Effect of gold electronic state on the catalytic performance of nano gold catalysts in n-octanol oxidation
| Autor(a) principal: | |
|---|---|
| Data de Publicação: | 2020 |
| Outros Autores: | , , , , , , , , , , , , , |
| Tipo de documento: | Artigo |
| Idioma: | eng |
| Título da fonte: | Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) |
| Texto Completo: | http://hdl.handle.net/10362/103777 |
Resumo: | UIDB/50006/2020 project VIU-RSCBMT-65/2019 project 18-29-24037 (Russia) MINECO project CTQ2017-86170-R (Spain) |
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Effect of gold electronic state on the catalytic performance of nano gold catalysts in n-octanol oxidationAcid-base centersDFTGold active sitesGold catalystsGold electronic stateMetal contentN-octanol oxidationPretreatment atmosphereSelectivitySolvent adsorptionSupport modifiersChemical Engineering(all)Materials Science(all)UIDB/50006/2020 project VIU-RSCBMT-65/2019 project 18-29-24037 (Russia) MINECO project CTQ2017-86170-R (Spain)This study aims to identify the role of the various electronic states of gold in the catalytic behavior of Au/MxOy/TiO2 (where MxOy are Fe2O3 or MgO) for the liquid phase oxidation of n-octanol, under mild conditions. For this purpose, Au/MxOy/TiO2 catalysts were prepared by deposition-precipitation with urea, varying the gold content (0.5 or 4 wt.%) and pretreatment conditions (H2 or O2), and characterized by low temperature nitrogen adsorption-desorption, X-ray powder diffraction (XRD), energy dispersive spectroscopy (EDX), scanning transmission electron microscopy-high angle annular dark field (STEM HAADF), diffuse reflectance Fourier transform infrared (DRIFT) spectroscopy of CO adsorption, temperature-programmable desorption (TPD) of ammonia and carbon dioxide, and X-ray photoelectron spectroscopy (XPS). Three states of gold were identified on the surface of the catalysts, Au0, Au1+ and Au3+, and their ratio determined the catalysts performance. Based on a comparison of catalytic and spectroscopic results, it may be concluded that Au+ was the active site state, while Au0 had negative effect, due to a partial blocking of Au0 by solvent. Au3+ also inhibited the oxidation process, due to the strong adsorption of the solvent and/or water formed during the reaction. Density functional theory (DFT) simulations confirmed these suggestions. The dependence of selectivity on the ratio of Brønsted acid centers to Brønsted basic centers was revealed.LAQV@REQUIMTEDQ - Departamento de QuímicaRUNPakrieva, EkaterinaKolobova, EkaterinaKotolevich, YuliaPascual, LauraCarabineiro, Sónia A. C.Kharlanov, Andrey N.Pichugina, DariaNikitina, NadezhdaGerman, DmitriiPartida, Trino A. ZepedaVazquez, Hugo J. TiznadoFarías, Mario H.Bogdanchikova, NinaCorberán, Vicente CortésPestryakov, Alexey2020-09-09T02:34:17Z2020-052020-05-01T00:00:00Zinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/articleapplication/pdfhttp://hdl.handle.net/10362/103777eng2079-4991PURE: 18201329https://doi.org/10.3390/nano10050880info:eu-repo/semantics/openAccessreponame:Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos)instname:Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informaçãoinstacron:RCAAP2024-03-11T04:49:25Zoai:run.unl.pt:10362/103777Portal AgregadorONGhttps://www.rcaap.pt/oai/openaireopendoar:71602024-03-20T03:40:03.491278Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) - Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informaçãofalse |
| dc.title.none.fl_str_mv |
Effect of gold electronic state on the catalytic performance of nano gold catalysts in n-octanol oxidation |
| title |
Effect of gold electronic state on the catalytic performance of nano gold catalysts in n-octanol oxidation |
| spellingShingle |
Effect of gold electronic state on the catalytic performance of nano gold catalysts in n-octanol oxidation Pakrieva, Ekaterina Acid-base centers DFT Gold active sites Gold catalysts Gold electronic state Metal content N-octanol oxidation Pretreatment atmosphere Selectivity Solvent adsorption Support modifiers Chemical Engineering(all) Materials Science(all) |
| title_short |
