Universidade Do Estado Do Rio De Janeiro Centro De Tecnologia E Ciências Instituto De Química

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Universidade Do Estado Do Rio De Janeiro Centro De Tecnologia E Ciências Instituto De Química Universidade do Estado do Rio de Janeiro Centro de Tecnologia e Ciências Instituto de Química David Caetano Santos Estudo de estabilidade de petróleos e modelagem do parâmetro de solubilidade de petróleos e asfaltenos Rio de Janeiro 2017 David Caetano Santos Estudo de estabilidade de petróleos e modelagem do parâmetro de solubilidade de petróleos e asfaltenos Tese apresentada como requisito parcial para obtenção do título de Doutor ao Programa de Pós-Graduação em Engenharia Química da Universidade do Estado do Rio de Janeiro. Área de Concentração: Processos Químicos, Petróleo e Meio Ambiente. Orientadores: Prof. Dr. Márcio Luís Lyra Paredes Prof. Dr. Eduardo Rocha de Almeida Lima Rio de Janeiro 2017 CATALOGAÇÃO NA FONTE UERJ/REDE SIRIUS/CTC/Q S237 Santos, David Caetano Estudo de estabilidade de petróleos e modelagem do parâmetro de solubilidade de petróleos e asfaltenos. / David Caetano Santos. – 2017. 193 f. Orientador: Márcio Luis Lyra Paredes Co-orientador: Eduardo Rocha de Almeida Lima Tese (Doutorado) – Universidade do Estado do Rio de Janeiro, Instituto de Química. 1. Petróleo - Teses. 2. Asfalteno – Teses. 3. Solubilidade – Teses I. Paredes, Márcio Luis Lyra II. Lima, Eduardo Rocha de Almeida III. Universidade do Estado do Rio de Janeiro. Instituto de Química. IV. Título. CDU 622.323 Autorizo, apenas para fins acadêmicos e científicos, a reprodução total ou parcial desta tese. ____________________________________________ ___________________________ Assinatura Data David Caetano Santos Estudo de estabilidade de petróleos e modelagem do parâmetro de solubilidade de petróleos e asfaltenos Tese apresentada como requisito parcial para obtenção do título de Doutor ao Programa de Pós-Graduação em Engenharia Química da Universidade do Estado do Rio de Janeiro. Área de Concentração: Processos Químicos, Petróleo e Meio Ambiente. Aprovado em 16 de outubro de 2017 Orientadores: Prof. Dr. Márcio Luis Lyra Paredes Instituto de Química - UERJ Prof. Dr. Eduardo Rocha de Almeida Lima Instituto de Química - UERJ Banca examinadora: ____________________________________________ Prof. Dr. Cláudio Dariva Instituto de Tecnologia e Pesquisa - UNIT ____________________________________________ Prof. Dr. Papa Matar Ndiaye Escola de Química - UFRJ ____________________________________________ Dr. Felipe Mauro Rena Cardoso Centro de Pesquisas e Desenvolvimento Leopoldo Américo Miguêz de Melo - Petrobras ____________________________________________ Prof. Dr. Marco Antonio Gaya de Figueiredo Instituto de Química – UERJ ____________________________________________ Prof. Dr. Pedro Henrique Rodrigues Alijó Instituto de Química – UERJ Rio de Janeiro 2017 DEDICATÓRIA Dedico e apresento a Deus este trabalho que me foi confiado, pois ao longo desses quase cinco anos de doutorado Ele demonstrou sua fidelidade me capacitando para desenvolver com excelência esta tese. Dedico a minha esposa Lucivania por sempre compreender a necessidade de por muitas vezes ter que colocar este trabalho como prioridade. Também pelo incentivo e apoio que ultrapassou todos os limites, a partir do qual ela demonstrou seu verdadeiro amor e amizade. Dedico aos meus pais Adabel Caetano e Vilma Magalhães, pela educação que recebi, a qual é um legado que sempre abriram muitas portas em minha vida. Dedico também aos meus filhos Davi e Amanda que são as minhas principais fontes de motivação. AGRADECIMENTOS Aproveito este espaço para expressar a gratidão e admiração que tenho pelos professores Márcio Luís Lira Paredes e Eduardo Rocha de Almeida Lima do Instituto de Química da UERJ, os quais me aceitaram como aluno de doutorado investindo muita dedicação e paciência nesse processo de orientação. Tal investimento me possibilitou avançar muitas etapas da minha vida profissional. Sem dúvida, as páginas desta tese indicam a qualidade da orientação que recebi. Agradeço a Petrobras S.A. por financiar parte dos estudos, além de todo apoio material para a pesquisa. Também a CAPES pelo financiamento de bolsas de estudo durante todo o período de doutoramento. Mas quem sou eu, e quem é o meu povo para que pudéssemos contribuir tão generosamente como fizemos? Tudo vem de ti, e nós apenas te demos o que vem das tuas mãos. 1 Crônicas 29:14 RESUMO Santos, David Caetano. Estudo de estabilidade de petróleos e modelagem do parâmetro de solubilidade de petróleos e asfaltenos. Brasil, 2017, 285f. Tese (Doutorado em Engenharia Química) – Instituto de Química, Universidade do Estado do Rio de Janeiro, Rio de Janeiro, 2017. O desenvolvimento de modelos para a previsão do parâmetro de solubilidade de petróleos e frações pesadas é o principal motivador deste estudo. Esta propriedade vem se tornando uma referência