{"title":"无氧条件下NH3/NO和NH3/N2O混合物层流火焰及化学动力学分析","authors":"Biao Liu, Zunhua Zhang, Mengni Zhou, Gesheng Li","doi":"10.1016/j.combustflame.2025.114341","DOIUrl":null,"url":null,"abstract":"<div><div>Ammonia, as a zero-carbon fuel, has attracted significant attention. However, its combustion can lead to the emission of nitrogen oxides. While ammonia can reduce nitrogen oxides, the mechanism by which ammonia interacts with N<em><sub>i</sub></em>O (<em>i</em> = 1 and 2) remains unclear. In this study, the laminar burning velocities (LBVs) of NH<sub>3</sub>/N<em><sub>i</sub></em>O/N<sub>2</sub> (Ar) mixtures were measured using a high-pressure constant volume combustion platform. The predictive performances of 16 ammonia chemical kinetic mechanisms were assessed by calculating the mean relative errors (MREs) against experimental data. Additionally, the chemical kinetic interactions between NH<sub>3</sub> and N<em><sub>i</sub></em>O in the flames were analyzed. The results show that the LBVs of NH<sub>3</sub>/NO/N<sub>2</sub> mixtures initially increase and then decrease as the equivalence ratio rises from 1.1 to 1.9, peaking near 1.4. Similarly, the LBVs of NH<sub>3</sub>/N<sub>2</sub>O/N<sub>2</sub> mixtures initially increase and then decrease as the equivalence ratio rises from 0.7 to 1.5, peaking around 1.05. With an increasing N<em><sub>i</sub></em>O mixture ratio, the LBVs of the NH<sub>3</sub>/N<em><sub>i</sub></em>O/N<sub>2</sub> mixtures increase linearly. The LBVs of the NH<sub>3</sub>/N<em><sub>i</sub></em>O/N<sub>2</sub> mixtures increase with higher initial temperatures and decrease with higher initial pressures. Among the 16 mechanisms, those that accurately predict the LBVs of NH<sub>3</sub>/N<sub>2</sub>O/N<sub>2</sub> (Ar) mixtures may show significant MREs in predicting the LBVs of NH<sub>3</sub>/NO/N<sub>2</sub> (Ar) mixtures. In NH<sub>3</sub>/NO flames, NO directly reacts with key intermediates (ṄH<sub>2</sub> and <span><math><mrow><mover><mi>N</mi><mo>¨</mo></mover><mi>H</mi></mrow></math></span>) in NH<sub>3</sub> decomposition process. This indicates that NH<sub>3</sub> has strong selectivity for reactions with NO. In NH<sub>3</sub>/N<sub>2</sub>O flames, the Ö radical generated from the self-decomposition of N<sub>2</sub>O, along with the reaction between N<sub>2</sub>O and Ḣ radical to produce ȮH radical, further enhance the reactivity of NH<sub>3</sub> combustion system. The reduction of N<sub>2</sub>O by NH<sub>3</sub> exhibits relatively low selectivity.</div></div>","PeriodicalId":280,"journal":{"name":"Combustion and Flame","volume":"279 ","pages":"Article 114341"},"PeriodicalIF":5.8000,"publicationDate":"2025-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Laminar flames and chemical kinetics analysis of NH3/NO and NH3/N2O mixtures in the absence of oxygen\",\"authors\":\"Biao Liu, Zunhua Zhang, Mengni Zhou, Gesheng Li\",\"doi\":\"10.1016/j.combustflame.2025.114341\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Ammonia, as a zero-carbon fuel, has attracted significant attention. However, its combustion can lead to the emission of nitrogen oxides. While ammonia can reduce nitrogen oxides, the mechanism by which ammonia interacts with N<em><sub>i</sub></em>O (<em>i</em> = 1 and 2) remains unclear. In this study, the laminar burning velocities (LBVs) of NH<sub>3</sub>/N<em><sub>i</sub></em>O/N<sub>2</sub> (Ar) mixtures were measured using a high-pressure constant volume combustion platform. The predictive performances of 16 ammonia chemical kinetic mechanisms were assessed by calculating the mean relative errors (MREs) against experimental data. Additionally, the chemical kinetic interactions between NH<sub>3</sub> and N<em><sub>i</sub></em>O in the flames were analyzed. The results show that the LBVs of NH<sub>3</sub>/NO/N<sub>2</sub> mixtures initially increase and then decrease as the equivalence ratio rises from 1.1 to 1.9, peaking near 1.4. Similarly, the LBVs of NH<sub>3</sub>/N<sub>2</sub>O/N<sub>2</sub> mixtures initially increase and then decrease as the equivalence ratio rises from 0.7 to 1.5, peaking around 1.05. With an increasing N<em><sub>i</sub></em>O mixture ratio, the LBVs of the NH<sub>3</sub>/N<em><sub>i</sub></em>O/N<sub>2</sub> mixtures increase linearly. The LBVs of the NH<sub>3</sub>/N<em><sub>i</sub></em>O/N<sub>2</sub> mixtures