Utilização de um novo material mesoporoso funcionalizado PABA-MCM-41 na remoção de hidrocarbonetos policíclicos aromáticos (HPAs)

Detalhes bibliográficos
Ano de defesa: 2013
Autor(a) principal: Costa, José Arnaldo Santana lattes
Orientador(a): Romão, Luciane Pimenta Cruz lattes
Banca de defesa: Não Informado pela instituição
Tipo de documento: Dissertação
Tipo de acesso: Acesso aberto
Idioma: por
Instituição de defesa: Não Informado pela instituição
Programa de Pós-Graduação: Pós-Graduação em Química
Departamento: Não Informado pela instituição
País: Não Informado pela instituição
Palavras-chave em Português:
Palavras-chave em Inglês:
Área do conhecimento CNPq:
Link de acesso: https://ri.ufs.br/handle/riufs/6098
Resumo: This work describes the synthesis and characterization of the mesoporous material MCM-41 and a new functionalized mesoporous material, PABA-MCM-41, for use as adsorbents to remove the PAHs benzo[k]fluoranthene (B[k]F), benzo[a]pyrene (B[a]P), and benzo[b]fluoranthene (B[b]F). Both materials were synthesized using hydrothermal methods. PABA-MCM-41 was synthesized using a hydrothermal/co-condensation technique, with functionalization employing modified 4-aminobenzoic acid. The mesoporous materials were characterized using Fourier transform infrared spectroscopy (FTIR), small angle X-ray scattering (SAXS), nitrogen adsorption/desorption, scanning electron microscopy (SEM), and thermogravimetric analysis (TG). Batch adsorption experiments were employed to determine the effects of initial adsorbate concentration, contact time, and temperature on the removal of the PAHs. The co-condensation method was shown to be effective for the synthesis of functionalized PABA-MCM-41. The two mesoporous materials presented the hexagonal mesostructures typical of the M41S family, which were confirmed by the SAXS analyses and by the type IV isotherms with type H1 hysteresis. The materials possessed uniform mesopore size distributions, high surface areas, and were thermally stable. Adsorption tests showed that for both materials, the quantity adsorbed (qe) increased as the initial PAHs concentration was increased, with adsorption equilibrium reached in around 90 minutes. For adsorption by MCM-41, the equilibrium qe values were 12.49, 14.06, and 18.06 ìg g-1 for B[k]F, B[a]P, and B[b]F, respectively, while the corresponding values for the same PAHs were 22.51, 27.24, and 26.58 ìg g-1 when PABA-MCM-41 was used. The experimental kinetic data were fitted using the pseudo-second order model, and the Langmuir isotherm model was able to describe the process of PAH adsorption. At higher temperatures, there were increases in the initial adsorption rate and the kinetic constant for adsorption of the PAHs by PABA-MCM-41. The thermodynamic parameters indicated that the processes are spontaneous, endothermic, and with a tendency towards disorder of the system at the adsorbent/adsorbate interface. Functionalization of MCM-41 increased the efficiency of adsorption of the PAHs by 44.5, 48.4, and 32.0% for B[k]F, B[a]P, and B[b]F, respectively.
