{"title":"塞流反应器中 NH3/CO/O2/H2O 系统的氧化:实验和动力学模型研究","authors":"","doi":"10.1016/j.fuel.2024.133039","DOIUrl":null,"url":null,"abstract":"<div><p>Ammonia, as a carbon-free fuel, is easier to store and transport than hydrogen. Due to the high ignition energy and low reactivity of ammonia, adding hydrogen or carbon-based fuels as combustion aids may improve the ignition and burnout of ammonia. CO is an important intermediate product in the co-combustion process of ammonia and carbon-based fuels. Research on NH<sub>3</sub>/CO co-combustion will further promote the application of such co-fuel in propulsion systems and power generation. In this work, experimental results were supplemented with novel flow reactor results on the effect of NH<sub>3</sub> on CO oxidation in the absence of NO, and explained based on a detailed chemical kinetic model. The effects of temperature (1023–1223 K), NH<sub>3</sub> concentration (250–1500 ppm), and water content (1 %-10 %) on CO oxidation, NH<sub>3</sub> conversion, and NO generation were analyzed. In the NH<sub>3</sub>/CO system, the properties of CO always dominate. As the NH<sub>3</sub> content increases, NH<sub>3</sub> gradually inhibits the oxidation of CO by seizing free radicals (O, H, OH) and converting into NH<sub>2</sub>. NH<sub>2</sub> further interacts with free radicals to convert into NH or HNO, and ultimately into NO. An increase in temperature will decrease the release of NO and CO and gradually decrease the conversion of NO from NH<sub>3</sub>. However, ammonia concentration had little effect on the ratio of ammonia conversion to NO. When H<sub>2</sub>O increases from 1 % to 2 %, it has a significant inhibitory effect on the production of NO and promotes the oxidation of CO. When the water concentration increases from 5 % to 10 %, the inhibitory effect reaches saturation. The present work evaluates the amine subset of the reaction mechanism under the studied conditions and provides experimental data under different NH<sub>3</sub>/CO ratios, which can be used to construct and verify the reaction mechanism of mixed fuels of carbon-based fuels and ammonia.</p></div>","PeriodicalId":325,"journal":{"name":"Fuel","volume":null,"pages":null},"PeriodicalIF":6.7000,"publicationDate":"2024-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S0016236124021884/pdfft?md5=736fcf395eef8ac3baa0c7049d1fe94f&pid=1-s2.0-S0016236124021884-main.pdf","citationCount":"0","resultStr":"{\"title\":\"The oxidation of NH3/CO/O2/H2O system in a plug flow reactor: Experimental and kinetic modeling study\",\"authors\":\"\",\"doi\":\"10.1016/j.fuel.2024.133039\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Ammonia, as a carbon-free fuel, is easier to store and transport than hydrogen. Due to the high ignition energy and low reactivity of ammonia, adding hydrogen or carbon-based fuels as combustion aids may improve the ignition and burnout of ammonia. CO is an important intermediate product in the co-combustion process of ammonia and carbon-based fuels. Research on NH<sub>3</sub>/CO co-combustion will further promote the application of such co-fuel in propulsion systems and power generation. In this work, experimental results were supplemented with novel flow reactor results on the effect of NH<sub>3</sub> on CO oxidation in the absence of NO, and explained based on a detailed chemical kinetic model. The effects of temperature (1023–1223 K), NH<sub>3</sub> concentration (250–1500 ppm), and water content (1 %-10 %) on CO oxidation, NH<sub>3</sub> conversion, and NO generation were analyzed. In the NH<sub>3</sub>/CO system, the properties of CO always dominate. As the NH<sub>3</sub> content increases, NH<sub>3</sub> gradually inhibits the oxidation of CO by seizing free radicals (O, H, OH) and converting into NH<sub>2</sub>. NH<sub>2</sub> further interacts with free radicals to convert into NH or HNO, and ultimately into NO. An increase in temperature will decrease the release of NO and CO and gradually decrease the conversion of NO from NH<sub>3</sub>. However, ammonia concentration had little effect on the ratio of ammonia conversion to NO. When H<sub>2</sub>O increases from 1 % to 2 %, it has a significant inhibitory effect on the production of NO and promotes the oxidation of CO. When the water concentration increases from 5 % to 10 %, the inhibitory effect reaches saturation. The present work evaluates the amine subset of the reaction mechanism under the studied conditions and provides experimental data under different NH<sub>3</sub>/CO ratios, which can be used to construct and verify the reaction mechanism of mixed fuels of carbon-based fuels and ammonia.