Avaliação de catalisadores de cobre derivados de hidróxidos duplos lamelares para reação de deslocamento água-gás
Ano de defesa: | 2013 |
---|---|
Autor(a) principal: | |
Orientador(a): | |
Banca de defesa: | , |
Tipo de documento: | Dissertação |
Tipo de acesso: | Acesso aberto |
Idioma: | por |
Instituição de defesa: |
Universidade Federal de Santa Maria
|
Programa de Pós-Graduação: |
Programa de Pós-Graduação em Engenharia de Processos
|
Departamento: |
Engenharia de Processos
|
País: |
BR
|
Palavras-chave em Português: | |
Palavras-chave em Inglês: | |
Área do conhecimento CNPq: | |
Link de acesso: | http://repositorio.ufsm.br/handle/1/7967 |
Resumo: | Hydrogen is considered the fuel of the future, due to its high energy density and its application in fuel cells. Hydrogen is mainly obtained by light hydrocarbons reforming. In this process, the reaction product is a gas mixture composed by hydrogen, carbon monoxide and dioxide. However, carbon monoxide (CO) concentration in this mixture is extremely high for some applications, such as ammonia synthesis and fuel cells processes, where CO acts as a poison for some types of catalysts. To remove CO excess and improve hydrogen yield in reforming processes, it is used the Water-Gas Shift Reaction, which occurs in two steps: at high temperatures, around 400°C with Fe-Cr catalysts; and at low temperatures, around 250°C with Cu-Zn catalysts. The goal of this work was to develop and to evaluate copper, zinc and aluminum based catalysts derived from Lamellar Double Hydroxides (LDH) for the low temperature Water-Gas Shift Reaction. LDH, also called hydrotalcite-like materials, have useful properties for catalysis, such as homogeneous metal distribution throughout its structure, improving thermal stability and catalytic activity. An experimental design for the composition variables, Cu/Zn and (Cu+Zn)/Al molar ratios, was used, besides the aging treatment influence over LDH, which was verified by replicating the experiments in two groups: with and without aging. The catalysts were prepared by the co-precipitation method; and it was analyzed the influence of preparation conditions over their physical-chemical properties, such as composition, specific area, porous volume and diameter, as well as catalytic activity in low temperature Water-Gas Shift Reaction. The presence of Cu/Zn/Al LDH phase in all prepared catalysts was verified. In some samples, there were a few impurities, like malachite and aurichalcite in aged catalysts, and zinc and copper oxides in not aged materials. The aging step also affected the way the Cu/Zn and (Cu+Zn)/Al molar ratios influence the textural properties and the catalytic activity. In aged catalysts, the specific area does not show a strong dependency on the composition. However, these catalysts appear to have higher thermal stability in long period reactions. Experimental design allowed a better study of the influence of composition variables on catalysts final characteristics, aiding future studies in the synthesis of this type of material. |
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2014-06-112014-06-112013-03-11RIBEIRO, Glênio Rosinski. EVALUATION OF COPPER-BASED CATALYSTS DERIVED FROM LAMELAR DOUBLE HYDROXIDES FOR WATER-GAS SHIFT REACTION. 2013. 92 f. Dissertação (Mestrado em Engenharia) - Universidade Federal de Santa Maria, Santa Maria, 2013.http://repositorio.ufsm.br/handle/1/7967Hydrogen is considered the fuel of the future, due to its high energy density and its application in fuel cells. Hydrogen is mainly obtained by light hydrocarbons reforming. In this process, the reaction product is a gas mixture composed by hydrogen, carbon monoxide and dioxide. However, carbon monoxide (CO) concentration in this mixture is extremely high for some applications, such as ammonia synthesis and fuel cells processes, where CO acts as a poison for some types of catalysts. To remove CO excess and improve hydrogen yield in reforming processes, it is used the Water-Gas Shift Reaction, which occurs in two steps: at high temperatures, around 400°C with Fe-Cr catalysts; and at low temperatures, around 250°C with Cu-Zn catalysts. The goal of this work was to develop and to evaluate copper, zinc and aluminum based catalysts derived from Lamellar Double Hydroxides (LDH) for the low