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Spatiotemporal imaging of NH2 in plasma-assisted NH3 combustion via nanosecond pulsed discharge 纳秒脉冲放电等离子体辅助NH3燃烧过程中NH2的时空成像
IF 6.2 2区 工程技术 Q2 ENERGY & FUELS Pub Date : 2025-12-30 DOI: 10.1016/j.combustflame.2025.114739
Jinguo Sun , Kailun Zhang , Yupan Bao , Christian Brackmann , Mattias Richter , Alexander A. Konnov , Andreas Ehn
Direct, time-resolved measurements of the amino radical (NH2) are critical for understanding plasma-assisted ammonia (NH3) combustion, in terms of both plasma-accelerated NH3 decomposition and reduced NOx emission, yet such data remain scarce. The current study focuses on the spatiotemporal characteristics of NH2 using laser-induced fluorescence (LIF) in a quasi-one-dimensional NH3/air flame subjected to a pin-to-pin nanosecond pulsed discharge (NPD), and comparatively analyzes the plasma effects in both the unburnt and burnt zones. In the unburnt zone for both lean and rich flames, a considerable amount of NH2 is observed with signal intensities of 3–4 times that in the flame front without plasma, demonstrating the capability of NPD in enhancing NH3 decomposition. The spatial and temporal dynamics of plasma-produced NH2 are explored over timescales ranging from hundreds of nanoseconds to milliseconds following a single NPD pulse. The results indicate that NH2 reaches its peak before 700 ns after the discharge initiation, highlighting the role of plasma kinetics in dissociating NH3 through electrons, excited nitrogen molecules, and O(1D). The generated NH2 subsequently undergoes an exponential decay with a characteristic lifetime of 3–4 μs. This consumption is mainly driven by combustion kinetics, where several diverging pathways are identified as possible reaction routes. Moreover, a “butterfly-like” distribution of plasma-produced NH2, is characterized by lower signals and faster decay in the center, both of which are attributed to the higher temperature within the center of discharge channel. In the burnt zone, NH2 is only detected in the rich flame, and decays much faster (∼1.3 μs) compared to the unburnt zone. The unique experimental data of plasma-produced NH2 provide valuable insights into plasma-assisted NH3 combustion and deliver critical experimental data for the development and refinement of kinetic models.
直接的、时间分辨的氨基自由基(NH2)测量对于了解等离子体辅助氨(NH3)燃烧至关重要,因为等离子体加速了NH3分解和减少了NOx排放,但这类数据仍然很少。本研究利用激光诱导荧光(LIF)技术研究了准一维NH3/空气火焰在引脚对引脚纳秒脉冲放电(NPD)作用下NH2的时空特征,并对比分析了未燃烧区和燃烧区等离子体效应。贫火焰和富火焰的未燃烧区都观察到相当数量的NH2,其信号强度是无等离子体火焰锋面的3-4倍,证明了NPD增强NH3分解的能力。在单个NPD脉冲后,等离子体产生的NH2的时空动态在数百纳秒到毫秒的时间尺度上进行了探索。结果表明,NH2在放电开始后700 ns前达到峰值,突出了等离子体动力学在通过电子、受激氮分子和O解离NH3中的作用(1D)。生成的NH2随后经历指数衰减,特征寿命为3 ~ 4 μs。这种消耗主要是由燃烧动力学驱动的,其中几种不同的途径被确定为可能的反应路线。此外,等离子体产生的NH2呈“蝴蝶状”分布,其特征是信号较低,中心衰减较快,这都归因于放电通道中心温度较高。在燃烧区,NH2只在富火焰中检测到,并且与未燃烧区相比,衰减得快得多(~ 1.3 μs)。等离子体产生NH2的独特实验数据为等离子体辅助NH3燃烧提供了有价值的见解,并为动力学模型的开发和完善提供了关键的实验数据。
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引用次数: 0
Quantifying combustion efficiency in rotating detonation engines using MHz-rate scanned-wavelength-modulation spectroscopy 利用兆赫频率扫描波长调制光谱法量化旋转爆震发动机的燃烧效率
IF 6.2 2区 工程技术 Q2 ENERGY & FUELS Pub Date : 2025-12-29 DOI: 10.1016/j.combustflame.2025.114744
Jose I. Guerrero, Mirko Gamba
This work presents a framework to obtain reference-free combustion efficiency measurements in rotating detonation engines using a chemical balance model and a time-averaged H2O mole fraction. Because a time-resolved pressure measurement was not available, a new post-processing method was developed to estimate a time-averaged H2O mole fraction directly from time-resolved partial pressure measurements. The approach is demonstrated in an RDE with a 50% converging exit nozzle. Temperature and P H2O were measured in-situ at 1 MHz using a single-ended scanned-wavelength-modulation spectroscopy sensor. Results across a range of equivalence ratios (Φ0.55–1.5) and mass flowrates (150–350 g/s) showed combustion efficiencies of 50%–65%, with uncertainties between 14%–16% for most cases. Clear trends were identified between combustion efficiency, equivalence ratio, and wave speed ratios (D/D CJ). This framework enables accurate characterization of energy conversion losses in RDEs and supports future performance optimization.