increase with higher initial temperatures and decrease with higher initial pressures. Among the 16 mechanisms, those that accurately predict the LBVs of NH<sub>3</sub>/N<sub>2</sub>O/N<sub>2</sub> (Ar) mixtures may show significant MREs in predicting the LBVs of NH<sub>3</sub>/NO/N<sub>2</sub> (Ar) mixtures. In NH<sub>3</sub>/NO flames, NO directly reacts with key intermediates (ṄH<sub>2</sub> and <span><math><mrow><mover><mi>N</mi><mo>¨</mo></mover><mi>H</mi></mrow></math></span>) in NH<sub>3</sub> decomposition process. This indicates that NH<sub>3</sub> has strong selectivity for reactions with NO. In NH<sub>3</sub>/N<sub>2</sub>O flames, the Ö radical generated from the self-decomposition of N<sub>2</sub>O, along with the reaction between N<sub>2</sub>O and Ḣ radical to produce ȮH radical, further enhance the reactivity of NH<sub>3</sub> combustion system. The reduction of N<sub>2</sub>O by NH<sub>3</sub> exhibits relatively low selectivity.</div></div>\",\"PeriodicalId\":280,\"journal\":{\"name\":\"Combustion and Flame\",\"volume\":\"279 \",\"pages\":\"Article 114341\"},\"PeriodicalIF\":5.8000,\"publicationDate\":\"2025-07-10\",\"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/S0010218025003785\",\"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/S0010218025003785","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}
Laminar flames and chemical kinetics analysis of NH3/NO and NH3/N2O mixtures in the absence of oxygen
Ammonia, as a zero-carbon fuel, has attracted significant attention. However, its combustion can lead to the emission of nitrogen oxides. While ammonia can reduce nitrogen oxides, the mechanism by which ammonia interacts with NiO (i = 1 and 2) remains unclear. In this study, the laminar burning velocities (LBVs) of NH3/NiO/N2 (Ar) mixtures were measured using a high-pressure constant volume combustion platform. The predictive performances of 16 ammonia chemical kinetic mechanisms were assessed by calculating the mean relative errors (MREs) against experimental data. Additionally, the chemical kinetic interactions between NH3 and NiO in the flames were analyzed. The results show that the LBVs of NH3/NO/N2 mixtures initially increase and then decrease as the equivalence ratio rises from 1.1 to 1.9, peaking near 1.4. Similarly, the LBVs of NH3/N2O/N2 mixtures initially increase and then decrease as the equivalence ratio rises from 0.7 to 1.5, peaking around 1.05. With an increasing NiO mixture ratio, the LBVs of the NH3/NiO/N2 mixtures increase linearly. The LBVs of the NH3/NiO/N2 mixtures increase with higher initial temperatures and decrease with higher initial pressures. Among the 16 mechanisms, those that accurately predict the LBVs of NH3/N2O/N2 (Ar) mixtures may show significant MREs in predicting the LBVs of NH3/NO/N2 (Ar) mixtures. In NH3/NO flames, NO directly reacts with key intermediates (ṄH2 and ) in NH3 decomposition process. This indicates that NH3 has strong selectivity for reactions with NO. In NH3/N2O flames, the Ö radical generated from the self-decomposition of N2O, along with the reaction between N2O and Ḣ radical to produce ȮH radical, further enhance the reactivity of NH3 combustion system. The reduction of N2O by NH3 exhibits relatively low selectivity.
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:
Development and validation of reaction kinetics, reduction of reaction mechanisms and modeling of combustion systems, including:
Conventional, alternative and surrogate fuels;
Pollutants;
Particulate and aerosol formation and abatement;
Heterogeneous processes.
Experimental, theoretical, and computational studies of laminar and turbulent combustion phenomena, including:
Premixed and non-premixed flames;
Ignition and extinction phenomena;
Flame propagation;
Flame structure;
Instabilities and swirl;
Flame spread;
Multi-phase reactants.
Advances in diagnostic and computational methods in combustion, including:
Measurement and simulation of scalar and vector properties;
Novel techniques;
State-of-the art applications.
Fundamental investigations of combustion technologies and systems, including:
Internal combustion engines;
Gas turbines;
Small- and large-scale stationary combustion and power generation;
Catalytic combustion;
Combustion synthesis;
Combustion under extreme conditions;
New concepts.