Gabriel V. Oliveira , Vinícius de Macedo , Ernesto A. Urquieta-González , Zuy M. Magriotis , Cristiane A. Pereira
{"title":"用于氨的选择性催化氧化的 Fe2O3/γ-Al2O3 和 NiO/γ-Al2O3 催化剂","authors":"Gabriel V. Oliveira , Vinícius de Macedo , Ernesto A. Urquieta-González , Zuy M. Magriotis , Cristiane A. Pereira","doi":"10.1016/j.cattod.2024.114991","DOIUrl":null,"url":null,"abstract":"<div><p>Ammonia, a significant atmospheric pollutant, requires effective emission control due to its inherent toxicity and the generation of secondary pollutants like particulate matter. This control can be achieved through various methods, including catalytic processes. Therefore, our study focuses on evaluating the potential of catalysts based on iron oxide and nickel oxide supported on γ–Al<sub>2</sub>O<sub>3</sub> for the selective catalytic oxidation of NH<sub>3</sub> to N<sub>2</sub> (NH<sub>3</sub>-SCO). The γ–Al<sub>2</sub>O<sub>3</sub> was obtained by thermal decomposition of aluminum hydroxide, and 5 or 10 wt% of Fe or Ni was added through wetness incipient impregnation. XRD diffractograms confirmed the formation of the γ–Al<sub>2</sub>O<sub>3</sub> phase. XRD, H<sub>2</sub>-TPR, and UV–vis DRS data showed the presence of Fe<sub>2</sub>O<sub>3</sub>, NiO, and NiAl<sub>2</sub>O<sub>4</sub> in the catalysts. Introducing metal oxides onto the support led to a drop in the specific area, pore size, pore volume, and NH<sub>3</sub> desorption, which was higher for the catalysts containing Fe. The catalysts were active in NH<sub>3</sub>-SCO, and the insertion of Fe or Ni was essential because it promoted a significant increase in the NH<sub>3</sub> conversion (∼75 % Fe and ∼55 % Ni), compared to pure support (∼8 %), mainly from 400 °C. However, doubling the metal content has not resulted in a considerable increase in NH<sub>3</sub> conversion. The N<sub>2</sub> selectivity was higher for the catalysts containing Ni (∼85 %) from 400 °C compared to catalysts containing Fe (∼76 %). Such behavior was due to the larger surface area of the Ni-containing catalysts. Despite that, the 5Fe/γ–Al<sub>2</sub>O<sub>3</sub> catalyst emerged as the most effective option for NH<sub>3</sub>-SCO applications, combining higher NH<sub>3</sub> conversion and good N<sub>2</sub> selectivity.</p></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"444 ","pages":"Article 114991"},"PeriodicalIF":5.2000,"publicationDate":"2024-08-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Fe2O3/γ-Al2O3 and NiO/γ-Al2O3 catalysts for the selective catalytic oxidation of ammonia\",\"authors\":\"Gabriel V. Oliveira , Vinícius de Macedo , Ernesto A. Urquieta-González , Zuy M. Magriotis , Cristiane A. Pereira\",\"doi\":\"10.1016/j.cattod.2024.114991\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Ammonia, a significant atmospheric pollutant, requires effective emission control due to its inherent toxicity and the generation of secondary pollutants like particulate matter. This control can be achieved through various methods, including catalytic processes. Therefore, our study focuses on evaluating the potential of catalysts based on iron oxide and nickel oxide supported on γ–Al<sub>2</sub>O<sub>3</sub> for the selective catalytic oxidation of NH<sub>3</sub> to N<sub>2</sub> (NH<sub>3</sub>-SCO). The γ–Al<sub>2</sub>O<sub>3</sub> was obtained by thermal decomposition of aluminum hydroxide, and 5 or 10 wt% of Fe or Ni was added through wetness incipient impregnation. XRD diffractograms confirmed the formation of the γ–Al<sub>2</sub>O<sub>3</sub> phase. XRD, H<sub>2</sub>-TPR, and UV–vis DRS data showed the presence of Fe<sub>2</sub>O<sub>3</sub>, NiO, and NiAl<sub>2</sub>O<sub>4</sub> in the catalysts. Introducing metal oxides onto the support led to a drop in the specific area, pore size, pore volume, and NH<sub>3</sub> desorption, which was higher for the catalysts containing Fe. The catalysts were active in NH<sub>3</sub>-SCO, and