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spelling Costa, José Arnaldo Santanahttp://lattes.cnpq.br/3881897681788109Romão, Luciane Pimenta Cruzhttp://lattes.cnpq.br/59135786628708852017-09-27T13:57:41Z2017-09-27T13:57:41Z2013-10-23https://ri.ufs.br/handle/riufs/6098This work describes the synthesis and characterization of the mesoporous material MCM-41 and a new functionalized mesoporous material, PABA-MCM-41, for use as adsorbents to remove the PAHs benzo[k]fluoranthene (B[k]F), benzo[a]pyrene (B[a]P), and benzo[b]fluoranthene (B[b]F). Both materials were synthesized using hydrothermal methods. PABA-MCM-41 was synthesized using a hydrothermal/co-condensation technique, with functionalization employing modified 4-aminobenzoic acid. The mesoporous materials were characterized using Fourier transform infrared spectroscopy (FTIR), small angle X-ray scattering (SAXS), nitrogen adsorption/desorption, scanning electron microscopy (SEM), and thermogravimetric analysis (TG). Batch adsorption experiments were employed to determine the effects of initial adsorbate concentration, contact time, and temperature on the removal of the PAHs. The co-condensation method was shown to be effective for the synthesis of functionalized PABA-MCM-41. The two mesoporous materials presented the hexagonal mesostructures typical of the M41S family, which were confirmed by the SAXS analyses and by the type IV isotherms with type H1 hysteresis. The materials possessed uniform mesopore size distributions, high surface areas, and were thermally stable. Adsorption tests showed that for both materials, the quantity adsorbed (qe) increased as the initial PAHs concentration was increased, with adsorption equilibrium reached in around 90 minutes. For adsorption by MCM-41, the equilibrium qe values were 12.49, 14.06, and 18.06 ìg g-1 for B[k]F, B[a]P, and B[b]F, respectively, while the corresponding values for the same PAHs were 22.51, 27.24, and 26.58 ìg g-1 when PABA-MCM-41 was used. The experimental kinetic data were fitted using the pseudo-second order model, and the Langmuir isotherm model was able to describe the process of PAH adsorption. At higher temperatures, there were increases in the initial adsorption rate and the kinetic constant for adsorption of the PAHs by PABA-MCM-41. The thermodynamic parameters indicated that the processes are spontaneous, endothermic, and with a tendency towards disorder of the system at the adsorbent/adsorbate interface. Functionalization of MCM-41 increased the efficiency of adsorption of the PAHs by 44.5, 48.4, and 32.0% for B[k]F, B[a]P, and B[b]F, respectively.Este trabalho descreve a sintese e caracterizacao do material mesoporoso MCM-41 e do novo material mesoporoso funcionalizado PABA-MCM-41 para serem utilizados como materiais adsorventes na remocao dos HPAs benzo[k]fluoranteno (B[k]F), benzo[a]pireno (B[a]P) e benzo[b]fluoranteno (B[b]F). Os dois materiais foram sintetizados pelo metodo hidrotermal, sendo que PABA-MCM-41 foi sintetizado pelo metodo hidrotermal/co-condensacao, o qual foi funcionalizado pelo acido 4-aminobenzoico modificado. Os materiais mesoporosos sintetizados foram caracterizados por espectroscopia na regiao do infravermelho por transformada de Fourier (FTIR), espalhamento de raios-X a baixo angulo (SAXS), adsorcao/dessorcao de N2, microscopia eletronica de varredura (MEV) e analise termogravimetrica (TG). Os experimentos de adsorcao em batelada foram utilizados para determinar os efeitos da concentracao inicial do adsorbato, tempo de contato e temperatura na remocao dos HPAs B[k]F, B[a]P e B[b]F. O metodo da co-condensacao mostrou-se eficiente na sintese do material mesoporoso funcionalizado PABA-MCM-41. Os dois materiais mesoporosos apresentaram mesoestruturas hexagonais tipicas da familia M41S, as quais foram confirmadas por SAXS, com isotermas do tipo IV e histerese do tipo H1. Tambem, apresentaram distribuicao uniforme