Aplicação de ultrassom para remoção de enxofre e de nitrogênio do óleo diesel: avaliação de parâmetros do processo e determinação de enxofre e de nitrogênio por técnicas espectrométricas e cromatográficas
Ano de defesa: | 2011 |
---|---|
Autor(a) principal: | |
Orientador(a): | |
Banca de defesa: | , , , |
Tipo de documento: | Tese |
Tipo de acesso: | Acesso aberto |
Idioma: | por |
Instituição de defesa: |
Universidade Federal de Santa Maria
Centro de Ciências Naturais e Exatas |
Programa de Pós-Graduação: |
Programa de Pós-Graduação em Química
|
Departamento: |
Química
|
País: |
Brasil
|
Palavras-chave em Português: | |
Área do conhecimento CNPq: | |
Link de acesso: | http://repositorio.ufsm.br/handle/1/17335 |
Resumo: | In the present work, the ultrasound assisted oxidation of sulfur and nitrogen compounds present in diesel fuel was investigated. The oxidized compounds are more polar than their original forms and can be removed from oil by liquid-liquid extraction. Initially, different methods for the determination of total sulfur and nitrogen concentration were evaluated for the knowledge of sample composition before and after the treatment. For sulfur it was investigated the determination by ultraviolet fluorescence by means of direct injection in the total analyzer and also by inductively coupled plasma optical emission spectrometry (ICP OES) after sample decomposition by microwave assisted wet digestion in closed vessels. For nitrogen, the determination was performed by chemiluminescence after direct injection using the total analyzer. Moreover, chromatographic parameters were optimized for analysis of sulfur compounds by gas chromatography with pulsed flame photometric detector (GC-PFPD). Regarding to the removal process, different ultrasound systems were evaluated with different frequencies and nominal powers, among them ultrasonic baths (35 kHz and 160 W, 35 kHz and 200 W, 130 kHz and 200 W and 582 kHz e 200 W), ultrasonic horns (20 kHz and 130 W and 20 kHz and 750 W) and also a cup horn system (20 kHz and 750 W). For all systems, two oxidation mixtures were evaluated: the combination H2O2/H3PO4.12WO3 with tetraoctylammonium bromide as surfactant and also the combination H2O2/AcOH. In addition, the removal efficiency under mechanical agitation (2000 rpm) was also investigated instead of using ultrasound. Better results were obtained for lower frequencies and higher power, by using immersion probes and with the H2O2/AcOH oxidation mixture. After choosing the suitable system, process parameters were evaluated in order to obtain better efficiency, such as: reaction temperature, time of ultrasound or mechanical agitation, solvent for extraction and its amount, the amount of AcOH and H2O2, the type of the carboxylic acid, the ultrasound amplitude, the addition of gases to the reactor, the addition of auxiliary reagents to the oxidation mixture and the use of a previous solvent extraction before the oxidative process. After process parameters optimization the diesel oil samples, with different initial sulfur and nitrogen concentrations and different classes of sulfur compounds were submitted to the oxidative process, with and without ultrasound. Using 7 min of ultrasound (20 kHz, 750 W, amplitude of 40%) at 90 °C, for the treatment of 25 mL of diesel oil, using molar proportion of S+N:H2O2:AcOH corresponding to 1:28:557 and extraction with MeOH (3x8 mL) the removal efficiency was from 80 to 86% for sulfur and from 74 to 91% for nitrogen. Without ultrasound under the same experimental conditions, the sulfur and nitrogen removal efficiency were from 50 to 75% and 75 to 90%, respectively, indicating the improvement of the ultrasound energy on the sulfur removal efficiency. |
