Ning Liu, Bowen Mei, Xingqian Mao, Ziyu Wang, Zijian Sun, Yijie Xu, Zhiyu Shi, Yiguang Ju
{"title":"纳秒脉冲放电中的低温等离子体辅助 NH3/H2 氧化动力学","authors":"Ning Liu, Bowen Mei, Xingqian Mao, Ziyu Wang, Zijian Sun, Yijie Xu, Zhiyu Shi, Yiguang Ju","doi":"10.1016/j.proci.2024.105353","DOIUrl":null,"url":null,"abstract":"Ammonia (NH) has been widely recognized as one of the carbon-neutral fuels. However, ammonia combustion suffers low reactivity and high NO/NO emissions. To overcome these issues, this work reports plasma assisted NH/H oxidation and unveils the kinetics of fuel oxidation and NO/NO formation by combining time-resolved laser diagnostics with plasma modeling. Firstly, we found that the NH consumption is promoted with a H blending ratio of 0.3, due to enhancements of H and OH formation by plasma assisted H dissociation. Secondly, at a high reduced electric field, when the H blending ratio increases, the NH oxidation is promoted due to both the HO formation and strong NO kinetic enhancement via NO-HO and NO-H pathways. In the meantime, it is shown that the NO mole fraction also increases with H blending ratio, because the NO formation is enhanced via N(D)-O pathways, and the DeNO chemistry is weakened with less NH production. By contrast, at a lower reduced electric field, when the H blending ratio increases, the decreased N(D) formation does not produce enough NO to replenish the NO formation drop caused by lower NH concentration. Thirdly, the reduced electric field non-monotonically affects fuel consumption and NO/NO formation by manipulating electron energy deposition pathways. The NH consumption is maximized with an optimal reduced electric field where N* excitation and O dissociation are most efficient. When the reduced electric field deviates from its optimum, the NH consumption decreases due to the discharge energy deposition to either vibrational excitation or dissociation of N. The NO/NO emissions governed by the NH oxidation follow the above NH consumption trend.","PeriodicalId":408,"journal":{"name":"Proceedings of the Combustion Institute","volume":null,"pages":null},"PeriodicalIF":5.3000,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Kinetics of low temperature plasma assisted NH3/H2 oxidation in a nanosecond-pulsed discharge\",\"authors\":\"Ning Liu, Bowen Mei, Xingqian Mao, Ziyu Wang, Zijian Sun, Yijie Xu, Zhiyu Shi, Yiguang Ju\",\"doi\":\"10.1016/j.proci.2024.105353\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Ammonia (NH) has been widely recognized as one of the carbon-neutral fuels. However, ammonia combustion suffers low reactivity and high NO/NO emissions. To overcome these issues, this work reports plasma assisted NH/H oxidation and unveils the kinetics of fuel oxidation and NO/NO formation by combining time-resolved laser diagnostics with plasma modeling. Firstly, we found that the NH consumption is promoted with a H blending ratio of 0.3, due to enhancements of H and OH formation by plasma assisted H dissociation. Secondly, at a high reduced electric field, when the H blending ratio increases, the NH oxidation is promoted due to both the HO formation and strong NO kinetic enhancement via NO-HO and NO-H pathways. In the meantime, it is shown that the NO mole fraction also increases with H blending ratio, because the NO formation is enhanced via N(D)-O pathways, and the DeNO chemistry is weakened with less NH production. By contrast, at a lower reduced electric field, when the H blending ratio increases, the decreased N(D) formation does not produce enough NO to replenish the NO formation drop caused by lower NH concentration. Thirdly, the reduced electric field non-monotonically affects fuel consumption and NO/NO formation by manipulating electron energy deposition pathways. The NH consumption is maximized with an optimal reduced electric field where N* excitation and O dissociation are most efficient. When the reduced electric field deviates from its optimum, the NH consumption decreases due to the discharge energy deposition to either vibrational excitation or dissociation of N. The NO/NO emissions governed by the NH oxidation follow the above NH consumption trend.