do tamanho de mesoporos, alta area superficial e estabilidade termica. Os ensaios de adsorcao mostraram que ocorreu um aumento da quantidade adsorvida (qe) com o aumento da concentracao inicial dos HPAs, isto para os dois materiais mesoporosos utilizados, sendo que o equilibrio de adsorcao foi alcancado em cerca de 90 minutos. Os valores de qe obtidos no equilibrio foram de 12,49; 14,06 e 18,06 Êg g-1, respectivamente, na adsorcao do B[k]F, B[a]P e B[b]F pelo MCM-41 e de 22,51; 27,24 e 26,58 Êg g-1, respectivamente, na adsorcao dos mesmos pelo PABA-MCM-41. Os dados cineticos experimentais se ajustaram melhor ao modelo cinetico de pseudo-segunda ordem e o modelo de isoterma de Langmuir descreveu melhor o processo de adsorcao dos HPAs pelo MCM-41 e PABA-MCM-41. Foi verificado que em temperaturas mais altas houve um aumento na taxa inicial de adsorcao e na constante cinetica de adsorcao dos HPAs pelo PABA-MCM-41. Os parametros termodinamicos indicaram que o processo e espontaneo, endotermico e com uma tendencia para desordem do sistema na interface adsorvente/adsorbato. Com a funcionalizacao do MCM-41 foi verificado um aumento na eficiencia de adsorcao dos HPAs de 44,5; 48,4 e 32,0 %, respectivamente para o B[k]F, B[a]P e B[b]F.application/pdfporQuímica inorgânicaMateriais mesoporososQuímica de superfíciesAdsorçãoHidrocarbonetosPABA-MCM-41HPAsHidrocarbonetos policíclicos aromáticosAdsorptionInorganic chemistryHydrocarbonsMesoporous materialsSurface chemistryCNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICAUtilização de um novo material mesoporoso funcionalizado PABA-MCM-41 na remoção de hidrocarbonetos policíclicos aromáticos (HPAs)info:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/masterThesisPós-Graduação em Químicainfo:eu-repo/semantics/openAccessreponame:Repositório Institucional da UFSinstname:Universidade Federal de Sergipe (UFS)instacron:UFSORIGINALJOSE_ARNALDO_SANTANA_COSTA.pdfapplication/pdf2430130https://ri.ufs.br/jspui/bitstream/riufs/6098/1/JOSE_ARNALDO_SANTANA_COSTA.pdffb7f8983d8278e5386619eb66d891678MD51TEXTJOSE_ARNALDO_SANTANA_COSTA.pdf.txtJOSE_ARNALDO_SANTANA_COSTA.pdf.txtExtracted texttext/plain132166https://ri.ufs.br/jspui/bitstream/riufs/6098/2/JOSE_ARNALDO_SANTANA_COSTA.pdf.txtbd84f43a17f21026828119ebed0dce4eMD52THUMBNAILJOSE_ARNALDO_SANTANA_COSTA.pdf.jpgJOSE_ARNALDO_SANTANA_COSTA.pdf.jpgGenerated Thumbnailimage/jpeg1257https://ri.ufs.br/jspui/bitstream/riufs/6098/3/JOSE_ARNALDO_SANTANA_COSTA.pdf.jpg7a61f5ea511a35de93274147b6812485MD53riufs/60982018-01-17 21:09:31.71oai:ufs.br:riufs/6098Repositório InstitucionalPUBhttps://ri.ufs.br/oai/requestrepositorio@academico.ufs.bropendoar:2018-01-18T00:09:31Repositório Institucional da UFS - Universidade Federal de Sergipe (UFS)false
dc.title.por.fl_str_mv Utilização de um novo material mesoporoso funcionalizado PABA-MCM-41 na remoção de hidrocarbonetos policíclicos aromáticos (HPAs)
title Utilização de um novo material mesoporoso funcionalizado PABA-MCM-41 na remoção de hidrocarbonetos policíclicos aromáticos (HPAs)
spellingShingle Utilização de um novo material mesoporoso funcionalizado PABA-MCM-41 na remoção de hidrocarbonetos policíclicos aromáticos (HPAs)
Costa, José Arnaldo Santana
Química inorgânica
Materiais mesoporosos
Química de superfícies
Adsorção
Hidrocarbonetos
PABA-MCM-41
HPAs
Hidrocarbonetos policíclicos aromáticos
Adsorption
Inorganic chemistry
Hydrocarbons
Mesoporous materials
Surface chemistry
CNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICA
title_short Utilização de um novo material mesoporoso funcionalizado PABA-MCM-41 na remoção de hidrocarbonetos policíclicos aromáticos (HPAs)
title_full Utilização de um novo material mesoporoso funcionalizado PABA-MCM-41 na remoção de hidrocarbonetos policíclicos aromáticos (HPAs)
title_fullStr Utilização de um novo material mesoporoso funcionalizado PABA-MCM-41 na remoção de hidrocarbonetos policíclicos aromáticos (HPAs)
