetitiaGómez, ElviraPlatíCatàlisiHidrogenacióPlatinumCatalysisHydrogenationIn pursuit of friendlier conditions for the preparation of high-value biochemicals, we developed a catalytic synthesis of -valerolactone by levulinic acid hydrogenation with formic acid as the hydrogen source. Both levulinic and formic acid are intermediate products in the biomass transformation processes. The objective of the work is two-fold; development of a novel approach for milder synthesis conditions to produce -valerolactone and the reduction of the economic cost of the catalyst. Ni-rich Ni-Pt mesoporous nanowires were synthesized in an aqueous medium using a combined hard-soft template-assisted electrodeposition method, in which porous polycarbonate membranes controlled the shape, and the pluronic P-123 copolymer served as the porogen agent. The electrodeposition conditions selected favored nickel deposition and generated nanowires with nickel percentages above the 75 at. %. The increase in deposition potential favored nickel deposition. However, it was detrimental for the porous diameter, because the mesoporous structure is promoted by the presence of the platinum-rich micelles near the substrate, which is not favored at the more negative potentials. The prepared catalysts promoted the complete transformation to -valerolactone in a yield of around 99% and proceeded with the absence of by-products. The couple temperature and reaction time were optimized considering the energy cost. The threshold operational temperature was established at 140 ºC, at which, 120 minutes were sufficient for attaining the complete transformation. Working temperatures below 140 ºC rendered the reaction completion difficult. The Ni78Pt22 nanowires exhibited excellent reusability, with minimal nickel leaching into the reaction mixture, whereas those with higher nickel contents showed corrosion.American Chemical Society2021202220212021info:eu-repo/semantics/articleinfo:eu-repo/semantics/acceptedVersion12 p.application/pdfhttps://hdl.handle.net/2445/176706Articles publicats en revistes (Ciència dels Materials i Química Física)reponame:Recercat. Dipósit de la Recerca de Catalunyainstname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)InglésVersió postprint del document publicat a: https://doi.org/10.1021/acs.langmuir.1c00461Langmuir, 2021, vol. 37, p. 4666-4677https://doi.org/10.1021/acs.langmuir.1c00461(c) American Chemical Society , 2021info:eu-repo/semantics/openAccessoai:recercat.cat:2445/1767062026-05-29T05:05:01Z |
| dc.title.none.fl_str_mv |
Electrodeposited Ni-rich Ni-Pt mesoporous nanowires for selective and efficient formic acid-assisted hydrogenation of levulinic acid to γ-valerolactone |
| title |
Electrodeposited Ni-rich Ni-Pt mesoporous nanowires for selective and efficient formic acid-assisted hydrogenation of levulinic acid to γ-valerolactone |
| spellingShingle |
Electrodeposited Ni-rich Ni-Pt mesoporous nanowires for selective and efficient formic acid-assisted hydrogenation of levulinic acid to γ-valerolactone Serrà i Ramos, Albert Platí Catàlisi Hidrogenació Platinum Catalysis Hydrogenation |
| title_short |
Electrodeposited Ni-rich Ni-Pt mesoporous nanowires for selective and efficient formic acid-assisted hydrogenation of levulinic acid to γ-valerolactone |
| title_full |
Electrodeposited Ni-rich Ni-Pt mesoporous nanowires for selective and efficient formic acid-assisted hydrogenation of levulinic acid to γ-valerolactone |
| title_fullStr |
Electrodeposited Ni-rich Ni-Pt mesoporous nanowires for selective and efficient formic acid-assisted hydrogenation of levulinic acid to γ-valerolactone |
| title_full_unstemmed |
Electrodeposited Ni-rich Ni-Pt mesoporous nanowires for selective and efficient formic acid-assisted hydrogenation of levulinic acid to γ-valerolactone |
| title_sort |
Electrodeposited Ni-rich Ni-Pt mesoporous nanowires for selective and efficient formic acid-assisted hydrogenation of levulinic acid to γ-valerolactone |