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2019-07-05T18:46:25Z2019-07-05T18:46:25Z2011-09-29http://repositorio.ufsm.br/handle/1/17335In the present work, the ultrasound assisted oxidation of sulfur and nitrogen compounds present in diesel fuel was investigated. The oxidized compounds are more polar than their original forms and can be removed from oil by liquid-liquid extraction. Initially, different methods for the determination of total sulfur and nitrogen concentration were evaluated for the knowledge of sample composition before and after the treatment. For sulfur it was investigated the determination by ultraviolet fluorescence by means of direct injection in the total analyzer and also by inductively coupled plasma optical emission spectrometry (ICP OES) after sample decomposition by microwave assisted wet digestion in closed vessels. For nitrogen, the determination was performed by chemiluminescence after direct injection using the total analyzer. Moreover, chromatographic parameters were optimized for analysis of sulfur compounds by gas chromatography with pulsed flame photometric detector (GC-PFPD). Regarding to the removal process, different ultrasound systems were evaluated with different frequencies and nominal powers, among them ultrasonic baths (35 kHz and 160 W, 35 kHz and 200 W, 130 kHz and 200 W and 582 kHz e 200 W), ultrasonic horns (20 kHz and 130 W and 20 kHz and 750 W) and also a cup horn system (20 kHz and 750 W). For all systems, two oxidation mixtures were evaluated: the combination H2O2/H3PO4.12WO3 with tetraoctylammonium bromide as surfactant and also the combination H2O2/AcOH. In addition, the removal efficiency under mechanical agitation (2000 rpm) was also investigated instead of using ultrasound. Better results were obtained for lower frequencies and higher power, by using immersion probes and with the H2O2/AcOH oxidation mixture. After choosing the suitable system, process parameters were evaluated in order to obtain better efficiency, such as: reaction temperature, time of ultrasound or mechanical agitation, solvent for extraction and its amount, the amount of AcOH and H2O2, the type of the carboxylic acid, the ultrasound amplitude, the addition of gases to the reactor, the addition of auxiliary reagents to the oxidation mixture and the use of a previous solvent extraction before the oxidative process. After process parameters optimization the diesel oil samples, with different initial sulfur and nitrogen concentrations and different classes of sulfur compounds were submitted to the oxidative process, with and without ultrasound. Using 7 min of ultrasound (20 kHz, 750 W, amplitude of 40%) at 90 °C, for the treatment of 25 mL of diesel oil, using molar proportion of S+N:H2O2:AcOH corresponding to 1:28:557 and extraction with MeOH (3x8 mL) the removal efficiency was from 80 to 86% for sulfur and from 74 to 91% for nitrogen. Without ultrasound under the same experimental conditions, the sulfur and nitrogen removal efficiency were from 50 to 75% and 75 to 90%, respectively, indicating the improvement of the ultrasound energy on the sulfur removal efficiency.No presente trabalho investigou-se a aplicabilidade do ultrassom no processo de oxitratamento para conversão de compostos de enxofre e de nitrogênio em óleo diesel às suas formas oxidadas, que são mais polares e podem ser removidas por extração líquido-líquido. Inicialmente, foram avaliados diferentes métodos de determinação de enxofre e de nitrogênio total para o conhecimento da composição das amostras antes do processo e avaliação das concentrações finais no óleo diesel após o tratamento. Para enxofre, foi avaliada a determinação por fluorescência no ultravioleta após injeção direta da amostra utilizando um analisador total e, também, a determinação por espectrometria de emissão óptica com plasma indutivamente acoplado (ICP OES) após prévia decomposição das amostras por via úmida assistida por radiação micro-ondas em sistema