title_full_unstemmed Utilização de um novo material mesoporoso funcionalizado PABA-MCM-41 na remoção de hidrocarbonetos policíclicos aromáticos (HPAs)
title_sort Utilização de um novo material mesoporoso funcionalizado PABA-MCM-41 na remoção de hidrocarbonetos policíclicos aromáticos (HPAs)
author Costa, José Arnaldo Santana
author_facet Costa, José Arnaldo Santana
author_role author
dc.contributor.author.fl_str_mv Costa, José Arnaldo Santana
dc.contributor.advisor1Lattes.fl_str_mv http://lattes.cnpq.br/3881897681788109
dc.contributor.advisor1.fl_str_mv Romão, Luciane Pimenta Cruz
dc.contributor.authorLattes.fl_str_mv http://lattes.cnpq.br/5913578662870885
contributor_str_mv Romão, Luciane Pimenta Cruz
dc.subject.por.fl_str_mv Química inorgânica
Materiais mesoporosos
Química de superfícies
Adsorção
Hidrocarbonetos
PABA-MCM-41
HPAs
Hidrocarbonetos policíclicos aromáticos
topic Química inorgânica
Materiais mesoporosos
Química de superfícies
Adsorção
Hidrocarbonetos
PABA-MCM-41
HPAs
Hidrocarbonetos policíclicos aromáticos
Adsorption
Inorganic chemistry
Hydrocarbons
Mesoporous materials
Surface chemistry
CNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICA
dc.subject.eng.fl_str_mv Adsorption
Inorganic chemistry
Hydrocarbons
Mesoporous materials
Surface chemistry
dc.subject.cnpq.fl_str_mv CNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICA
description This work describes the synthesis and characterization of the mesoporous material MCM-41 and a new functionalized mesoporous material, PABA-MCM-41, for use as adsorbents to remove the PAHs benzo[k]fluoranthene (B[k]F), benzo[a]pyrene (B[a]P), and benzo[b]fluoranthene (B[b]F). Both materials were synthesized using hydrothermal methods. PABA-MCM-41 was synthesized using a hydrothermal/co-condensation technique, with functionalization employing modified 4-aminobenzoic acid. The mesoporous materials were characterized using Fourier transform infrared spectroscopy (FTIR), small angle X-ray scattering (SAXS), nitrogen adsorption/desorption, scanning electron microscopy (SEM), and thermogravimetric analysis (TG). Batch adsorption experiments were employed to determine the effects of initial adsorbate concentration, contact time, and temperature on the removal of the PAHs. The co-condensation method was shown to be effective for the synthesis of functionalized PABA-MCM-41. The two mesoporous materials presented the hexagonal mesostructures typical of the M41S family, which were confirmed by the SAXS analyses and by the type IV isotherms with type H1 hysteresis. The materials possessed uniform mesopore size distributions, high surface areas, and were thermally stable. Adsorption tests showed that for both materials, the quantity adsorbed (qe) increased as the initial PAHs concentration was increased, with adsorption equilibrium reached in around 90 minutes. For adsorption by MCM-41, the equilibrium qe values were 12.49, 14.06, and 18.06 ìg g-1 for B[k]F, B[a]P, and B[b]F, respectively, while the corresponding values for the same PAHs were 22.51, 27.24, and 26.58 ìg g-1 when PABA-MCM-41 was used. The experimental kinetic data were fitted using the pseudo-second order model, and the Langmuir isotherm model was able to describe the process of PAH adsorption. At higher temperatures, there were increases in the initial adsorption rate and the kinetic constant for adsorption of the PAHs by PABA-MCM-41. The thermodynamic parameters indicated that the processes are spontaneous, endothermic, and with a tendency towards disorder of the system at the adsorbent/adsorbate interface. Functionalization of MCM-41 increased the efficiency of adsorption of the PAHs by 44.5, 48.4, and 32.0% for B[k]F, B[a]P, and B[b]F, respectively.
publishDate 2013
dc.date.issued.fl_str_mv 2013-10-23
dc.date.accessioned.fl_str_mv 2017-09-27T13:57:41Z
dc.date.available.fl_str_mv 2017-09-27T13:57:41Z
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