Zhi-Hao Zheng , Kai-Ru Jin , Du Wang , Wang Li , Xu-Peng Yu , Teng-Long Lv , Xiao-Dong Wang , Long Zhao , Jiu-Zhong Yang , Zhen-Yu Tian
{"title":"利用 SVUV 飞行时间质谱对异丙胺氧化进行实验和动力学建模研究","authors":"Zhi-Hao Zheng , Kai-Ru Jin , Du Wang , Wang Li , Xu-Peng Yu , Teng-Long Lv , Xiao-Dong Wang , Long Zhao , Jiu-Zhong Yang , Zhen-Yu Tian","doi":"10.1016/j.combustflame.2024.113483","DOIUrl":null,"url":null,"abstract":"<div><p>Atmospheric oxidation experiments of iso-propylamine (IPA) were conducted in a jet-stirred reactor over the temperature range from 550 to 870 K at fuel-equivalence ratios of 0.5 and 2.0. A combination of synchrotron vacuum ultraviolet (SVUV) photoionization and time-of-flight mass spectrometry (TOFMS) was utilized to identify and quantify oxidation products and intermediates. Compared to the previous n-propylamine (NPA) low-temperature oxidation [Proc. Combust. Inst., 39 (2023) 295–303.], some intermediates and products were newly observed among the 34 detected species, including nitrosyl hydride, methylamine, acetonitrile, nitrous oxide, ethyl isocyanide, propanenitrile, 2-propanimine, n-methylformamide and 2-methylallylamine. A kinetic model consisting of 815 species and 4402 reactions was developed based on the iso-propanol model [Prog. Energy Combust. Sci. 67 (2018) 31–68.] and an ethylamine model [Prog. Energy Combust. Sci. 44 (2014) 40–102.]. The onset temperature of IPA and O<sub>2</sub> consumption is 750 K under both lean and rich conditions. Rate-of-production (ROP) and sensitivity analyses were performed at 800 K to illustrate the reacting paths from parent fuel to major intermediates and products, and identify the most sensitive reactions. H<sub>2</sub>O<sub>2</sub>(+M) = 2OH(+M) is the most sensitive reaction with a promoting effect on IPA consumption while 2HO<sub>2</sub> = H<sub>2</sub>O<sub>2</sub>+O<sub>2</sub> is the most inhibiting one. Important N-containing pollutants like NH<sub>3</sub>, NOx, HCN, CH<sub>3</sub>NH<sub>2</sub> and so on were analyzed with respect to their reaction routes. (CH<sub>3</sub>)<sub>2</sub>CNH is abundant due to the H-abstraction reactions between tC<sub>3</sub>H<sub>6</sub>NH<sub>2</sub> radical with O<sub>2</sub>. This work was made for gaining a more comprehensive insight into the oxidation of IPA and make a foundation for further exploring amine chemistry.</p></div>","PeriodicalId":280,"journal":{"name":"Combustion and Flame","volume":null,"pages":null},"PeriodicalIF":5.8000,"publicationDate":"2024-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Experimental and kinetic modeling study of iso-propylamine oxidation with SVUV-time of flight mass spectrometry\",\"authors\":\"Zhi-Hao Zheng , Kai-Ru Jin , Du Wang , Wang Li , Xu-Peng Yu , Teng-Long Lv , Xiao-Dong Wang , Long Zhao , Jiu-Zhong Yang , Zhen-Yu Tian\",\"doi\":\"10.1016/j.combustflame.2024.113483\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Atmospheric oxidation experiments of iso-propylamine (IPA) were conducted in a jet-stirred reactor over the temperature range from 550 to 870 K at fuel-equivalence ratios of 0.5 and 2.0. A combination of synchrotron vacuum ultraviolet (SVUV) photoionization and time-of-flight mass spectrometry (TOFMS) was utilized to identify and quantify oxidation products and intermediates. Compared to the previous n-propylamine (NPA) low-temperature oxidation [Proc. Combust. Inst., 39 (2023) 295–303.], some intermediates and products were newly observed among the 34 detected species, including nitrosyl hydride, methylamine, acetonitrile, nitrous oxide, ethyl isocyanide, propanenitrile, 2-propanimine, n-methylformamide and 2-methylallylamine. A kinetic model consisting of 815 species and 4402 reactions was developed based on the iso-propanol model [Prog. Energy Combust. Sci. 67 (2018) 31–68.] and an ethylamine model [Prog. Energy Combust. Sci. 44 (2014) 40–102.]