fechado. Para nitrogênio, a determinação foi feita por quimiluminescência após injeção direta utilizando analisador total. Além disso, foram otimizados os parâmetros cromatográficos para determinação de compostos de enxofre por cromatografia a gás com detector fotométrico de chama pulsada (GC-PFPD). Em relação ao processo de remoção de enxofre e de nitrogênio foram avaliados diferentes sistemas de aplicação de ultrassom com frequências e potências nominais variadas, sendo eles banhos (35 kHz e 160 W, 35 kHz e 200 W, 130 kHz e 200 W e 582 kHz e 200 W), sondas (20 kHz e 130 W e 20 kHz e 750 W) e um sistema tipo cup horn (20 kHz e 750 W). Para todos os sistemas, duas misturas de oxidação foram avaliadas: a combinação H2O2/H3PO4.12WO3 na presença de brometo de tetraoctilamônio como surfactante e a combinação H2O2/AcOH. Paralelamente, foi investigada a eficiência de remoção utilizando agitação mecânica (2000 rpm) em substituição ao ultrassom. Melhores resultados foram obtidos para frequências mais baixas e potências mais altas, com o uso de sondas com probes de imersão e com a mistura de oxidação H2O2/AcOH. Após a escolha do melhor sistema, foram avaliados os parâmetros do processo na busca da melhor eficiência de remoção, tais como: temperatura, o tempo de aplicação de ultrassom ou agitação mecânica, o solvente de extração e sua quantidade, a quantidade de AcOH e de H2O2, o tipo de ácido carboxílico para a formação do perácido orgânico, a amplitude de ultrassom, a adição de gases ao reator, a adição de reagentes auxiliares à mistura de oxidação e a aplicabilidade de uma etapa de pré-extração com solvente antes da etapa de oxitratamento. Após a definição dos parâmetros do processo, as amostras de óleo diesel, com diferentes concentrações iniciais de enxofre e de nitrogênio total e diferente classes de compostos de enxofre foram submetidas ao oxitratamento, com e sem aplicação de ultrassom. Dentre os resultados obtidos, para o processo com 7 min de ultrassom (20 kHz, 750 W, amplitude de 40%) a 90 °C, para o tratamento de 25 mL de óleo diesel, utilizando a proporção molar S+N:H2O2:AcOH de 1:28:557 e extração com MeOH (3x8 mL) a eficiência de remoção ficou entre 80 e 86% para enxofre e entre 74 e 91% para nitrogênio, para todas as amostras. Sem a aplicação de ultrassom, nas mesmas condições de processo, a remoção de enxofre foi de 50 a 75% e a de nitrogênio foi de 75 a 90%, mostrando que, para enxofre, o emprego de ultrassom contribui para a melhoria da eficiência do processo de remoção.Coordenação de Aperfeiçoamento de Pessoal de Nível Superior - CAPESporUniversidade Federal de Santa MariaCentro de Ciências Naturais e ExatasPrograma de Pós-Graduação em QuímicaUFSMBrasilQuímicaAttribution-NonCommercial-NoDerivatives 4.0 Internationalhttp://creativecommons.org/licenses/by-nc-nd/4.0/info:eu-repo/semantics/openAccessQuímica analíticaÓleo dieselEnxofreNitrogênioDeterminaçãoCompostosUltrassomCNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICAAplicação de ultrassom para remoção de enxofre e de nitrogênio do óleo diesel: avaliação de parâmetros do processo e determinação de enxofre e de nitrogênio por técnicas espectrométricas e cromatográficasinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/doctoralThesisFlores, Érico Marlon de Moraeshttp://lattes.cnpq.br/7167629055579212Müller, Edson Irineuhttp://lattes.cnpq.br/5994311290376153Duarte, Fábio Andreihttp://lattes.cnpq.br/3503633944419329Barin, Juliano Smaniotohttp://lattes.cnpq.br/7545847424095994Dressler, Valderi Luizhttp://lattes.cnpq.br/4054740296547580http://lattes.cnpq.br/2189500441942469Mello, Paola de Azevedo100600000000600a9c2788c-7913-4d7b-92e1-3429800ac028cfc00b10-ce4d-479e-85f3-972480787a1348134181-e983-450f-9543-d2f1522e87a97b2cc41c-5584-4228-a9bf-b1eb4d91e1e461d23861-d241-4d88-80dc-1de363d97bcf041d14df-2bfb-4de7-ba28-c81b80787eaereponame:Biblioteca Digital de Teses e Dissertações do UFSMinstname:Universidade Federal de Santa Maria (UFSM)instacron:UFSMORIGINALTES_PPGQUIMICA_2011_MELLO_PAOLA.pdfTES_PPGQUIMICA_2011_MELLO_PAOLA.pdfTese de Doutoradoapplication/pdf563275http://repositorio.ufsm.br/bitstream/1/17335/1/TES_PPGQUIMICA_2011_MELLO_PAOLA.pdf05ba5243984b561c9922e4baf3acecabMD51CC-LICENSElicense_rdflicense_rdfapplication/rdf+xml; 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dc.title.por.fl_str_mv |