para inúmeras aplicações na indústria de petróleo e tem encontrado sua maior aplicação para previsão da compatibilidade e estabilidade de petróleos. O parâmetro de solubilidade é uma propriedade termodinâmica que “nasce” dentro da concepção de uma teoria de soluções - a chamada teoria das soluções regulares - idealizada por J. H. Hildebrand e pode ser facilmente calculada a partir da entalpia de vaporização e dados de composição de misturas. No entanto, a obtenção dos dados dessas duas propriedades para petróleos é uma etapa crítica, desde que são misturas extremamente complexas em termos composicionais e possuem frações que não vaporizam, as quais são justamente as principais responsáveis por problemas relacionados à incompatibilidade e instabilidade de misturas de petróleos. Desta forma, nesta tese, foram realizadas várias ratificações relacionadas a um método experimental para previsão do parâmetro de solubilidade de petróleos o qual é baseado em dados de floculação dos asfaltenos. O valor numérico obtido a partir desse método é considerado um dado pseudoexperimental e se tornou uma ferramenta útil para mensurar a qualidade dos resultados obtidos a partir dos novos modelos propostos nessa tese. A partir de então, exploraram-se as informações termodinâmicas existentes entre a energia coesiva e à pressão interna para calcular o parâmetro de solubilidade dos petróleos. Embora esta relação já tenha sido objeto de numerosos estudos, ainda não tinha sido explorada sistematicamente para petróleos. Dados de velocidade do som, densidade e capacidade calorífica a pressão constante de hidrocarbonetos puros foram utilizados para ajustar os modelos. Portanto, são propostos modelos para estimar o parâmetro de solubilidade de petróleos em uma forma termodinamicamente consistente usando apenas propriedades monofásicas ao invés dos dados usuais de vaporização. Novas correlações empíricas baseadas na relação da energia potencial e em simplificações da expressão analítica da pressão interna também são propostas. A modelagem termodinâmica dos dados experimentais de floculação dos asfaltenos foi realizada a partir de modificações dos chamados “modelos de solubilidade”. Como resultado, são demonstradas algumas modificações e estratégias numéricas para a utilização desses modelos que renderam bons resultados tanto qualitativos quanto quantitativos. Por fim, foi desenvolvida uma equação de estado cúbica parametrizada somente com dados de sistemas monofásicos mais o parâmetro de solubilidade. Com esta proposta, além do parâmetro de solubilidade, o coeficiente de compressibilidade isotérmica, o coeficiente de expansão térmica, a velocidade do som e a densidade de hidrocarbonetos tipicamente encontrados nas frações C7+ foram adequadamente modelados. Além disso, o modelo proposto prevê um fator de compressibilidade crítico dependente da substância. Na medida em que (até onde se pôde averiguar) nenhuma equação de estado cúbica disponível na literatura foi capaz de prever o parâmetro de solubilidade, mantendo uma descrição adequada das propriedades PVT (especialmente a compressibilidade de líquidos), esses resultados são importantes, pois demonstram que estratégias numéricas diferenciadas para a parametrização desse tipo de equação são eficazes e possibilitam avançar em aplicações em que as equações de estado cúbicas encontram dificuldades. Palavras-chave: Petróleo. Asfalteno. Parâmetro de solubilidade. Pressão interna. ABSTRACT Santos, David Caetano, Study of Petroleum Stability and Modeling of the Solubility Parameter of Petroleum and Asphaltenes, Brazil, 2017, 285f. Thesis (PhD in chemical engineering) - Institute of Chemistry, Rio de Janeiro State University, Rio de Janeiro, 2017. The development of models for the prediction of the solubility parameter of crude oils and heavy oil fractions is the main motivator of this study. This property has become a reference for several applications in the petroleum industry and it has been applied mainly for the prediction of compatibility and stability of crude oils. The solubility parameter is a thermodynamic property that is originated from the solution theory - the so-called Regular Solution Theory - idealized by J. H. Hildebrand and it can be easily calculated from the enthalpy of vaporization and mixture composition data. However, obtaining data of these two properties for crude oils is a critical step since they are extremely complex mixtures in terms of their composition and have non-vaporizing species, which are precisely the main responsible for problems related to incompatibility and instability of crude oil mixtures. Thus, in this thesis, several ratifications were made related to an experimental method for predicting solubility parameter of crude oils, which is based on asphaltene flocculation data. The numerical value obtained from this method is considered a pseudo-experimental
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