Novelty and Significance Statement
This work involves the development and application of a novel method for measuring the combustion efficiency of H2-air rotating detonation engines (RDEs) using a chemical balance model and measurable state quantities. The approach is innovative for three reasons: (1) it defines combustion efficiency based on a conserved quantity (mass), allowing the pressure gain combustion community to move beyond proxy definitions, which facilitates integration of measurements with reduced-order models, (2) it eliminates the need for both a reference equilibrium state and a time-resolved pressure measurement when interpreting measured state quantities, and (3) it is applicable across the full operating range of RDEs. In addition, the measurements in this work are the first publicly available combustion efficiency dataset obtained across a range of operating conditions using laser absorption spectroscopy at acquisition rates exceeding 50 kHz. The method and dataset provide a foundation for quantitatively assessing energy conversion processes and performance deficits in detonation-based engines.
这项工作提出了一个框架,以获得无参考燃烧效率测量在旋转爆震发动机使用化学平衡模型和时间平均H2O摩尔分数。由于无法进行时间分辨压力测量,因此开发了一种新的后处理方法,直接从时间分辨分压测量中估计时间平均H2O摩尔分数。该方法在具有50%会聚出口喷嘴的RDE中得到了验证。使用单端扫描波长调制光谱传感器在1 MHz频率下测量温度和ph2o。等效比(Φ≈0.55-1.5)和质量流量(150-350 g/s)范围内的结果表明,燃烧效率为50%-65%,大多数情况下的不确定性在14%-16%之间。燃烧效率、等效比和波速比(D/D CJ)之间存在明显的趋势。该框架能够准确表征rde中的能量转换损失,并支持未来的性能优化。新颖性和意义声明:这项工作涉及开发和应用一种使用化学平衡模型和可测量状态量来测量h2 -空气旋转爆震发动机(RDEs)燃烧效率的新方法。该方法的创新之处在于三个方面:(1)它基于守恒量(质量)定义燃烧效率,允许压力增益燃烧界超越代理定义,这有助于将测量与降阶模型相结合;(2)在解释测量状态量时,它不需要参考平衡状态和时间分辨压力测量;(3)它适用于rde的整个工作范围。此外,这项工作中的测量是第一个公开可用的燃烧效率数据集,使用激光吸收光谱以超过50 kHz的采集速率在一系列操作条件下获得。该方法和数据集为定量评估爆轰发动机的能量转换过程和性能缺陷提供了基础。
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引用次数: 0
Role of reaction rate uncertainties on the dynamics of two-dimensional detonation 反应速率不确定度对二维爆轰动力学的影响
IF 6.2 2区 工程技术 Q2 ENERGY & FUELS Pub Date : 2025-12-29 DOI: 10.1016/j.combustflame.2025.114731
Vigneshwaran Sankar , Xiangrong Huang , Karl P. Chatelain , Rémy Mével , Deanna A. Lacoste
<div><div>This study examines the impact of reaction rate uncertainties by performing a series of two-dimensional simulations of detonation propagating in a weakly unstable mixture 2H<sub>2</sub>+O<sub>2</sub>+3.76Ar at 20 kPa and 295<!--> <!-->K. Several chemical models, namely, FFCM-2, Hong 2011, Mével 2014, and San Diego 2016, were employed, while the experimental targets used for quantifying the impact of uncertainties correspond to the cell width (<span><math><mi>λ</mi></math></span>), its distribution (<span><math><mrow><mn>2</mn><mi>σ</mi><mo>/</mo><mi>λ</mi></mrow></math></span>), the induction zone length (<span><math><msub><mrow><mi>Δ</mi></mrow><mrow><mi>i</mi></mrow></msub></math></span>), and the normalized shock speed (<span><math><mrow><mi>D</mi><mo>/</mo><msub><mrow><mi>D</mi></mrow><mrow><mi>CJ</mi></mrow></msub></mrow></math></span>) dynamics within a cell cycle. Two extreme versions of each model, either maximizing or minimizing <span><math><msub><mrow><mi>Δ</mi></mrow><mrow><mi>i</mi></mrow></msub></math></span>, are created by perturbing the five most sensitive reactions within their (1<span><math><mi>σ</mi></math></span>) uncertainty limit: denoted by <span><math><msub><mrow></mrow><mrow><mo>±</mo><mn>1</mn><mi>σ</mi></mrow></msub></math></span>. Depending