temperature Water-Gas Shift Reaction. LDH, also called hydrotalcite-like materials, have useful properties for catalysis, such as homogeneous metal distribution throughout its structure, improving thermal stability and catalytic activity. An experimental design for the composition variables, Cu/Zn and (Cu+Zn)/Al molar ratios, was used, besides the aging treatment influence over LDH, which was verified by replicating the experiments in two groups: with and without aging. The catalysts were prepared by the co-precipitation method; and it was analyzed the influence of preparation conditions over their physical-chemical properties, such as composition, specific area, porous volume and diameter, as well as catalytic activity in low temperature Water-Gas Shift Reaction. The presence of Cu/Zn/Al LDH phase in all prepared catalysts was verified. In some samples, there were a few impurities, like malachite and aurichalcite in aged catalysts, and zinc and copper oxides in not aged materials. The aging step also affected the way the Cu/Zn and (Cu+Zn)/Al molar ratios influence the textural properties and the catalytic activity. In aged catalysts, the specific area does not show a strong dependency on the composition. However, these catalysts appear to have higher thermal stability in long period reactions. Experimental design allowed a better study of the influence of composition variables on catalysts final characteristics, aiding future studies in the synthesis of this type of material.O hidrogênio é considerado o combustível do futuro, devido a sua alta densidade energética e a sua aplicação em células a combustível. A obtenção de hidrogênio ocorre, principalmente, através da reforma de hidrocarbonetos leves. Neste processo, o produto da reação de reforma é uma corrente gasosa composta por hidrogênio, monóxido e dióxido de carbono. Entretanto, as concentrações do monóxido de carbono (CO) na mistura reacional são extremamente elevadas para certas aplicações, como síntese de amônia e utilização em células a combustível, em que o CO atua como veneno para alguns tipos de catalisadores. Para remover o excesso de CO e aumentar o rendimento a hidrogênio nos processos de reforma, é utilizada a reação de deslocamento água-gás (Water-Gas Shift), que ocorre em dois estágios: a altas temperaturas, em torno de 400°C com catalisadores de Fe-Cr; e a baixas temperaturas, em torno de 250°C com catalisadores de Cu-Zn. O objetivo deste trabalho foi desenvolver e avaliar catalisadores de cobre, zinco e alumínio derivados de Hidróxidos Duplos Lamelares (HDL) para a reação de deslocamento água-gás a baixas temperaturas. Os HDL, também denominados materiais do tipo hidrotalcita, possuem características úteis à catálise, como a distribuição homogênea de metais na sua estrutura, proporcionando uma maior estabilidade térmica e atividade ao catalisador. Foi utilizado um planejamento de experimentos para as duas variáveis de composição, as razões molares Cu/Zn e (Cu+Zn)/Al, além de replicá-los em dois grupos de experimentos com e sem envelhecimento, para verificar a influência desta etapa nas propriedades dos HDL. Os catalisadores foram preparados por coprecipitação; e foi analisada a influência das condições de preparo sobre suas propriedades físico-químicas, tais como composição, área específica, volume e diâmetro médio de poros, além da atividade catalítica na reação de deslocamento água-gás a baixas temperaturas. Foi possível verificar a presença da fase de HDL de Cu/Zn/Al em todos os catalisadores obtidos. Em algumas amostras, houve a formação de pequenas impurezas, como malaquita e auricalcita, nos catalisadores envelhecidos, e óxidos de cobre e de zinco nos materiais sem envelhecimento. A etapa de envelhecimento também afetou a influência das razões molares Cu/Zn e (Cu+Zn)/Al sobre as propriedades texturais dos catalisadores e sobre a atividade catalítica. Para catalisadores envelhecidos, a área específica não depende de forma expressiva da composição. Entretanto, estes catalisadores aparentam possuir maior estabilidade térmica em reações prolongadas. O planejamento de experimentos permitiu um melhor estudo de influência das variáveis de composição nas características finais dos catalisadores, auxiliando futuros estudos de síntese deste tipo de material.Coordenação de Aperfeiçoamento