the insertion of Fe or Ni was essential because it promoted a significant increase in the NH<sub>3</sub> conversion (∼75 % Fe and ∼55 % Ni), compared to pure support (∼8 %), mainly from 400 °C. However, doubling the metal content has not resulted in a considerable increase in NH<sub>3</sub> conversion. The N<sub>2</sub> selectivity was higher for the catalysts containing Ni (∼85 %) from 400 °C compared to catalysts containing Fe (∼76 %). Such behavior was due to the larger surface area of the Ni-containing catalysts. Despite that, the 5Fe/γ–Al<sub>2</sub>O<sub>3</sub> catalyst emerged as the most effective option for NH<sub>3</sub>-SCO applications, combining higher NH<sub>3</sub> conversion and good N<sub>2</sub> selectivity.</p></div>\",\"PeriodicalId\":264,\"journal\":{\"name\":\"Catalysis Today\",\"volume\":\"444 \",\"pages\":\"Article 114991\"},\"PeriodicalIF\":5.2000,\"publicationDate\":\"2024-08-21\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Catalysis Today\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0920586124004851\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, APPLIED\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Catalysis Today","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0920586124004851","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, APPLIED","Score":null,"Total":0}
Fe2O3/γ-Al2O3 and NiO/γ-Al2O3 catalysts for the selective catalytic oxidation of ammonia
Ammonia, a significant atmospheric pollutant, requires effective emission control due to its inherent toxicity and the generation of secondary pollutants like particulate matter. This control can be achieved through various methods, including catalytic processes. Therefore, our study focuses on evaluating the potential of catalysts based on iron oxide and nickel oxide supported on γ–Al2O3 for the selective catalytic oxidation of NH3 to N2 (NH3-SCO). The γ–Al2O3 was obtained by thermal decomposition of aluminum hydroxide, and 5 or 10 wt% of Fe or Ni was added through wetness incipient impregnation. XRD diffractograms confirmed the formation of the γ–Al2O3 phase. XRD, H2-TPR, and UV–vis DRS data showed the presence of Fe2O3, NiO, and NiAl2O4 in the catalysts. Introducing metal oxides onto the support led to a drop in the specific area, pore size, pore volume, and NH3 desorption, which was higher for the catalysts containing Fe. The catalysts were active in NH3-SCO, and the insertion of Fe or Ni was essential because it promoted a significant increase in the NH3 conversion (∼75 % Fe and ∼55 % Ni), compared to pure support (∼8 %), mainly from 400 °C. However, doubling the metal content has not resulted in a considerable increase in NH3 conversion. The N2 selectivity was higher for the catalysts containing Ni (∼85 %) from 400 °C compared to catalysts containing Fe (∼76 %). Such behavior was due to the larger surface area of the Ni-containing catalysts. Despite that, the 5Fe/γ–Al2O3 catalyst emerged as the most effective option for NH3-SCO applications, combining higher NH3 conversion and good N2 selectivity.
期刊介绍:
Catalysis Today focuses on the rapid publication of original invited papers devoted to currently important topics in catalysis and related subjects. The journal only publishes special issues (Proposing a Catalysis Today Special Issue), each of which is supervised by Guest Editors who recruit individual papers and oversee the peer review process. Catalysis Today offers researchers in the field of catalysis in-depth overviews of topical issues.
Both fundamental and applied aspects of catalysis are covered. Subjects such as catalysis of immobilized organometallic and biocatalytic systems are welcome. Subjects related to catalysis such as experimental techniques, adsorption, process technology, synthesis, in situ characterization, computational, theoretical modeling, imaging and others are included if there is a clear relationship to catalysis.