{"title":"二氧化铈催化微通道反应器中氮氧化物辅助异相催化燃烧烟尘的 N2O 形成机理研究","authors":"","doi":"10.1016/j.joei.2024.101842","DOIUrl":null,"url":null,"abstract":"<div><div>A CeO<sub>2</sub>-based catalytic microchannel reactor fixed-bed experiment was carried out to investigate the N<sub>2</sub>O formation in NO<sub>x</sub>-assisted catalytic combustion with fresh and hydrothermally aging catalysts during NOx-assisted heterogeneous catalytic combustion of soot. An evolved NOx-assisted soot catalytic combustion reaction mechanism was built to investigate N<sub>2</sub>O formation and key reaction pathways based on in situ Fourier Transform Infrared Spectroscopy (FTIR) diagnostics and destiny functional theory (DFT) computations. It was found that the temperature range of N<sub>2</sub>O formation was the same as the initiation temperature of soot catalytic combustion, while the significant catalytic activity of CeO<sub>2</sub> catalyst induced a decrease in the temperature range of N<sub>2</sub>O formation. The CeO<sub>2</sub> catalyst inhibited N<sub>2</sub>O formations from NOx-assisted soot catalytic combustion, while its inhibition effect was gradually weakened with the decrease of catalyst activities. The inhibitory effect of CeO<sub>2</sub> on N<sub>2</sub>O was revealed in the reduction of CN formation rate in high temperatures. Fresh CeO<sub>2</sub> catalyst increased the dominance in the CN formation reaction, reduced the CN production rate, and contributed to the decrease in the reaction rate of CNO oxidation by NO and NO<sub>2</sub>. The increase in the ratio of NOx to soot (<em>β</em>) was more sensitive to N<sub>2</sub>O formation than the ratio <em>α</em> (NO<sub>2</sub> to NOx) and <em>γ</em> (O<sub>2</sub> to NO<sub>x</sub>), led to a stronger inhibition of N<sub>2</sub>O formation.</div></div>","PeriodicalId":17287,"journal":{"name":"Journal of The Energy Institute","volume":null,"pages":null},"PeriodicalIF":5.6000,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Study of the N2O formation mechanism in NOx-assisted heterogeneous catalytic combustion of soot in CeO2-based catalytic microchannel reactor\",\"authors\":\"\",\"doi\":\"10.1016/j.joei.2024.101842\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>A CeO<sub>2</sub>-based catalytic microchannel reactor fixed-bed experiment was carried out to investigate the N<sub>2</sub>O formation in NO<sub>x</sub>-assisted catalytic combustion with fresh and hydrothermally aging catalysts during NOx-assisted heterogeneous catalytic combustion of soot. An evolved NOx-assisted soot catalytic combustion reaction mechanism was built to investigate N<sub>2</sub>O formation and key reaction pathways based on in situ Fourier Transform Infrared Spectroscopy (FTIR) diagnostics and destiny functional theory (DFT) computations. It was found that the temperature range of N<sub>2</sub>O formation was the same as the initiation temperature of soot catalytic combustion, while the significant catalytic activity of CeO<sub>2</sub> catalyst induced a decrease in the temperature range of N<sub>2</sub>O formation. The CeO<sub>2</sub> catalyst inhibited N<sub>2</sub>O formations from NOx-assisted soot catalytic combustion, while its inhibition effect was gradually weakened with the decrease of catalyst activities. The inhibitory effect of CeO<sub>2</sub> on N<sub>2</sub>O was revealed in the reduction of CN formation rate in high temperatures. Fresh CeO<sub>2</sub> catalyst increased the dominance in the CN formation reaction, reduced the CN production rate, and contributed to the decrease in the reaction rate of CNO oxidation by NO and NO<sub>2</sub>. The increase in the ratio of NOx to soot (<em>β</em>) was more sensitive to N<sub>2</sub>O formation than the ratio <em>α</em> (NO<sub>2</sub> to NOx) and <em>γ</em> (O<sub>2</sub> to NO<sub>x</sub>), led to a stronger inhibition of N<sub>2</sub>O formation.</div></div>\",\"PeriodicalId\":17287,\"journal\":{\"name\":\"Journal of The Energy Institute\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":5.6000,\"publicationDate\":\"2024-09-26\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of The Energy Institute\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1743967124003209\",\"RegionNum\":2,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"ENERGY & FUELS\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of The Energy Institute","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1743967124003209","RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENERGY & FUELS","Score":null,"Total":0}
Study of the N2O formation mechanism in NOx-assisted heterogeneous catalytic combustion of soot in CeO2-based catalytic microchannel reactor
A CeO2-based catalytic microchannel reactor fixed-bed experiment was carried out to investigate the N2O formation in NOx-assisted catalytic combustion with fresh and hydrothermally aging catalysts during NOx-assisted heterogeneous catalytic combustion of soot. An evolved NOx-assisted soot catalytic combustion reaction mechanism was built to investigate N2O formation and key reaction pathways based on in situ Fourier Transform Infrared Spectroscopy (FTIR) diagnostics and destiny functional theory (DFT) computations. It was found that the temperature range of N2O formation was the same as the initiation temperature of soot catalytic combustion, while the significant catalytic activity of CeO2 catalyst induced a decrease in the temperature range of N2O formation. The CeO2 catalyst inhibited N2O formations from NOx-assisted soot catalytic combustion, while its inhibition effect was gradually weakened with the decrease of catalyst activities. The inhibitory effect of CeO2 on N2O was revealed in the reduction of CN formation rate in high temperatures. Fresh CeO2 catalyst increased the dominance in the CN formation reaction, reduced the CN production rate, and contributed to the decrease in the reaction rate of CNO oxidation by NO and NO2. The increase in the ratio of NOx to soot (β) was more sensitive to N2O formation than the ratio α (NO2 to NOx) and γ (O2 to NOx), led to a stronger inhibition of N2O formation.
期刊介绍:
The Journal of the Energy Institute provides peer reviewed coverage of original high quality research on energy, engineering and technology.The coverage is broad and the main areas of interest include:
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