on the reaction model, the <span><math><msub><mrow><mi>λ</mi></mrow><mrow><mtext>mean</mtext></mrow></msub></math></span> predictions may be strongly influenced by the initial kinetic model and rate perturbations. The variability of the cell size (<span><math><mrow><mn>2</mn><mi>σ</mi><mo>/</mo><mi>λ</mi></mrow></math></span>) differs by factors of 1.2 to 8 when perturbed reaction models are used, with some models transitioning from a regular to an irregular cellular structure. FFCM-2<span><math><msub><mrow></mrow><mrow><mo>−</mo><mn>1</mn><mi>σ</mi></mrow></msub></math></span> shows the closest agreement with experimental <span><math><msub><mrow><mi>λ</mi></mrow><mrow><mtext>mean</mtext></mrow></msub></math></span> and <span><math><mrow><mn>2</mn><mi>σ</mi><mo>/</mo><mi>λ</mi></mrow></math></span>. While <span><math><msub><mrow><mi>Δ</mi></mrow><mrow><mi>i</mi></mrow></msub></math></span> predictions improve with FFCM-2<span><math><msub><mrow></mrow><mrow><mo>−</mo><mn>1</mn><mi>σ</mi></mrow></msub></math></span>, the slope of <span><math><mrow><msub><mrow><mi>Δ</mi></mrow><mrow><mi>i</mi></mrow></msub><mo>=</mo><mi>f</mi><mrow><mo>(</mo><mi>D</mi><mo>/</mo><msub><mrow><mi>D</mi></mrow><mrow><mi>CJ</mi></mrow></msub><mo>)</mo></mrow></mrow></math></span> remains largely unaffected by reaction rate uncertainty. Similarly, the evolution of <span><math><msub><mrow><mi>Δ</mi></mrow><mrow><mi>i</mi></mrow></msub></math></span> as a function of the relative cell length, or as a function of the distance between consecutive triple points <span><math><mrow><mo>(</mo><msub><mrow><mi>d</mi></mrow><mrow><mtext>TP</mtext></mrow></msub><mo>)</mo></mrow></math></span>, is the closest fo
本研究通过对2H2+O2+3.76Ar弱不稳定混合物在20 kPa和295 K下的爆轰传播进行一系列二维模拟,考察了反应速率不确定性的影响。本文采用了FFCM-2、Hong 2011、m录影带2014和San Diego 2016等化学模型,而用于量化不确定性影响的实验目标分别为细胞宽度(λ)、细胞宽度分布(2σ/λ)、诱导区长度(Δi)和细胞周期内的归一化激波速度(D/DCJ)动态。每个模型的两个极端版本,要么最大化要么最小化Δi,是通过在(1σ)不确定性极限内扰动五个最敏感的反应来创建的:用±1σ表示。根据反应模型的不同,λ均值预测可能受到初始动力学模型和速率扰动的强烈影响。当使用微扰反应模型时,细胞大小的可变性(2σ/λ)相差1.2至8倍,一些模型从规则细胞结构过渡到不规则细胞结构。FFCM-2−1σ与实验λ均值和2σ/λ最接近。虽然使用FFCM-2−1σ可以改善Δi的预测,但Δi=f(D/DCJ)的斜率在很大程度上不受反应速率不确定性的影响。同样,对于FFCM-2−1σ, Δi作为相对细胞长度的函数,或作为连续三点之间的距离(dTP)的函数的演化最接近,但与实验结果仍然存在一些差异。在爆轰模拟中观察到的典型的实验-数值差异不能仅仅归因于反应速率的不确定性。化学模型性能、三维效应、振动非平衡或它们的非线性相互作用中的其他因素也必须对差异负责。未来的爆轰模拟应系统地评估其1σ反应速率不确定性的重要性,因为反应模型对这些不确定性的敏感性不能先验地估计。新颖性和意义声明:本研究利用四种氢氧化动力学模型对二维爆轰模拟中的反应速率不确定性提供了一种新的综合定量评估方法。通过在不确定性(±1σ)范围内系统地干扰最敏感的反应速率,本研究分离了模型选择和速率不确定性对关键爆轰指标(即细胞大小、细胞变异性和诱导区长度动力学)的各自贡献。这项工作的意义在于证明了反应速率的不确定性不能单独解释典型的实验-数值差异。此外,本研究强调需要将±1σ不确定性分析作为未来多维爆炸模拟的标准实践。本文的结论得到了12个二维爆轰模拟的综合分析的支持。
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Several chemical models, namely, FFCM-2, Hong 2011, Mével 2014, and San Diego 2016, were employed, while the experimental targets used for quantifying the impact of uncertainties correspond to the cell width (&lt;span&gt;&lt;math&gt;&lt;mi&gt;λ&lt;/mi&gt;&lt;/math&gt;&lt;/span&gt;), its distribution (&lt;span&gt;&lt;math&gt;&lt;mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;mi&gt;σ&lt;/mi&gt;&lt;mo&gt;/&lt;/mo&gt;&lt;mi&gt;λ&lt;/mi&gt;&lt;/mrow&gt;&lt;/math&gt;&lt;/span&gt;), the induction zone length (&lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;mi&gt;Δ&lt;/mi&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mi&gt;i&lt;/mi&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt;), and