Aplicação de ultrassom para remoção de enxofre e de nitrogênio do óleo diesel: avaliação de parâmetros do processo e determinação de enxofre e de nitrogênio por técnicas espectrométricas e cromatográficas |
title |
Aplicação de ultrassom para remoção de enxofre e de nitrogênio do óleo diesel: avaliação de parâmetros do processo e determinação de enxofre e de nitrogênio por técnicas espectrométricas e cromatográficas |
spellingShingle |
Aplicação de ultrassom para remoção de enxofre e de nitrogênio do óleo diesel: avaliação de parâmetros do processo e determinação de enxofre e de nitrogênio por técnicas espectrométricas e cromatográficas Mello, Paola de Azevedo Química analítica Óleo diesel Enxofre Nitrogênio Determinação Compostos Ultrassom CNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICA |
title_short |
Aplicação de ultrassom para remoção de enxofre e de nitrogênio do óleo diesel: avaliação de parâmetros do processo e determinação de enxofre e de nitrogênio por técnicas espectrométricas e cromatográficas |
title_full |
Aplicação de ultrassom para remoção de enxofre e de nitrogênio do óleo diesel: avaliação de parâmetros do processo e determinação de enxofre e de nitrogênio por técnicas espectrométricas e cromatográficas |
title_fullStr |
Aplicação de ultrassom para remoção de enxofre e de nitrogênio do óleo diesel: avaliação de parâmetros do processo e determinação de enxofre e de nitrogênio por técnicas espectrométricas e cromatográficas |
title_full_unstemmed |
Aplicação de ultrassom para remoção de enxofre e de nitrogênio do óleo diesel: avaliação de parâmetros do processo e determinação de enxofre e de nitrogênio por técnicas espectrométricas e cromatográficas |
title_sort |
Aplicação de ultrassom para remoção de enxofre e de nitrogênio do óleo diesel: avaliação de parâmetros do processo e determinação de enxofre e de nitrogênio por técnicas espectrométricas e cromatográficas |
author |
Mello, Paola de Azevedo |
author_facet |
Mello, Paola de Azevedo |
author_role |
author |
dc.contributor.advisor1.fl_str_mv |
Flores, Érico Marlon de Moraes |
dc.contributor.advisor1Lattes.fl_str_mv |
http://lattes.cnpq.br/7167629055579212 |
dc.contributor.referee1.fl_str_mv |
Müller, Edson Irineu |
dc.contributor.referee1Lattes.fl_str_mv |
http://lattes.cnpq.br/5994311290376153 |
dc.contributor.referee2.fl_str_mv |
Duarte, Fábio Andrei |
dc.contributor.referee2Lattes.fl_str_mv |
http://lattes.cnpq.br/3503633944419329 |
dc.contributor.referee3.fl_str_mv |
Barin, Juliano Smanioto |
dc.contributor.referee3Lattes.fl_str_mv |
http://lattes.cnpq.br/7545847424095994 |
dc.contributor.referee4.fl_str_mv |
Dressler, Valderi Luiz |
dc.contributor.referee4Lattes.fl_str_mv |
http://lattes.cnpq.br/4054740296547580 |
dc.contributor.authorLattes.fl_str_mv |
http://lattes.cnpq.br/2189500441942469 |
dc.contributor.author.fl_str_mv |
Mello, Paola de Azevedo |
contributor_str_mv |
Flores, Érico Marlon de Moraes Müller, Edson Irineu Duarte, Fábio Andrei Barin, Juliano Smanioto Dressler, Valderi Luiz |
dc.subject.por.fl_str_mv |
Química analítica Óleo diesel Enxofre Nitrogênio Determinação Compostos Ultrassom |
topic |
Química analítica Óleo diesel Enxofre Nitrogênio Determinação Compostos Ultrassom CNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICA |
dc.subject.cnpq.fl_str_mv |
CNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICA |
description |
In the present work, the ultrasound assisted oxidation of sulfur and nitrogen compounds present in diesel fuel was investigated. The oxidized compounds are more polar than their original forms and can be removed from oil by liquid-liquid extraction. Initially, different methods for the determination of total sulfur and nitrogen concentration were evaluated for the knowledge of sample composition before and after the treatment. For sulfur it was investigated the determination by ultraviolet fluorescence by means of direct injection in the total analyzer and also by inductively coupled plasma optical emission spectrometry (ICP OES) after sample decomposition by microwave assisted wet digestion in closed vessels. For nitrogen, the determination was performed by chemiluminescence after direct injection using the total analyzer. Moreover, chromatographic parameters were optimized for analysis of sulfur compounds by gas chromatography with pulsed flame photometric detector (GC-PFPD). Regarding to the removal process, different ultrasound systems were evaluated with different frequencies and nominal powers, among them ultrasonic baths (35 kHz and 160 W, 35 kHz and 200 W, 130 kHz and 200 W and 582 kHz e 200 W), ultrasonic horns (20 kHz and 130 W and 20 kHz and 750 W) and also a cup horn system (20 kHz and 750 W). For all systems, two oxidation mixtures were evaluated: the combination H2O2/H3PO4.12WO3 with tetraoctylammonium bromide as surfactant and also the combination H2O2/AcOH. In addition, the removal efficiency under mechanical agitation (2000 rpm) was also investigated instead of using ultrasound. Better results were obtained for lower frequencies and higher power, by using immersion probes and with the H2O2/AcOH oxidation mixture. After choosing the suitable system, process parameters were evaluated in order to obtain better efficiency, such as: reaction temperature, time of ultrasound or mechanical agitation, solvent for extraction and its amount, the amount of AcOH and H2O2, the type of the carboxylic acid, the ultrasound amplitude, the addition of gases to the reactor, the addition of auxiliary reagents to the oxidation mixture and the use of a previous solvent extraction before the oxidative process. After process parameters optimization the diesel oil samples, with different initial sulfur and nitrogen concentrations and different classes of sulfur compounds were submitted to the oxidative process, with and without ultrasound. Using 7 min of ultrasound (20 kHz, 750 W, amplitude of 40%) at 90 °C, for the treatment of 25 mL of diesel oil, using molar proportion of S+N:H2O2:AcOH corresponding to 1:28:557 and extraction with MeOH (3x8 mL) the removal efficiency was from 80 to 86% for sulfur and from 74 to 91% for nitrogen. Without ultrasound under the same experimental conditions, the sulfur and nitrogen removal efficiency were from 50 to 75% and 75 to 90%, respectively, indicating the improvement of the ultrasound energy on the sulfur removal efficiency. |
publishDate |
2011 |
dc.date.issued.fl_str_mv |
2011-09-29 |
dc.date.accessioned.fl_str_mv |
2019-07-05T18:46:25Z |
dc.date.available.fl_str_mv |
2019-07-05T18:46:25Z |
dc.type.status.fl_str_mv |
info:eu-repo/semantics/publishedVersion |
dc.type.driver.fl_str_mv |
info:eu-repo/semantics/doctoralThesis |
format |
doctoralThesis |
status_str |
publishedVersion |
dc.identifier.uri.fl_str_mv |
http://repositorio.ufsm.br/handle/1/17335 |
url |
http://repositorio.ufsm.br/handle/1/17335 |
dc.language.iso.fl_str_mv |
por |
language |
por |
dc.relation.cnpq.fl_str_mv |
100600000000 |
dc.relation.confidence.fl_str_mv |
600 |
dc.relation.authority.fl_str_mv |
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Universidade Federal de Santa Maria Centro de Ciências Naturais e Exatas |
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