Niobium on BEA dealuminated zeolite for high selectivity dehydration reactions of ethanol and xylose into diethyl ether and furfural
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| Publication Date: | 2020 |
| Other Authors: | , , , , |
| Format: | Article |
| Language: | eng |
| Source: | Repositório Institucional da UnB |
| Download full: | https://repositorio.unb.br/handle/10482/39298 https://doi.org/10.3390/nano10071269 https://orcid.org/0000-0003-4622-2445 https://orcid.org/0000-0003-0042-0091 https://orcid.org/0000-0002-3351-9226 |
Summary: | : In this work, we investigated the role of solid-state dealumination by (NH4)2SiF6 (25% Al removal and 13% Si insertion), the impregnation of niobium (10, 18, and 25 wt. %) on dealuminated *BEA (DB) zeolite and their catalytic properties in ethanol and xylose transformations. Among all the studied catalysts, 18%Nb-DB showed increased mesoporosity and external areas. A leveling effect in the number and strength of the proposed two sites (Brønsted and Lewis) present in the catalyst (n1 = 0.24 mmol g−1 , −∆H1 = 49 kJ mol−1 , and n2 = 0.20 mmol g−1 , –∆H2 = 42 kJ mol−1 ) in the catalyst 18%Nb-DB, might be responsible for its good activity. This catalyst presented the highest selectivity for diethyl ether, DEE (97%) with 61% conversion after 50 ethanol pulses at 230 ◦C (turnover number, TON DEE = 1.15). These features allowed catalytically fruitful bonding of the ethanol molecules to the neighboring sites on the channels, facilitating bimolecular ether formation through a possible SN2 mechanism. The same catalyst was active and selective for transformation of xylose at 180 ◦C, showing 64% conversion and 51% selectivity for furfural (TON Furfural = 24.7) using water as a green solvent. |
| _version_ | 1871442400448086016 |
|---|---|
| author | Valadares, Deborah da Silva |
| author2 | Clemente, Maria Clara Hortêncio Freitas, Elon Ferreira de Martins, Gesley Alex Veloso Dias, José Alves Dias, Silvia Clara Loureiro |
| author2_role | author author author author author |
| author_browse | Clemente, Maria Clara Hortêncio Dias, José Alves Dias, Silvia Clara Loureiro Freitas, Elon Ferreira de Martins, Gesley Alex Veloso Valadares, Deborah da Silva |
| author_facet | Valadares, Deborah da Silva Clemente, Maria Clara Hortêncio Freitas, Elon Ferreira de Martins, Gesley Alex Veloso Dias, José Alves Dias, Silvia Clara Loureiro |
| author_role | author |
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| bitstream.url.fl_str_mv | http://repositorio2.unb.br/jspui/bitstream/10482/39298/2/license.txt http://repositorio2.unb.br/jspui/bitstream/10482/39298/1/ARTIGO_NiobiumBEADealuminated.pdf |
| collection | Repositório Institucional da UnB |
| dc.contributor.author.fl_str_mv | Valadares, Deborah da Silva Clemente, Maria Clara Hortêncio Freitas, Elon Ferreira de Martins, Gesley Alex Veloso Dias, José Alves Dias, Silvia Clara Loureiro |
| dc.date.accessioned.fl_str_mv | 2020-07-24T22:08:25Z |
| dc.date.available.fl_str_mv | 2020-07-24T22:08:25Z |
| dc.date.issued.fl_str_mv | 2020 |
| dc.identifier.citation.fl_str_mv | VALADARES, Deborah S. et al. Niobium on BEA dealuminated zeolite for high selectivity dehydration reactions of ethanol and xylose into diethyl ether and furfural. Nanomaterials, v. 10, n. 7, 2020. DOI: https://doi.org/10.3390/nano10071269. Disponível em: https://www.mdpi.com/2079-4991/10/7/1269. |
| dc.identifier.doi.pt_BR.fl_str_mv | https://doi.org/10.3390/nano10071269 |
| dc.identifier.orcid.pt_BR.fl_str_mv | https://orcid.org/0000-0003-4622-2445 https://orcid.org/0000-0003-0042-0091 https://orcid.org/0000-0002-3351-9226 |
| dc.identifier.uri.fl_str_mv | https://repositorio.unb.br/handle/10482/39298 |
| dc.language.iso.fl_str_mv | eng |