\",\"PeriodicalId\":408,\"journal\":{\"name\":\"Proceedings of the Combustion Institute\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":5.3000,\"publicationDate\":\"2024-06-27\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Proceedings of the Combustion Institute\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://doi.org/10.1016/j.proci.2024.105353\",\"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":"Proceedings of the Combustion Institute","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.1016/j.proci.2024.105353","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}
引用次数: 0
摘要
氨(NH)已被公认为碳中性燃料之一。然而,氨燃烧存在反应活性低和 NO/NO 排放量高的问题。为了克服这些问题,本研究报告了等离子体辅助 NH/H 氧化,并通过结合时间分辨激光诊断和等离子体建模揭示了燃料氧化和 NO/NO 形成的动力学。首先,我们发现当 H 混合比为 0.3 时,NH 的消耗会增加,这是由于等离子体辅助 H 解离会促进 H 和 OH 的形成。其次,在高还原电场下,当 H 混合比增加时,由于 HO 的形成以及通过 NO-HO 和 NO-H 途径产生的 NO 动力性增强,促进了 NH 的氧化。同时,由于通过 N(D)-O 途径促进了 NO 的形成,并且由于 NH 生成较少,DeNO 化学性质减弱,因此 NO 分子分数也会随着 H 混合比的增加而增加。相反,在较低的还原电场中,当 H 混合比增加时,N(D) 形成的减少并不能产生足够的 NO 来补充 NH 浓度降低导致的 NO 形成下降。第三,降低的电场通过操纵电子能量沉积途径对燃料消耗和 NO/NO 形成产生非单调影响。在 N* 激发和 O 解离效率最高的最佳还原电场中,NH 消耗量最大。当还原电场偏离最佳值时,由于放电能量沉积到 N 的振动激发或解离,NH 消耗量会减少。
Kinetics of low temperature plasma assisted NH3/H2 oxidation in a nanosecond-pulsed discharge
Ammonia (NH) has been widely recognized as one of the carbon-neutral fuels. However, ammonia combustion suffers low reactivity and high NO/NO emissions. To overcome these issues, this work reports plasma assisted NH/H oxidation and unveils the kinetics of fuel oxidation and NO/NO formation by combining time-resolved laser diagnostics with plasma modeling. Firstly, we found that the NH consumption is promoted with a H blending ratio of 0.3, due to enhancements of H and OH formation by plasma assisted H dissociation. Secondly, at a high reduced electric field, when the H blending ratio increases, the NH oxidation is promoted due to both the HO formation and strong NO kinetic enhancement via NO-HO and NO-H pathways. In the meantime, it is shown that the NO mole fraction also increases with H blending ratio, because the NO formation is enhanced via N(D)-O pathways, and the DeNO chemistry is weakened with less NH production. By contrast, at a lower reduced electric field, when the H blending ratio increases, the decreased N(D) formation does not produce enough NO to replenish the NO formation drop caused by lower NH concentration. Thirdly, the reduced electric field non-monotonically affects fuel consumption and NO/NO formation by manipulating electron energy deposition pathways. The NH consumption is maximized with an optimal reduced electric field where N* excitation and O dissociation are most efficient. When the reduced electric field deviates from its optimum, the NH consumption decreases due to the discharge energy deposition to either vibrational excitation or dissociation of N. The NO/NO emissions governed by the NH oxidation follow the above NH consumption trend.
期刊介绍:
The Proceedings of the Combustion Institute contains forefront contributions in fundamentals and applications of combustion science. For more than 50 years, the Combustion Institute has served as the peak international society for dissemination of scientific and technical research in the combustion field. In addition to author submissions, the Proceedings of the Combustion Institute includes the Institute''s prestigious invited strategic and topical reviews that represent indispensable resources for emergent research in the field. All papers are subjected to rigorous peer review.
Research papers and invited topical reviews; Reaction Kinetics; Soot, PAH, and other large molecules; Diagnostics; Laminar Flames; Turbulent Flames; Heterogeneous Combustion; Spray and Droplet Combustion; Detonations, Explosions & Supersonic Combustion; Fire Research; Stationary Combustion Systems; IC Engine and Gas Turbine Combustion; New Technology Concepts
The electronic version of Proceedings of the Combustion Institute contains supplemental material such as reaction mechanisms, illustrating movies, and other data.