Insights into the Preparation of Copper Catalysts Supported on Layered Double Hydroxide Derived Mixed Oxides for Ethanol Dehydrogenation
Autor(a) principal: | |
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Data de Publicação: | 2021 |
Outros Autores: | , , |
Tipo de documento: | Artigo |
Idioma: | eng |
Título da fonte: | Repositório Institucional da UNESP |
Texto Completo: | http://dx.doi.org/10.1021/acsami.1c04541 http://hdl.handle.net/11449/233160 |
Resumo: | Acetaldehyde is an important chemical commodity and a building block for producing several other high-value products in the chemical industry. This has motivated the search for suitable, efficient, stable, and selective catalysts, as well as renewable raw materials such as ethanol. In this work, supported copper catalysts were prepared from CuZnAl layered double hydroxides (LDHs) with different copper contents (5, 10, and 20 wt %) for application in the ethanol dehydrogenation reaction (EDR). The samples were thoroughly characterized by a series of techniques, which allowed for analysis of all of the copper and zinc species involved in the different catalyst preparation steps and during the EDR. The results obtained by in situ quick extended X-ray absorption fine structure (EXAFS) measurements, combined with multivariate data analysis, showed that the copper content in the pristine LDH influenced the phase composition of the mixed oxide support, which consequently affected the dispersion of copper nanoparticles. The higher the copper content, the higher are the ZnAl2O4 and zinc tetrahedral prenuclei (TPN) contents, to the detriment of the ZnO content. All the samples showed high selectivity (>97%) and stability in the catalytic reactions at 300 and 350 °C, with no observed deactivation during 6 h on-stream. Although the samples with lower copper content presented higher copper dispersion and reactivity, the sample containing 20 wt % of copper outperformed the others, with greater conversion and higher activity toward acetaldehyde. |
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Insights into the Preparation of Copper Catalysts Supported on Layered Double Hydroxide Derived Mixed Oxides for Ethanol Dehydrogenationacetaldehydecopper-based catalystethanol-dehydrogenation reaction (EDR)layered double hydroxide (LDH)operando quick-EXAFSAcetaldehyde is an important chemical commodity and a building block for producing several other high-value products in the chemical industry. This has motivated the search for suitable, efficient, stable, and selective catalysts, as well as renewable raw materials such as ethanol. In this work, supported copper catalysts were prepared from CuZnAl layered double hydroxides (LDHs) with different copper contents (5, 10, and 20 wt %) for application in the ethanol dehydrogenation reaction (EDR). The samples were thoroughly characterized by a series of techniques, which allowed for analysis of all of the copper and zinc species involved in the different catalyst preparation steps and during the EDR. The results obtained by in situ quick extended X-ray absorption fine structure (EXAFS) measurements, combined with multivariate data analysis, showed that the copper content in the pristine LDH influenced the phase composition of the mixed oxide support, which consequently affected the dispersion of copper nanoparticles. The higher the copper content, the higher are the ZnAl2O4 and zinc tetrahedral prenuclei (TPN) contents, to the detriment of the ZnO content. All the samples showed high selectivity (>97%) and stability in the catalytic reactions at 300 and 350 °C, with no observed deactivation during 6 h on-stream. Although the samples with lower copper content presented higher copper dispersion and reactivity, the sample containing 20 wt % of copper outperformed the others, with greater conversion and higher activity toward acetaldehyde.Institute of Chemistry São Paulo State University (UNESP), Rua Prof. Francisco Degni 55,São PauloSoleil Synchrotron L'Orme des Merisiers BP48, Gif-sur-YvetteInstitute of Chemistry São Paulo State University (UNESP), Rua Prof. Francisco Degni 55,São PauloUniversidade Estadual Paulista (UNESP)BP48Santos, Rodrigo M. M. [UNESP]Briois, ValérieMartins, Leandro [UNESP]Santilli, Celso V. [UNESP]2022-05-01T05:29:02Z2022-05-01T05:29:02Z2021-06-09info:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/article26001-26012http://dx.doi.org/10.1021/acsami.1c04541ACS Applied Materials and Interfaces, v. 13, n. 22, p. 26001-26012, 2021.1944-82521944-8244http://hdl.handle.net/11449/23316010.1021/acsami.1c045412-s2.0-85108020947Scopusreponame:Repositório Institucional da UNESPinstname:Universidade Estadual Paulista (UNESP)instacron:UNESPengACS Applied Materials and Interfacesinfo:eu-repo/semantics/openAccess2022-05-01T05:29:02Zoai:repositorio.unesp.br:11449/233160Repositório InstitucionalPUBhttp://repositorio.unesp.br/oai/requestopendoar:29462024-08-05T21:40:35.514577Repositório Institucional da UNESP - Universidade Estadual Paulista (UNESP)false |
dc.title.none.fl_str_mv |
Insights into the Preparation of Copper Catalysts Supported on Layered Double Hydroxide Derived Mixed Oxides for Ethanol Dehydrogenation |