the normalized shock speed (&lt;span&gt;&lt;math&gt;&lt;mrow&gt;&lt;mi&gt;D&lt;/mi&gt;&lt;mo&gt;/&lt;/mo&gt;&lt;msub&gt;&lt;mrow&gt;&lt;mi&gt;D&lt;/mi&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mi&gt;CJ&lt;/mi&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/mrow&gt;&lt;/math&gt;&lt;/span&gt;) dynamics within a cell cycle. Two extreme versions of each model, either maximizing or minimizing &lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;mi&gt;Δ&lt;/mi&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mi&gt;i&lt;/mi&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt;, are created by perturbing the five most sensitive reactions within their (1&lt;span&gt;&lt;math&gt;&lt;mi&gt;σ&lt;/mi&gt;&lt;/math&gt;&lt;/span&gt;) uncertainty limit: denoted by &lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mo&gt;±&lt;/mo&gt;&lt;mn&gt;1&lt;/mn&gt;&lt;mi&gt;σ&lt;/mi&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt;. Depending on the reaction model, the &lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;mi&gt;λ&lt;/mi&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mtext&gt;mean&lt;/mtext&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt; predictions may be strongly influenced by the initial kinetic model and rate perturbations. The variability of the cell size (&lt;span&gt;&lt;math&gt;&lt;mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;mi&gt;σ&lt;/mi&gt;&lt;mo&gt;/&lt;/mo&gt;&lt;mi&gt;λ&lt;/mi&gt;&lt;/mrow&gt;&lt;/math&gt;&lt;/span&gt;) differs by factors of 1.2 to 8 when perturbed reaction models are used, with some models transitioning from a regular to an irregular cellular structure. FFCM-2&lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mo&gt;−&lt;/mo&gt;&lt;mn&gt;1&lt;/mn&gt;&lt;mi&gt;σ&lt;/mi&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt; shows the closest agreement with experimental &lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;mi&gt;λ&lt;/mi&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mtext&gt;mean&lt;/mtext&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt; and &lt;span&gt;&lt;math&gt;&lt;mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;mi&gt;σ&lt;/mi&gt;&lt;mo&gt;/&lt;/mo&gt;&lt;mi&gt;λ&lt;/mi&gt;&lt;/mrow&gt;&lt;/math&gt;&lt;/span&gt;. While &lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;mi&gt;Δ&lt;/mi&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mi&gt;i&lt;/mi&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt; predictions improve with FFCM-2&lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mo&gt;−&lt;/mo&gt;&lt;mn&gt;1&lt;/mn&gt;&lt;mi&gt;σ&lt;/mi&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt;, the slope of &lt;span&gt;&lt;math&gt;&lt;mrow&gt;&lt;msub&gt;&lt;mrow&gt;&lt;mi&gt;Δ&lt;/mi&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mi&gt;i&lt;/mi&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;mo&gt;=&lt;/mo&gt;&lt;mi&gt;f&lt;/mi&gt;&lt;mrow&gt;&lt;mo&gt;(&lt;/mo&gt;&lt;mi&gt;D&lt;/mi&gt;&lt;mo&gt;/&lt;/mo&gt;&lt;msub&gt;&lt;mrow&gt;&lt;mi&gt;D&lt;/mi&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mi&gt;CJ&lt;/mi&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;mo&gt;)&lt;/mo&gt;&lt;/mrow&gt;&lt;/mrow&gt;&lt;/math&gt;&lt;/span&gt; remains