Effect of gold electronic state on the catalytic performance of nano gold catalysts in n-octanol oxidation |
| title_full |
Effect of gold electronic state on the catalytic performance of nano gold catalysts in n-octanol oxidation |
| title_fullStr |
Effect of gold electronic state on the catalytic performance of nano gold catalysts in n-octanol oxidation |
| title_full_unstemmed |
Effect of gold electronic state on the catalytic performance of nano gold catalysts in n-octanol oxidation |
| title_sort |
Effect of gold electronic state on the catalytic performance of nano gold catalysts in n-octanol oxidation |
| author |
Pakrieva, Ekaterina |
| author_facet |
Pakrieva, Ekaterina Kolobova, Ekaterina Kotolevich, Yulia Pascual, Laura Carabineiro, Sónia A. C. Kharlanov, Andrey N. Pichugina, Daria Nikitina, Nadezhda German, Dmitrii Partida, Trino A. Zepeda Vazquez, Hugo J. Tiznado Farías, Mario H. Bogdanchikova, Nina Corberán, Vicente Cortés Pestryakov, Alexey |
| author_role |
author |
| author2 |
Kolobova, Ekaterina Kotolevich, Yulia Pascual, Laura Carabineiro, Sónia A. C. Kharlanov, Andrey N. Pichugina, Daria Nikitina, Nadezhda German, Dmitrii Partida, Trino A. Zepeda Vazquez, Hugo J. Tiznado Farías, Mario H. Bogdanchikova, Nina Corberán, Vicente Cortés Pestryakov, Alexey |
| author2_role |
author author author author author author author author author author author author author author |
| dc.contributor.none.fl_str_mv |
LAQV@REQUIMTE DQ - Departamento de Química RUN |
| dc.contributor.author.fl_str_mv |
Pakrieva, Ekaterina Kolobova, Ekaterina Kotolevich, Yulia Pascual, Laura Carabineiro, Sónia A. C. Kharlanov, Andrey N. Pichugina, Daria Nikitina, Nadezhda German, Dmitrii Partida, Trino A. Zepeda Vazquez, Hugo J. Tiznado Farías, Mario H. Bogdanchikova, Nina Corberán, Vicente Cortés Pestryakov, Alexey |
| dc.subject.por.fl_str_mv |
Acid-base centers DFT Gold active sites Gold catalysts Gold electronic state Metal content N-octanol oxidation Pretreatment atmosphere Selectivity Solvent adsorption Support modifiers Chemical Engineering(all) Materials Science(all) |
| topic |
Acid-base centers DFT Gold active sites Gold catalysts Gold electronic state Metal content N-octanol oxidation Pretreatment atmosphere Selectivity Solvent adsorption Support modifiers Chemical Engineering(all) Materials Science(all) |
| description |
UIDB/50006/2020 project VIU-RSCBMT-65/2019 project 18-29-24037 (Russia) MINECO project CTQ2017-86170-R (Spain) |
| publishDate |
2020 |
| dc.date.none.fl_str_mv |
2020-09-09T02:34:17Z 2020-05 2020-05-01T00:00:00Z |
| dc.type.status.fl_str_mv |
info:eu-repo/semantics/publishedVersion |
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info:eu-repo/semantics/article |
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article |
| status_str |
publishedVersion |
| dc.identifier.uri.fl_str_mv |
http://hdl.handle.net/10362/103777 |
| url |
http://hdl.handle.net/10362/103777 |
| dc.language.iso.fl_str_mv |
eng |
| language |
eng |
| dc.relation.none.fl_str_mv |
2079-4991 PURE: 18201329 https://doi.org/10.3390/nano10050880 |
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info:eu-repo/semantics/openAccess |
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openAccess |
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application/pdf |
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reponame:Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) instname:Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informação instacron:RCAAP |
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Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informação |
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RCAAP |
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RCAAP |
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Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) |
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Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) |
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Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) - Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informação |
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