Assessment of Ag Nanoparticles Interaction over Low-Cost Mesoporous Silica in Deep Desulfurization of Diesel
Autor(a) principal: | |
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Data de Publicação: | 2019 |
Outros Autores: | , , , , , , , , |
Tipo de documento: | Artigo |
Idioma: | eng |
Título da fonte: | Repositório Institucional da UFRN |
Texto Completo: | https://repositorio.ufrn.br/handle/123456789/30341 |
Resumo: | Chemical interactions between metal particles (Ag or Ni) dispersed in a low-cost MCM-41M produced from beach sand amorphous silica and sulfur compounds were evaluated in the deep adsorptive desulfurization process of real diesel fuel. N2 adsorption-desorption isotherms, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), high-resolution transmission electron microscopy (HRTEM) and scanning transmission electron microscopy coupled to energy-dispersive X-ray spectroscopy (STEM-EDX) were used for characterizing the adsorbents. HRTEM and XPS confirmed the high dispersion of Ag nanoparticles on the MCM-41 surface, and its chemical interaction with support and sulfur compounds by diverse mechanisms such as π-complexation and oxidation. Thermodynamic tests indicated that the adsorption of sulfur compounds over Ag(I)/MCM-41M is an endothermic process under the studied conditions. The magnitude of DH◦ (42.1 kJ/mol) indicates that chemisorptive mechanisms govern the sulfur removal. The best fit of kinetic and equilibrium data to pseudo-second order (R2 > 0.99) and Langmuir models (R2 > 0.98), respectively, along with the results for intraparticle diffusion and Boyd’s film-diffusion kinetic models, suggest that the chemisorptive interaction between organosulfur compounds and Ag nanosites controls sulfur adsorption, as seen in the XPS results. Its adsorption capacity (qm = 31.25 mgS/g) was 10 times higher than that obtained for pure MCM-41M and double the qm for the Ag(I)/MCM-41C adsorbent from commercial silica. Saturated adsorbents presented a satisfactory regeneration rate after a total of five sulfur adsorption cycles |
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Bicudo, Tatiana de CamposSales, Rafael V.Moura, Heloise O. M. A.Câmara, Anne B. F.Rodríguez-Castellón, EnriqueSilva, José A. B.Pergher, Sibele B. C.Campos, Leila M. A.Urbina, Maritza M.Carvalho, Luciene S. de2020-10-08T23:32:52Z2020-10-08T23:32:52Z2019-07-30SALES, Rafael V.; MOURA, Heloise O. M. A.; CÂMARA, Anne B. F.; RODRÍGUEZ-CASTELLÓN, Enrique; SILVA, José A. B.; PERGHER, Sibele B. C.; CAMPOS, Leila M. A.; URBINA, Maritza M.; BICUDO, Tatiana C.; CARVALHO, Luciene S. de. Assessment of Ag Nanoparticles Interaction over Low-Cost Mesoporous Silica in Deep Desulfurization of Diesel. Catalysts, [S.L.], v. 9, n. 8, p. 651-651, 30 jul. 2019. Disponível em: https://www.mdpi.com/2073-4344/9/8/651. Acesso em: 08 set. 2020. http://dx.doi.org/10.3390/catal9080651.2073-4344https://repositorio.ufrn.br/handle/123456789/3034110.3390/catal9080651MDPI AGAttribution 3.0 Brazilhttp://creativecommons.org/licenses/by/3.0/br/info:eu-repo/semantics/openAccessDesulfurizationChemisorptionMPI silicaMCM-41Ag nanoparticlesXPS assessmentAssessment of Ag Nanoparticles Interaction over Low-Cost Mesoporous Silica in Deep Desulfurization of Dieselinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/articleChemical interactions between metal particles (Ag or Ni) dispersed in a low-cost MCM-41M produced from beach sand amorphous silica and sulfur compounds were evaluated in the deep adsorptive desulfurization process of real diesel fuel. N2 adsorption-desorption isotherms, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), high-resolution transmission electron microscopy (HRTEM) and scanning transmission electron microscopy coupled to energy-dispersive X-ray spectroscopy (STEM-EDX) were used for characterizing the adsorbents. HRTEM and XPS confirmed the high dispersion of Ag nanoparticles on the MCM-41 surface, and its chemical interaction with support and sulfur compounds by diverse mechanisms such as π-complexation and oxidation. Thermodynamic tests indicated