largely unaffected by reaction rate uncertainty. Similarly, the evolution of &lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;mi&gt;Δ&lt;/mi&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mi&gt;i&lt;/mi&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt; as a function of the relative cell length, or as a function of the distance between consecutive triple points &lt;span&gt;&lt;math&gt;&lt;mrow&gt;&lt;mo&gt;(&lt;/mo&gt;&lt;msub&gt;&lt;mrow&gt;&lt;mi&gt;d&lt;/mi&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mtext&gt;TP&lt;/mtext&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;mo&gt;)&lt;/mo&gt;&lt;/mrow&gt;&lt;/math&gt;&lt;/span&gt;, is the closest fo","PeriodicalId":280,"journal":{"name":"Combustion and Flame","volume":"285 ","pages":"Article 114731"},"PeriodicalIF":6.2,"publicationDate":"2025-12-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145881335","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
An experimental and kinetic modeling study of the autoignition mechanism of 2-ethylhexyl nitrate combustion 硝酸2-乙基己基燃烧自燃机理的实验与动力学模拟研究
IF 6.2 2区 工程技术 Q2 ENERGY & FUELS Pub Date : 2025-12-28 DOI: 10.1016/j.combustflame.2025.114743
Jiaxin Xie , Mengmeng Jia , Frederick Nii Ofei Bruce , Chong-Wen Zhou , Henry Curran , Taufiq Yap Yun Hin , Song Cheng , Ce Sun , Fei Qin , Yang Li
2-Ethylhexyl nitrate (EHN) has attracted attention for its high reactivity, making it a promising candidate for use in propellants and as a combustion-enhancing fuel additive. To gain a fundamental understanding of its combustion behavior and support its practical application in advanced propulsion systems, it is essential to develop an accurate and reliable chemical kinetic model. In this study, ignition delay times (IDTs) of EHN/O₂/N₂ mixtures were systematically measured using a high-pressure shock tube. Experiments were conducted over a temperature range of 900–2000 K, at pressures of 5 and 10 bar, and under equivalence ratios of 0.5 and 1.0. The results clearly demonstrate the characteristic two-stage ignition behavior of EHN. Moreover, the IDTs were found to be highly sensitive to changes in both equivalence ratio and pressure. In the theoretical investigation, the initial decomposition pathways of EHN were systematically explored using high-level quantum chemical calculations at the QCISD(T)/CBS//M06–2X/6–311++G (d,p) level. The results indicate that cleavage of the O–N bond is the dominant reaction channel. A detailed kinetic model for EHN was developed based on the C3MechV3.3 reaction mechanism. The model predictions show good agreement with experimentally measured IDT. Furthermore, based on the current kinetic model, sensitivity, flux, and OH radical rate of production analyses were performed to identify key controlling steps and characterize radical-driven kinetics. The results show that in the first stage of ignition, over 90% of EHN is consumed via O–N bond cleavage, producing the 2-ethylhexoxy radical (EHO) and NO₂, which spontaneously initiate the NO₂–NO catalytic cycle and significantly enhance the system’s initial reactivity. In contrast, during the second stage, the chain-branching reaction H + O₂ → O + OH becomes dominant and serves as the primary driving force behind the rapid acceleration of system reactivity.
