Avaliação de catalisadores de cobre derivados de hidróxidos duplos lamelares para reação de deslocamento água-gás

Detalhes bibliográficos
Ano de defesa: 2013
Autor(a) principal: Ribeiro, Glênio Rosinski lattes
Orientador(a): Schwaab, Marcio lattes
Banca de defesa: Souza, Mariana de Mattos Vieira Mello lattes, Castilhos, Fernanda de lattes
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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spelling 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
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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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