title |
Insights into the Preparation of Copper Catalysts Supported on Layered Double Hydroxide Derived Mixed Oxides for Ethanol Dehydrogenation |
spellingShingle |
Insights into the Preparation of Copper Catalysts Supported on Layered Double Hydroxide Derived Mixed Oxides for Ethanol Dehydrogenation Santos, Rodrigo M. M. [UNESP] acetaldehyde copper-based catalyst ethanol-dehydrogenation reaction (EDR) layered double hydroxide (LDH) operando quick-EXAFS |
title_short |
Insights into the Preparation of Copper Catalysts Supported on Layered Double Hydroxide Derived Mixed Oxides for Ethanol Dehydrogenation |
title_full |
Insights into the Preparation of Copper Catalysts Supported on Layered Double Hydroxide Derived Mixed Oxides for Ethanol Dehydrogenation |
title_fullStr |
Insights into the Preparation of Copper Catalysts Supported on Layered Double Hydroxide Derived Mixed Oxides for Ethanol Dehydrogenation |
title_full_unstemmed |
Insights into the Preparation of Copper Catalysts Supported on Layered Double Hydroxide Derived Mixed Oxides for Ethanol Dehydrogenation |
title_sort |
Insights into the Preparation of Copper Catalysts Supported on Layered Double Hydroxide Derived Mixed Oxides for Ethanol Dehydrogenation |
author |
Santos, Rodrigo M. M. [UNESP] |
author_facet |
Santos, Rodrigo M. M. [UNESP] Briois, Valérie Martins, Leandro [UNESP] Santilli, Celso V. [UNESP] |
author_role |
author |
author2 |
Briois, Valérie Martins, Leandro [UNESP] Santilli, Celso V. [UNESP] |
author2_role |
author author author |
dc.contributor.none.fl_str_mv |
Universidade Estadual Paulista (UNESP) BP48 |
dc.contributor.author.fl_str_mv |
Santos, Rodrigo M. M. [UNESP] Briois, Valérie Martins, Leandro [UNESP] Santilli, Celso V. [UNESP] |
dc.subject.por.fl_str_mv |
acetaldehyde copper-based catalyst ethanol-dehydrogenation reaction (EDR) layered double hydroxide (LDH) operando quick-EXAFS |
topic |
acetaldehyde copper-based catalyst ethanol-dehydrogenation reaction (EDR) layered double hydroxide (LDH) operando quick-EXAFS |
description |
Acetaldehyde is an important chemical commodity and a building block for producing several other high-value products in the chemical industry. This has motivated the search for suitable, efficient, stable, and selective catalysts, as well as renewable raw materials such as ethanol. In this work, supported copper catalysts were prepared from CuZnAl layered double hydroxides (LDHs) with different copper contents (5, 10, and 20 wt %) for application in the ethanol dehydrogenation reaction (EDR). The samples were thoroughly characterized by a series of techniques, which allowed for analysis of all of the copper and zinc species involved in the different catalyst preparation steps and during the EDR. The results obtained by in situ quick extended X-ray absorption fine structure (EXAFS) measurements, combined with multivariate data analysis, showed that the copper content in the pristine LDH influenced the phase composition of the mixed oxide support, which consequently affected the dispersion of copper nanoparticles. The higher the copper content, the higher are the ZnAl2O4 and zinc tetrahedral prenuclei (TPN) contents, to the detriment of the ZnO content. All the samples showed high selectivity (>97%) and stability in the catalytic reactions at 300 and 350 °C, with no observed deactivation during 6 h on-stream. Although the samples with lower copper content presented higher copper dispersion and reactivity, the sample containing 20 wt % of copper outperformed the others, with greater conversion and higher activity toward acetaldehyde. |
publishDate |
2021 |
dc.date.none.fl_str_mv |
2021-06-09 2022-05-01T05:29:02Z 2022-05-01T05:29:02Z |
dc.type.status.fl_str_mv |
info:eu-repo/semantics/publishedVersion |
dc.type.driver.fl_str_mv |
info:eu-repo/semantics/article |
format |
article |
status_str |
publishedVersion |
dc.identifier.uri.fl_str_mv |
http://dx.doi.org/10.1021/acsami.1c04541 ACS Applied Materials and Interfaces, v. 13, n. 22, p. 26001-26012, 2021. 1944-8252 1944-8244 http://hdl.handle.net/11449/233160 10.1021/acsami.1c04541 2-s2.0-85108020947 |
url |
http://dx.doi.org/10.1021/acsami.1c04541 http://hdl.handle.net/11449/233160 |
identifier_str_mv |
ACS Applied Materials and Interfaces, v. 13, n. 22, p. 26001-26012, 2021. 1944-8252 1944-8244 10.1021/acsami.1c04541 2-s2.0-85108020947 |
dc.language.iso.fl_str_mv |
eng |
language |
eng |
dc.relation.none.fl_str_mv |
ACS Applied Materials and Interfaces |
dc.rights.driver.fl_str_mv |
info:eu-repo/semantics/openAccess |
eu_rights_str_mv |
openAccess |
dc.format.none.fl_str_mv |
26001-26012 |
dc.source.none.fl_str_mv |
Scopus reponame:Repositório Institucional da UNESP instname:Universidade Estadual Paulista (UNESP) instacron:UNESP |
instname_str |
Universidade Estadual Paulista (UNESP) |
instacron_str |
UNESP |
institution |
UNESP |
reponame_str |
Repositório Institucional da UNESP |
collection |
Repositório Institucional da UNESP |
repository.name.fl_str_mv |
Repositório Institucional da UNESP - Universidade Estadual Paulista (UNESP) |
repository.mail.fl_str_mv |
|
_version_ |
1808129345529577472 |