2-乙基己基硝酸酯(EHN)因其高活性而备受关注,是一种很有前途的推进剂和增燃燃料添加剂。为了对其燃烧行为有一个基本的了解,并支持其在先进推进系统中的实际应用,建立一个准确可靠的化学动力学模型是必不可少的。采用高压激波管系统测量了EHN/O₂/N₂混合物的点火延迟时间(IDTs)。实验在900-2000 K的温度范围内,在5和10 bar的压力下,在0.5和1.0的当量比下进行。结果表明,EHN具有明显的两级点火特性。此外,发现idt对等效比和压力的变化都高度敏感。在理论研究中,利用QCISD(T)/CBS// M06-2X / 6-311 ++G (d,p)水平的高阶量子化学计算系统地探索了EHN的初始分解途径。结果表明,O-N键的断裂是主要的反应通道。基于C3MechV3.3反应机理,建立了EHN的详细动力学模型。模型预测结果与实测IDT吻合较好。此外,基于现有的动力学模型,进行了灵敏度、通量和OH自由基生成速率分析,以确定关键控制步骤并表征自由基驱动动力学。结果表明:在点火第一阶段,超过90%的EHN通过O-N键裂解被消耗,生成2-乙基己氧基自由基(EHO)和NO₂,自发启动NO₂-NO催化循环,显著提高了体系的初始反应活性;在第二阶段,链支反应H + O₂→O + OH占主导地位,是体系反应性快速加速的主要驱动力。
{"title":"An experimental and kinetic modeling study of the autoignition mechanism of 2-ethylhexyl nitrate combustion","authors":"Jiaxin Xie ,&nbsp;Mengmeng Jia ,&nbsp;Frederick Nii Ofei Bruce ,&nbsp;Chong-Wen Zhou ,&nbsp;Henry Curran ,&nbsp;Taufiq Yap Yun Hin ,&nbsp;Song Cheng ,&nbsp;Ce Sun ,&nbsp;Fei Qin ,&nbsp;Yang Li","doi":"10.1016/j.combustflame.2025.114743","DOIUrl":"10.1016/j.combustflame.2025.114743","url":null,"abstract":"<div><div>2-Ethylhexyl nitrate (EHN) has attracted attention for its high reactivity, making it a promising candidate for use in propellants and as a combustion-enhancing fuel additive. To gain a fundamental understanding of its combustion behavior and support its practical application in advanced propulsion systems, it is essential to develop an accurate and reliable chemical kinetic model. In this study, ignition delay times (IDTs) of EHN/O₂/N₂ mixtures were systematically measured using a high-pressure shock tube. Experiments were conducted over a temperature range of 900–2000 K, at pressures of 5 and 10 bar, and under equivalence ratios of 0.5 and 1.0. The results clearly demonstrate the characteristic two-stage ignition behavior of EHN. Moreover, the IDTs were found to be highly sensitive to changes in both equivalence ratio and pressure. In the theoretical investigation, the initial decomposition pathways of EHN were systematically explored using high-level quantum chemical calculations at the QCISD(T)/CBS//M06–2X/6–311++<em>G</em> (d,p) level. The results indicate that cleavage of the O–N bond is the dominant reaction channel. A detailed kinetic model for EHN was developed based on the C3MechV3.3 reaction mechanism. The model predictions show good agreement with experimentally measured IDT. Furthermore, based on the current kinetic model, sensitivity, flux, and OH radical rate of production analyses were performed to identify key controlling steps and characterize radical-driven kinetics. The results show that in the first stage of ignition, over 90% of EHN is consumed via O–N bond cleavage, producing the 2-ethylhexoxy radical (EHO) and NO₂, which spontaneously initiate the NO₂–NO catalytic cycle and significantly enhance the system’s initial reactivity. In contrast, during the second stage, the chain-branching reaction <em>H</em> + <em>O</em>₂ → <em>O</em> + OH becomes dominant and serves as the primary driving force behind the rapid acceleration of system reactivity.</div></div>","PeriodicalId":280,"journal":{"name":"Combustion and Flame","volume":"285 ","pages":"Article 114743"},"PeriodicalIF":6.2,"publicationDate":"2025-12-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145881340","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Ammonia/hydrogen non-premixed turbulent jet flames stabilized on a hot and diluted co-flow burner 氨/氢非预混湍流射流火焰稳定在热和稀释共流燃烧器
IF 6.2 2区 工程技术 Q2 ENERGY & FUELS Pub Date : 2025-12-27 DOI: 10.1016/j.combustflame.2025.114741
Lele Ren , Adamu Alfazazi , Aurora Maffei , Sonu Kumar , Heinz Pitsch , Bassam Dally