de Pessoal de Nível Superiorapplication/pdfporUniversidade Federal de Santa MariaPrograma de Pós-Graduação em Engenharia de ProcessosUFSMBREngenharia de ProcessosEngenharia de produçãoCatalisadoresHidrogênioProduction engineeringCatalystsHydrogenCNPQ::ENGENHARIAS::ENGENHARIA DE PRODUCAOAvaliação de catalisadores de cobre derivados de hidróxidos duplos lamelares para reação de deslocamento água-gásEvaluation of copper-based catalysts derived from lamelar double hydroxides for water-gas shift reactioninfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/masterThesisSchwaab, Marciohttp://lattes.cnpq.br/7572439258027513Coutinho, Elisa Barbosahttp://lattes.cnpq.br/0551304679934048Souza, Mariana de Mattos Vieira Mellohttp://lattes.cnpq.br/8882084525542926Castilhos, Fernanda dehttp://lattes.cnpq.br/4590978604104577http://lattes.cnpq.br/3045740221684132Ribeiro, Glênio Rosinski3008000000054003003003003003006cf90fef-7b71-4f2c-afce-8ee5697dc4defe96d77d-4fe6-4f3f-bd4c-1398df99d977fe5e7a55-7991-46a7-aa57-ea2250b2e84c00fcb2eb-5d1a-410f-83e2-c39f5f8f318ba449cb86-b983-405a-ba9d-b938f1f90e80info:eu-repo/semantics/openAccessreponame:Biblioteca Digital de Teses e Dissertações do UFSMinstname:Universidade Federal de Santa Maria (UFSM)instacron:UFSMORIGINALRIBEIRO, GLENIO ROSINSKI.pdfapplication/pdf2099486http://repositorio.ufsm.br/bitstream/1/7967/1/RIBEIRO%2c%20GLENIO%20ROSINSKI.pdf400d1b275c02a56ff821a0b791d4d0b2MD51TEXTRIBEIRO, GLENIO ROSINSKI.pdf.txtRIBEIRO, GLENIO ROSINSKI.pdf.txtExtracted texttext/plain156896http://repositorio.ufsm.br/bitstream/1/7967/2/RIBEIRO%2c%20GLENIO%20ROSINSKI.pdf.txt79132a655e6591a664164ce0ce47fd53MD52THUMBNAILRIBEIRO, GLENIO ROSINSKI.pdf.jpgRIBEIRO, GLENIO ROSINSKI.pdf.jpgIM Thumbnailimage/jpeg5069http://repositorio.ufsm.br/bitstream/1/7967/3/RIBEIRO%2c%20GLENIO%20ROSINSKI.pdf.jpg5dd899091041b86d1206a36fe18cf0e5MD531/79672022-01-24 08:53:50.788oai:repositorio.ufsm.br:1/7967Biblioteca Digital de Teses e Dissertaçõeshttps://repositorio.ufsm.br/ONGhttps://repositorio.ufsm.br/oai/requestatendimento.sib@ufsm.br||tedebc@gmail.comopendoar:2022-01-24T11:53:50Biblioteca Digital de Teses e Dissertações do UFSM - Universidade Federal de Santa Maria (UFSM)false |
dc.title.por.fl_str_mv |
Avaliação de catalisadores de cobre derivados de hidróxidos duplos lamelares para reação de deslocamento água-gás |
dc.title.alternative.eng.fl_str_mv |
Evaluation of copper-based catalysts derived from lamelar double hydroxides for water-gas shift reaction |
title |
Avaliação de catalisadores de cobre derivados de hidróxidos duplos lamelares para reação de deslocamento água-gás |
spellingShingle |
Avaliação de catalisadores de cobre derivados de hidróxidos duplos lamelares para reação de deslocamento água-gás Ribeiro, Glênio Rosinski Engenharia de produção Catalisadores Hidrogênio Production engineering Catalysts Hydrogen CNPQ::ENGENHARIAS::ENGENHARIA DE PRODUCAO |
title_short |
Avaliação de catalisadores de cobre derivados de hidróxidos duplos lamelares para reação de deslocamento água-gás |
title_full |
Avaliação de catalisadores de cobre derivados de hidróxidos duplos lamelares para reação de deslocamento água-gás |
title_fullStr |
Avaliação de catalisadores de cobre derivados de hidróxidos duplos lamelares para reação de deslocamento água-gás |
title_full_unstemmed |
Avaliação de catalisadores de cobre derivados de hidróxidos duplos lamelares para reação de deslocamento água-gás |
title_sort |
Avaliação de catalisadores de cobre derivados de hidróxidos duplos lamelares para reação de deslocamento água-gás |
author |
Ribeiro, Glênio Rosinski |
author_facet |
Ribeiro, Glênio Rosinski |
author_role |
author |
dc.contributor.advisor1.fl_str_mv |
Schwaab, Marcio |
dc.contributor.advisor1Lattes.fl_str_mv |
http://lattes.cnpq.br/7572439258027513 |
dc.contributor.advisor-co1.fl_str_mv |
Coutinho, Elisa Barbosa |
dc.contributor.advisor-co1Lattes.fl_str_mv |
http://lattes.cnpq.br/0551304679934048 |
dc.contributor.referee1.fl_str_mv |
Souza, Mariana de Mattos Vieira Mello |
dc.contributor.referee1Lattes.fl_str_mv |
http://lattes.cnpq.br/8882084525542926 |
dc.contributor.referee2.fl_str_mv |
Castilhos, Fernanda de |
dc.contributor.referee2Lattes.fl_str_mv |
http://lattes.cnpq.br/4590978604104577 |
dc.contributor.authorLattes.fl_str_mv |
http://lattes.cnpq.br/3045740221684132 |