that the adsorption of sulfur compounds over Ag(I)/MCM-41M is an endothermic process under the studied conditions. The magnitude of DH◦ (42.1 kJ/mol) indicates that chemisorptive mechanisms govern the sulfur removal. The best fit of kinetic and equilibrium data to pseudo-second order (R2 > 0.99) and Langmuir models (R2 > 0.98), respectively, along with the results for intraparticle diffusion and Boyd’s film-diffusion kinetic models, suggest that the chemisorptive interaction between organosulfur compounds and Ag nanosites controls sulfur adsorption, as seen in the XPS results. Its adsorption capacity (qm = 31.25 mgS/g) was 10 times higher than that obtained for pure MCM-41M and double the qm for the Ag(I)/MCM-41C adsorbent from commercial silica. Saturated adsorbents presented a satisfactory regeneration rate after a total of five sulfur adsorption cyclesengreponame:Repositório Institucional da UFRNinstname:Universidade Federal do Rio Grande do Norte (UFRN)instacron:UFRNORIGINALAssessmentNanoparticles_BICUDO_2019.pdfAssessmentNanoparticles_BICUDO_2019.pdfapplication/pdf5322724https://repositorio.ufrn.br/bitstream/123456789/30341/1/AssessmentNanoparticles_BICUDO_2019.pdf59d2dec7c4a53861b4f35f873fd3aecdMD51CC-LICENSElicense_rdflicense_rdfapplication/rdf+xml; charset=utf-8914https://repositorio.ufrn.br/bitstream/123456789/30341/2/license_rdf4d2950bda3d176f570a9f8b328dfbbefMD52LICENSElicense.txtlicense.txttext/plain; charset=utf-81484https://repositorio.ufrn.br/bitstream/123456789/30341/3/license.txte9597aa2854d128fd968be5edc8a28d9MD53TEXTAssessmentNanoparticles_BICUDO_2019.pdf.txtAssessmentNanoparticles_BICUDO_2019.pdf.txtExtracted texttext/plain84071https://repositorio.ufrn.br/bitstream/123456789/30341/4/AssessmentNanoparticles_BICUDO_2019.pdf.txtfebe767d8096918b9195bbec4606eb40MD54THUMBNAILAssessmentNanoparticles_BICUDO_2019.pdf.jpgAssessmentNanoparticles_BICUDO_2019.pdf.jpgGenerated Thumbnailimage/jpeg1642https://repositorio.ufrn.br/bitstream/123456789/30341/5/AssessmentNanoparticles_BICUDO_2019.pdf.jpgbc057b419bd34446adbc60cf03a7fbcdMD55123456789/303412020-10-11 04:38:28.43oai:https://repositorio.ufrn.br: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Repositório de PublicaçõesPUBhttp://repositorio.ufrn.br/oai/opendoar:2020-10-11T07:38:28Repositório Institucional da UFRN - Universidade Federal do Rio Grande do Norte (UFRN)false |
dc.title.pt_BR.fl_str_mv |
Assessment of Ag Nanoparticles Interaction over Low-Cost Mesoporous Silica in Deep Desulfurization of Diesel |
title |
Assessment of Ag Nanoparticles Interaction over Low-Cost Mesoporous Silica in Deep Desulfurization of Diesel |
spellingShingle |
Assessment of Ag Nanoparticles Interaction over Low-Cost Mesoporous Silica in Deep Desulfurization of Diesel Bicudo, Tatiana de Campos Desulfurization Chemisorption MPI silica MCM-41 Ag nanoparticles XPS assessment |
title_short |
Assessment of Ag Nanoparticles Interaction over Low-Cost Mesoporous Silica in Deep Desulfurization of Diesel |
title_full |
Assessment of Ag Nanoparticles Interaction over Low-Cost Mesoporous Silica in Deep Desulfurization of Diesel |
title_fullStr |
Assessment of Ag Nanoparticles Interaction over Low-Cost Mesoporous Silica in Deep Desulfurization of Diesel |
title_full_unstemmed |
Assessment of Ag Nanoparticles Interaction over Low-Cost Mesoporous Silica in Deep Desulfurization of Diesel |
title_sort |
Assessment of Ag Nanoparticles Interaction over Low-Cost Mesoporous Silica in Deep Desulfurization of Diesel |
author |
Bicudo, Tatiana de Campos |
author_facet |
Bicudo, Tatiana de Campos Sales, Rafael V. Moura, Heloise O. M. A. Câmara, Anne B. F. Rodríguez-Castellón, Enrique Silva, José A. B. Pergher, Sibele B. C. Campos, Leila M. A. Urbina, Maritza M. Carvalho, Luciene S. de |
author_role |
author |
author2 |
Sales, Rafael V. Moura, Heloise O. M. A. Câmara, Anne B. F. Rodríguez-Castellón, Enrique Silva, José A. B. Pergher, Sibele B. C. Campos, Leila M. A. Urbina, Maritza M. Carvalho, Luciene S. de |
author2_role |
author author author author author author author author author |
dc.contributor.author.fl_str_mv |