. The onset temperature of IPA and O<sub>2</sub> consumption is 750 K under both lean and rich conditions. Rate-of-production (ROP) and sensitivity analyses were performed at 800 K to illustrate the reacting paths from parent fuel to major intermediates and products, and identify the most sensitive reactions. H<sub>2</sub>O<sub>2</sub>(+M) = 2OH(+M) is the most sensitive reaction with a promoting effect on IPA consumption while 2HO<sub>2</sub> = H<sub>2</sub>O<sub>2</sub>+O<sub>2</sub> is the most inhibiting one. Important N-containing pollutants like NH<sub>3</sub>, NOx, HCN, CH<sub>3</sub>NH<sub>2</sub> and so on were analyzed with respect to their reaction routes. (CH<sub>3</sub>)<sub>2</sub>CNH is abundant due to the H-abstraction reactions between tC<sub>3</sub>H<sub>6</sub>NH<sub>2</sub> radical with O<sub>2</sub>. This work was made for gaining a more comprehensive insight into the oxidation of IPA and make a foundation for further exploring amine chemistry.</p></div>\",\"PeriodicalId\":280,\"journal\":{\"name\":\"Combustion and Flame\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":5.8000,\"publicationDate\":\"2024-05-06\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Combustion and Flame\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0010218024001925\",\"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":"Combustion and Flame","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0010218024001925","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}
Experimental and kinetic modeling study of iso-propylamine oxidation with SVUV-time of flight mass spectrometry
Atmospheric oxidation experiments of iso-propylamine (IPA) were conducted in a jet-stirred reactor over the temperature range from 550 to 870 K at fuel-equivalence ratios of 0.5 and 2.0. A combination of synchrotron vacuum ultraviolet (SVUV) photoionization and time-of-flight mass spectrometry (TOFMS) was utilized to identify and quantify oxidation products and intermediates. Compared to the previous n-propylamine (NPA) low-temperature oxidation [Proc. Combust. Inst., 39 (2023) 295–303.], some intermediates and products were newly observed among the 34 detected species, including nitrosyl hydride, methylamine, acetonitrile, nitrous oxide, ethyl isocyanide, propanenitrile, 2-propanimine, n-methylformamide and 2-methylallylamine. A kinetic model consisting of 815 species and 4402 reactions was developed based on the iso-propanol model [Prog. Energy Combust. Sci. 67 (2018) 31–68.] and an ethylamine model [Prog. Energy Combust. Sci. 44 (2014) 40–102.]. The onset temperature of IPA and O2 consumption is 750 K under both lean and rich conditions. Rate-of-production (ROP) and sensitivity analyses were performed at 800 K to illustrate the reacting paths from parent fuel to major intermediates and products, and identify the most sensitive reactions. H2O2(+M) = 2OH(+M) is the most sensitive reaction with a promoting effect on IPA consumption while 2HO2 = H2O2+O2 is the most inhibiting one. Important N-containing pollutants like NH3, NOx, HCN, CH3NH2 and so on were analyzed with respect to their reaction routes. (CH3)2CNH is abundant due to the H-abstraction reactions between tC3H6NH2 radical with O2. This work was made for gaining a more comprehensive insight into the oxidation of IPA and make a foundation for further exploring amine chemistry.
期刊介绍:
The mission of the journal is to publish high quality work from experimental, theoretical, and computational investigations on the fundamentals of combustion phenomena and closely allied matters. While submissions in all pertinent areas are welcomed, past and recent focus of the journal has been on:
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