dc.contributor.author.fl_str_mv |
Ribeiro, Glênio Rosinski |
contributor_str_mv |
Schwaab, Marcio Coutinho, Elisa Barbosa Souza, Mariana de Mattos Vieira Mello Castilhos, Fernanda de |
dc.subject.por.fl_str_mv |
Engenharia de produção Catalisadores Hidrogênio |
topic |
Engenharia de produção Catalisadores Hidrogênio Production engineering Catalysts Hydrogen CNPQ::ENGENHARIAS::ENGENHARIA DE PRODUCAO |
dc.subject.eng.fl_str_mv |
Production engineering Catalysts Hydrogen |
dc.subject.cnpq.fl_str_mv |
CNPQ::ENGENHARIAS::ENGENHARIA DE PRODUCAO |
description |
Hydrogen is considered the fuel of the future, due to its high energy density and its application in fuel cells. Hydrogen is mainly obtained by light hydrocarbons reforming. In this process, the reaction product is a gas mixture composed by hydrogen, carbon monoxide and dioxide. However, carbon monoxide (CO) concentration in this mixture is extremely high for some applications, such as ammonia synthesis and fuel cells processes, where CO acts as a poison for some types of catalysts. To remove CO excess and improve hydrogen yield in reforming processes, it is used the Water-Gas Shift Reaction, which occurs in two steps: at high temperatures, around 400°C with Fe-Cr catalysts; and at low temperatures, around 250°C with Cu-Zn catalysts. The goal of this work was to develop and to evaluate copper, zinc and aluminum based catalysts derived from Lamellar Double Hydroxides (LDH) for the low temperature Water-Gas Shift Reaction. LDH, also called hydrotalcite-like materials, have useful properties for catalysis, such as homogeneous metal distribution throughout its structure, improving thermal stability and catalytic activity. An experimental design for the composition variables, Cu/Zn and (Cu+Zn)/Al molar ratios, was used, besides the aging treatment influence over LDH, which was verified by replicating the experiments in two groups: with and without aging. The catalysts were prepared by the co-precipitation method; and it was analyzed the influence of preparation conditions over their physical-chemical properties, such as composition, specific area, porous volume and diameter, as well as catalytic activity in low temperature Water-Gas Shift Reaction. The presence of Cu/Zn/Al LDH phase in all prepared catalysts was verified. In some samples, there were a few impurities, like malachite and aurichalcite in aged catalysts, and zinc and copper oxides in not aged materials. The aging step also affected the way the Cu/Zn and (Cu+Zn)/Al molar ratios influence the textural properties and the catalytic activity. In aged catalysts, the specific area does not show a strong dependency on the composition. However, these catalysts appear to have higher thermal stability in long period reactions. Experimental design allowed a better study of the influence of composition variables on catalysts final characteristics, aiding future studies in the synthesis of this type of material. |
publishDate |
2013 |
dc.date.issued.fl_str_mv |
2013-03-11 |
dc.date.accessioned.fl_str_mv |
2014-06-11 |
dc.date.available.fl_str_mv |
2014-06-11 |
dc.type.status.fl_str_mv |
info:eu-repo/semantics/publishedVersion |
dc.type.driver.fl_str_mv |
info:eu-repo/semantics/masterThesis |
format |
masterThesis |
status_str |
publishedVersion |
dc.identifier.citation.fl_str_mv |
RIBEIRO, Glênio Rosinski. EVALUATION OF COPPER-BASED CATALYSTS DERIVED FROM LAMELAR DOUBLE HYDROXIDES FOR WATER-GAS SHIFT REACTION. 2013. 92 f. Dissertação (Mestrado em Engenharia) - Universidade Federal de Santa Maria, Santa Maria, 2013. |
dc.identifier.uri.fl_str_mv |
http://repositorio.ufsm.br/handle/1/7967 |
identifier_str_mv |
RIBEIRO, Glênio Rosinski. EVALUATION OF COPPER-BASED CATALYSTS DERIVED FROM LAMELAR DOUBLE HYDROXIDES FOR WATER-GAS SHIFT REACTION. 2013. 92 f. Dissertação (Mestrado em Engenharia) - Universidade Federal de Santa Maria, Santa Maria, 2013. |
url |
http://repositorio.ufsm.br/handle/1/7967 |
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300800000005 |
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UFSM |
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Engenharia de Processos |
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Universidade Federal de Santa Maria |
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