| dc.creator.none.fl_str_mv |
Serrà i Ramos, Albert Artal López, Raúl Philippe, Laetitia Gómez, Elvira |
| author |
Serrà i Ramos, Albert |
| author_facet |
Serrà i Ramos, Albert Artal López, Raúl Philippe, Laetitia Gómez, Elvira |
| author_role |
author |
| author2 |
Artal López, Raúl Philippe, Laetitia Gómez, Elvira |
| author2_role |
author author author |
| dc.subject.none.fl_str_mv |
Platí Catàlisi Hidrogenació Platinum Catalysis Hydrogenation |
| topic |
Platí Catàlisi Hidrogenació Platinum Catalysis Hydrogenation |
| description |
In pursuit of friendlier conditions for the preparation of high-value biochemicals, we developed a catalytic synthesis of -valerolactone by levulinic acid hydrogenation with formic acid as the hydrogen source. Both levulinic and formic acid are intermediate products in the biomass transformation processes. The objective of the work is two-fold; development of a novel approach for milder synthesis conditions to produce -valerolactone and the reduction of the economic cost of the catalyst. Ni-rich Ni-Pt mesoporous nanowires were synthesized in an aqueous medium using a combined hard-soft template-assisted electrodeposition method, in which porous polycarbonate membranes controlled the shape, and the pluronic P-123 copolymer served as the porogen agent. The electrodeposition conditions selected favored nickel deposition and generated nanowires with nickel percentages above the 75 at. %. The increase in deposition potential favored nickel deposition. However, it was detrimental for the porous diameter, because the mesoporous structure is promoted by the presence of the platinum-rich micelles near the substrate, which is not favored at the more negative potentials. The prepared catalysts promoted the complete transformation to -valerolactone in a yield of around 99% and proceeded with the absence of by-products. The couple temperature and reaction time were optimized considering the energy cost. The threshold operational temperature was established at 140 ºC, at which, 120 minutes were sufficient for attaining the complete transformation. Working temperatures below 140 ºC rendered the reaction completion difficult. The Ni78Pt22 nanowires exhibited excellent reusability, with minimal nickel leaching into the reaction mixture, whereas those with higher nickel contents showed corrosion. |
| publishDate |
2021 |
| dc.date.none.fl_str_mv |
2021 2021 2021 2022 |
| dc.type.none.fl_str_mv |
info:eu-repo/semantics/article info:eu-repo/semantics/acceptedVersion |
| format |
article |
| status_str |
acceptedVersion |
| dc.identifier.none.fl_str_mv |
https://hdl.handle.net/2445/176706 |
| url |
https://hdl.handle.net/2445/176706 |
| dc.language.none.fl_str_mv |
Inglés |
| language_invalid_str_mv |
Inglés |
| dc.relation.none.fl_str_mv |
Versió postprint del document publicat a: https://doi.org/10.1021/acs.langmuir.1c00461 Langmuir, 2021, vol. 37, p. 4666-4677 https://doi.org/10.1021/acs.langmuir.1c00461 |
| dc.rights.none.fl_str_mv |
(c) American Chemical Society , 2021 info:eu-repo/semantics/openAccess |
| rights_invalid_str_mv |
(c) American Chemical Society , 2021 |
| eu_rights_str_mv |
openAccess |
| dc.format.none.fl_str_mv |
12 p. application/pdf |
| dc.publisher.none.fl_str_mv |
American Chemical Society |
| publisher.none.fl_str_mv |
American Chemical Society |
| dc.source.none.fl_str_mv |
Articles publicats en revistes (Ciència dels Materials i Química Física) reponame:Recercat. Dipósit de la Recerca de Catalunya instname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya) |
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Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya) |
| reponame_str |
Recercat. Dipósit de la Recerca de Catalunya |
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Recercat. Dipósit de la Recerca de Catalunya |
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1869407851668045824 |
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15,198674 |