</p></div>\",\"PeriodicalId\":325,\"journal\":{\"name\":\"Fuel\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":6.7000,\"publicationDate\":\"2024-09-07\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://www.sciencedirect.com/science/article/pii/S0016236124021884/pdfft?md5=736fcf395eef8ac3baa0c7049d1fe94f&pid=1-s2.0-S0016236124021884-main.pdf\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Fuel\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0016236124021884\",\"RegionNum\":1,\"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":"Fuel","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0016236124021884","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENERGY & FUELS","Score":null,"Total":0}
引用次数: 0
摘要
氨作为一种无碳燃料,比氢更易于储存和运输。由于氨的点火能量高、反应活性低,添加氢或碳基燃料作为助燃剂可改善氨的点火和燃烧。CO 是氨和碳基燃料共燃过程中的重要中间产物。对 NH3/CO 协同燃烧的研究将进一步促进这种协同燃料在推进系统和发电中的应用。在这项工作中,实验结果得到了新型流动反应器结果的补充,即在没有 NO 的情况下,NH3 对 CO 氧化的影响,并根据详细的化学动力学模型进行了解释。分析了温度(1023-1223 K)、NH3 浓度(250-1500 ppm)和含水量(1 %-10 %)对 CO 氧化、NH3 转化和 NO 生成的影响。在 NH3/CO 系统中,CO 的特性始终占主导地位。随着 NH3 含量的增加,NH3 通过捕捉自由基(O、H、OH)并转化为 NH2,逐渐抑制 CO 的氧化。NH2 进一步与自由基相互作用,转化为 NH 或 HNO,最终转化为 NO。温度升高会减少 NO 和 CO 的释放,并逐渐减少 NO 从 NH3 的转化。然而,氨浓度对氨转化为 NO 的比例影响不大。当 H2O 从 1 % 增加到 2 % 时,对 NO 的产生有明显的抑制作用,并促进 CO 的氧化。当水的浓度从 5 % 增加到 10 % 时,抑制作用达到饱和。本研究评估了所研究条件下反应机理的胺子集,并提供了不同 NH3/CO 比例下的实验数据,可用于构建和验证碳基燃料与氨混合燃料的反应机理。
The oxidation of NH3/CO/O2/H2O system in a plug flow reactor: Experimental and kinetic modeling study
Ammonia, as a carbon-free fuel, is easier to store and transport than hydrogen. Due to the high ignition energy and low reactivity of ammonia, adding hydrogen or carbon-based fuels as combustion aids may improve the ignition and burnout of ammonia. CO is an important intermediate product in the co-combustion process of ammonia and carbon-based fuels. Research on NH3/CO co-combustion will further promote the application of such co-fuel in propulsion systems and power generation. In this work, experimental results were supplemented with novel flow reactor results on the effect of NH3 on CO oxidation in the absence of NO, and explained based on a detailed chemical kinetic model. The effects of temperature (1023–1223 K), NH3 concentration (250–1500 ppm), and water content (1 %-10 %) on CO oxidation, NH3 conversion, and NO generation were analyzed. In the NH3/CO system, the properties of CO always dominate. As the NH3 content increases, NH3 gradually inhibits the oxidation of CO by seizing free radicals (O, H, OH) and converting into NH2. NH2 further interacts with free radicals to convert into NH or HNO, and ultimately into NO. An increase in temperature will decrease the release of NO and CO and gradually decrease the conversion of NO from NH3. However, ammonia concentration had little effect on the ratio of ammonia conversion to NO. When H2O increases from 1 % to 2 %, it has a significant inhibitory effect on the production of NO and promotes the oxidation of CO. When the water concentration increases from 5 % to 10 %, the inhibitory effect reaches saturation. The present work evaluates the amine subset of the reaction mechanism under the studied conditions and provides experimental data under different NH3/CO ratios, which can be used to construct and verify the reaction mechanism of mixed fuels of carbon-based fuels and ammonia.
期刊介绍:
The exploration of energy sources remains a critical matter of study. For the past nine decades, fuel has consistently held the forefront in primary research efforts within the field of energy science. This area of investigation encompasses a wide range of subjects, with a particular emphasis on emerging concerns like environmental factors and pollution.