| dc.publisher.none.fl_str_mv | MDPI |
| dc.rights.driver.fl_str_mv | info:eu-repo/semantics/openAccess |
| dc.source.none.fl_str_mv | reponame:Repositório Institucional da UnB instname:Universidade de Brasília (UnB) instacron:UNB |
| dc.subject.keyword.pt_BR.fl_str_mv | Zeólitas Nióbio Desidratação de etanol Éter Dietílico Xilose Furfural |
| dc.title.pt_BR.fl_str_mv | Niobium on BEA dealuminated zeolite for high selectivity dehydration reactions of ethanol and xylose into diethyl ether and furfural |
| dc.type.driver.fl_str_mv | info:eu-repo/semantics/article |
| dc.type.status.fl_str_mv | info:eu-repo/semantics/publishedVersion |
| description | : In this work, we investigated the role of solid-state dealumination by (NH4)2SiF6 (25% Al removal and 13% Si insertion), the impregnation of niobium (10, 18, and 25 wt. %) on dealuminated *BEA (DB) zeolite and their catalytic properties in ethanol and xylose transformations. Among all the studied catalysts, 18%Nb-DB showed increased mesoporosity and external areas. A leveling effect in the number and strength of the proposed two sites (Brønsted and Lewis) present in the catalyst (n1 = 0.24 mmol g−1 , −∆H1 = 49 kJ mol−1 , and n2 = 0.20 mmol g−1 , –∆H2 = 42 kJ mol−1 ) in the catalyst 18%Nb-DB, might be responsible for its good activity. This catalyst presented the highest selectivity for diethyl ether, DEE (97%) with 61% conversion after 50 ethanol pulses at 230 ◦C (turnover number, TON DEE = 1.15). These features allowed catalytically fruitful bonding of the ethanol molecules to the neighboring sites on the channels, facilitating bimolecular ether formation through a possible SN2 mechanism. The same catalyst was active and selective for transformation of xylose at 180 ◦C, showing 64% conversion and 51% selectivity for furfural (TON Furfural = 24.7) using water as a green solvent. |
| eu_rights_str_mv | openAccess |
| format | article |
| id | UNB_8fa6f7dbd64e99db8afea8aa694c679d |
| identifier_str_mv | VALADARES, Deborah S. et al. Niobium on BEA dealuminated zeolite for high selectivity dehydration reactions of ethanol and xylose into diethyl ether and furfural. Nanomaterials, v. 10, n. 7, 2020. DOI: https://doi.org/10.3390/nano10071269. Disponível em: https://www.mdpi.com/2079-4991/10/7/1269. |
| instacron_str | UNB |
| institution | UNB |
| instname_str | Universidade de Brasília (UnB) |
| language | eng |
| network_acronym_str | UNB |
| network_name_str | Repositório Institucional da UnB |
| oai_identifier_str | oai:repositorio.unb.br:10482/39298 |
| publishDate | 2020 |
| publishDateSort | 2020 |
| publisher.none.fl_str_mv | MDPI |
| reponame_str | Repositório Institucional da UnB |
| repository.mail.fl_str_mv | repositorio@unb.br |
| repository.name.fl_str_mv | Repositório Institucional da UnB - Universidade de Brasília (UnB) |
| repository_id_str | |
| spelling | Valadares, Deborah da SilvaClemente, Maria Clara HortêncioFreitas, Elon Ferreira deMartins, Gesley Alex VelosoDias, José AlvesDias, Silvia Clara Loureiro2020-07-24T22:08:25Z2020-07-24T22:08:25Z2020VALADARES, Deborah S. et al. Niobium on BEA dealuminated zeolite for high selectivity dehydration reactions of ethanol and xylose into diethyl ether and furfural. Nanomaterials, v. 10, n. 7, 2020. DOI: https://doi.org/10.3390/nano10071269. Disponível em: https://www.mdpi.com/2079-4991/10/7/1269.https://repositorio.unb.br/handle/10482/39298https://doi.org/10.3390/nano10071269https://orcid.org/0000-0003-4622-2445https://orcid.org/0000-0003-0042-0091https://orcid.org/0000-0002-3351-9226MDPI© 2020 by the authors. Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/).info:eu-repo/semantics/openAccessNiobium on BEA dealuminated zeolite for high selectivity dehydration reactions of ethanol and xylose into diethyl ether and furfuralinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/articleZeólitasNióbioDesidratação de etanolÉter DietílicoXiloseFurfural: In this work, we investigated the role of solid-state dealumination by (NH4)2SiF6 (25% Al removal and 13% Si insertion), the impregnation of niobium (10, 18, and 25 wt. %) on dealuminated *BEA (DB) zeolite and their catalytic properties in ethanol and xylose transformations. Among all the studied catalysts, 18%Nb-DB showed increased mesoporosity and external areas. A leveling effect in the number and strength of the proposed two sites (Brønsted and Lewis) present in the catalyst (n1 = 0.24 mmol g−1 , −∆H1 = 49 kJ mol−1 , and n2 = 0.20 mmol g−1 , –∆H2 = 42 kJ mol−1 ) in the catalyst 18%Nb-DB, might be responsible for its good activity. This catalyst presented the highest selectivity for diethyl ether, DEE (97%) with 61% conversion after 50 ethanol pulses at 230 ◦C (turnover number, TON DEE = 1.15). These features allowed catalytically fruitful bonding of the ethanol molecules to the neighboring sites on the channels, facilitating bimolecular ether formation through a possible SN2 mechanism. The same catalyst was active and selective for transformation of xylose at 180 ◦C, showing 64% conversion and 51% selectivity for furfural (TON Furfural = 24.7) using water as a green solvent.Instituto de Química (IQ)engreponame:Repositório Institucional da UnBinstname:Universidade de Brasília (UnB)instacron:UNBLICENSElicense.txtlicense.txttext/plain102http://repositorio2.unb.br/jspui/bitstream/10482/39298/2/license.txtaed4704d04bb260d4decd80db311aaa5MD52open accessORIGINALARTIGO_NiobiumBEADealuminated.pdfARTIGO_NiobiumBEADealuminated.pdfapplication/pdf3913294http://repositorio2.unb.br/jspui/bitstream/10482/39298/1/ARTIGO_NiobiumBEADealuminated.pdfdfa4138827ccdfec86163bcd578d06b7MD51open access10482/392982023-09-13 09:38:37.229open accessoai:repositorio.unb.br:10482/39298U3VibWlzc8OjbyBlZmV0aXZhZGEgZGUgYWNvcmRvIGNvbSBsaWNlbsOnYSBjb25jZWRpZGEgcGVsbyBhdXRvciBlL291IGRldGVudG9yIGRvcyBkaXJlaXRvcyBhdXRvcmFpcy4KRepositório InstitucionalPUBhttps://repositorio.unb.br/oai/requestrepositorio@unb.bropendoar:2023-09-13T12:38:37Repositório Institucional da UnB - Universidade de Brasília (UnB) |
| spellingShingle | Niobium on BEA dealuminated zeolite for high selectivity dehydration reactions of ethanol and xylose into diethyl ether and furfural Valadares, Deborah da Silva Zeólitas Nióbio Desidratação de etanol Éter Dietílico Xilose Furfural |
| status_str | publishedVersion |
| title | Niobium on BEA dealuminated zeolite for high selectivity dehydration reactions of ethanol and xylose into diethyl ether and furfural |
| title_full | Niobium on BEA dealuminated zeolite for high selectivity dehydration reactions of ethanol and xylose into diethyl ether and furfural |
| title_fullStr | Niobium on BEA dealuminated zeolite for high selectivity dehydration reactions of ethanol and xylose into diethyl ether and furfural |
| title_full_unstemmed | Niobium on BEA dealuminated zeolite for high selectivity dehydration reactions of ethanol and xylose into diethyl ether and furfural |
| title_short | Niobium on BEA dealuminated zeolite for high selectivity dehydration reactions of ethanol and xylose into diethyl ether and furfural |
| title_sort | Niobium on BEA dealuminated zeolite for high selectivity dehydration reactions of ethanol and xylose into diethyl ether and furfural |
| topic | Zeólitas Nióbio Desidratação de etanol Éter Dietílico Xilose Furfural |
| url | https://repositorio.unb.br/handle/10482/39298 https://doi.org/10.3390/nano10071269 https://orcid.org/0000-0003-4622-2445 https://orcid.org/0000-0003-0042-0091 https://orcid.org/0000-0002-3351-9226 |