Bicudo, Tatiana de Campos Sales, Rafael V. Moura, Heloise O. M. A. Câmara, Anne B. F. Rodríguez-Castellón, Enrique Silva, José A. B. Pergher, Sibele B. C. Campos, Leila M. A. Urbina, Maritza M. Carvalho, Luciene S. de |
dc.subject.por.fl_str_mv |
Desulfurization Chemisorption MPI silica MCM-41 Ag nanoparticles XPS assessment |
topic |
Desulfurization Chemisorption MPI silica MCM-41 Ag nanoparticles XPS assessment |
description |
Chemical interactions between metal particles (Ag or Ni) dispersed in a low-cost MCM-41M produced from beach sand amorphous silica and sulfur compounds were evaluated in the deep adsorptive desulfurization process of real diesel fuel. N2 adsorption-desorption isotherms, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), high-resolution transmission electron microscopy (HRTEM) and scanning transmission electron microscopy coupled to energy-dispersive X-ray spectroscopy (STEM-EDX) were used for characterizing the adsorbents. HRTEM and XPS confirmed the high dispersion of Ag nanoparticles on the MCM-41 surface, and its chemical interaction with support and sulfur compounds by diverse mechanisms such as π-complexation and oxidation. Thermodynamic tests indicated that the adsorption of sulfur compounds over Ag(I)/MCM-41M is an endothermic process under the studied conditions. The magnitude of DH◦ (42.1 kJ/mol) indicates that chemisorptive mechanisms govern the sulfur removal. The best fit of kinetic and equilibrium data to pseudo-second order (R2 > 0.99) and Langmuir models (R2 > 0.98), respectively, along with the results for intraparticle diffusion and Boyd’s film-diffusion kinetic models, suggest that the chemisorptive interaction between organosulfur compounds and Ag nanosites controls sulfur adsorption, as seen in the XPS results. Its adsorption capacity (qm = 31.25 mgS/g) was 10 times higher than that obtained for pure MCM-41M and double the qm for the Ag(I)/MCM-41C adsorbent from commercial silica. Saturated adsorbents presented a satisfactory regeneration rate after a total of five sulfur adsorption cycles |
publishDate |
2019 |
dc.date.issued.fl_str_mv |
2019-07-30 |
dc.date.accessioned.fl_str_mv |
2020-10-08T23:32:52Z |
dc.date.available.fl_str_mv |
2020-10-08T23:32:52Z |
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.citation.fl_str_mv |
SALES, Rafael V.; MOURA, Heloise O. M. A.; CÂMARA, Anne B. F.; RODRÍGUEZ-CASTELLÓN, Enrique; SILVA, José A. B.; PERGHER, Sibele B. C.; CAMPOS, Leila M. A.; URBINA, Maritza M.; BICUDO, Tatiana C.; CARVALHO, Luciene S. de. Assessment of Ag Nanoparticles Interaction over Low-Cost Mesoporous Silica in Deep Desulfurization of Diesel. Catalysts, [S.L.], v. 9, n. 8, p. 651-651, 30 jul. 2019. Disponível em: https://www.mdpi.com/2073-4344/9/8/651. Acesso em: 08 set. 2020. http://dx.doi.org/10.3390/catal9080651. |
dc.identifier.uri.fl_str_mv |
https://repositorio.ufrn.br/handle/123456789/30341 |
dc.identifier.issn.none.fl_str_mv |
2073-4344 |
dc.identifier.doi.none.fl_str_mv |
10.3390/catal9080651 |
identifier_str_mv |
SALES, Rafael V.; MOURA, Heloise O. M. A.; CÂMARA, Anne B. F.; RODRÍGUEZ-CASTELLÓN, Enrique; SILVA, José A. B.; PERGHER, Sibele B. C.; CAMPOS, Leila M. A.; URBINA, Maritza M.; BICUDO, Tatiana C.; CARVALHO, Luciene S. de. Assessment of Ag Nanoparticles Interaction over Low-Cost Mesoporous Silica in Deep Desulfurization of Diesel. Catalysts, [S.L.], v. 9, n. 8, p. 651-651, 30 jul. 2019. Disponível em: https://www.mdpi.com/2073-4344/9/8/651. Acesso em: 08 set. 2020. http://dx.doi.org/10.3390/catal9080651. 2073-4344 10.3390/catal9080651 |
url |
https://repositorio.ufrn.br/handle/123456789/30341 |
dc.language.iso.fl_str_mv |
eng |
language |
eng |
dc.rights.driver.fl_str_mv |
Attribution 3.0 Brazil http://creativecommons.org/licenses/by/3.0/br/ info:eu-repo/semantics/openAccess |
rights_invalid_str_mv |
Attribution 3.0 Brazil http://creativecommons.org/licenses/by/3.0/br/ |
eu_rights_str_mv |
openAccess |
dc.publisher.none.fl_str_mv |
MDPI AG |
publisher.none.fl_str_mv |
MDPI AG |
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