The current study investigates NH3/H2 non-premixed flames stabilized on a Jet-in-Hot-Co-flow (JHC) burner, with a focus on identifying the conditions that enable transition to the MILD regime. Experiments were conducted at a fixed co-flow temperature of 1180 K, with co-flow oxygen concentrations in H2/N2/O2 combustion products ranging from 3 % to 9 % by mass, and hydrogen dilution in the fuel varied between 0 % and 15 % by volume. Flame structure and radical distribution were characterized using simultaneous planar laser-induced fluorescence (PLIF) imaging of NH and OH radicals, in combination with temperature measurements. The results show that a small amount of hydrogen (1 % vol) effectively reduces the local auto-ignition temperature below the co-flow temperature, independent of the oxygen concentration. This implies that minor initial dissociation of ammonia can help in the transition to the MILD combustion regime. At 9 % oxygen concentration, three distinct combustion regimes were observed as hydrogen dilution increases from 0 % to 15%: no visible reaction, a stable visible reaction zone, and a standard turbulent flame. In contrast, such regime transitions were absent at 3 % oxygen, highlighting the essential role of oxidizer reactivity in enabling MILD combustion. Despite meeting the temperature-based criteria for MILD combustion, NO emissions remained relatively high and consistent (∼800 ppm) at 250 mm downstream of the jet across all MILD cases. N2O exhibited strong sensitivity to hydrogen dilution, increasing from 90 ppm to 780 ppm as the hydrogen dilution rose from 3 % to 15 %. These findings highlight the need for revised and more comprehensive criteria to define MILD combustion in NH₃-fueled environments.
目前的研究调查了在热共流射流(JHC)燃烧器上稳定的NH3/H2非预混火焰,重点是确定能够过渡到MILD状态的条件。实验在固定共流温度1180 K下进行,H2/N2/O2燃烧产物中共流氧浓度按质量计为3% ~ 9%,燃料中氢的稀释率按体积计为0% ~ 15%。结合温度测量,利用平面激光诱导荧光(PLIF)同时成像NH和OH自由基,对火焰结构和自由基分布进行了表征。结果表明,少量氢(1% vol)能有效降低局部自燃温度,使其低于共流温度,与氧浓度无关。这意味着氨的轻微初始解离有助于过渡到轻度燃烧状态。在9%的氧浓度下,当氢稀释度从0%增加到15%时,观察到三种不同的燃烧状态:无可见反应,稳定的可见反应区和标准湍流火焰。相比之下,在3%的氧气条件下,这种状态转变是不存在的,这突出了氧化剂反应性在轻度燃烧中的重要作用。尽管符合轻度燃烧的温度标准,但在所有轻度燃烧情况下,喷气机下游250毫米处的NO排放仍然相对较高且一致(~ 800 ppm)。N2O对氢稀释表现出很强的敏感性,当氢稀释度从3%增加到15%时,N2O从90 ppm增加到780 ppm。这些发现强调了需要修订和更全面的标准来定义NH₃燃料环境中的轻度燃烧。
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引用次数: 0
Pressure dependence of synergistic soot formation in ethylene/propane co-flow diffusion flames 乙烯/丙烷共流扩散火焰中协同烟灰形成的压力依赖性
IF 6.2 2区 工程技术 Q2 ENERGY & FUELS Pub Date : 2025-12-27 DOI: 10.1016/j.combustflame.2025.114755
Aryan Nobakht, Ahmet E. Karataş
This study investigates the influence of pressure on synergistic soot formation in co-flow laminar diffusion flames of ethylene/propane mixtures (1–6 atm). Radially resolved fields of soot volume fraction, temperature, and the soot absorption function, E(m), were obtained using three-color line-of-sight attenuation and spectral soot emission techniques. Synergistic promotion of soot formation was observed at all pressures, but its strength varied with pressure: at 1 atm, the peak soot volume fraction increased from 1.24 ppm in neat ethylene to 1.52 ppm with 5% carbon from propane, whereas at 6 atm it increased only marginally from 86.4 ppm to 90.3 ppm. Normalized soot yield revealed the strongest nonlinearity at 2 atm, followed by 3 atm, then 1 atm, 4 atm, 5 atm, and 6 atm. Temperatures for different mixtures at a given pressure were similar and primarily controlled by soot loading and associated radiative losses. The measurements show that E(m) varies both spectrally and spatially; values are notably lower than the commonly assumed 0.26 in nascent soot regions near the flame base and higher elsewhere. This variation demonstrates that a constant E(m) can misestimate soot volume fraction depending on location and wavelength. Despite substantial differences in soot concentration among mixtures, soot maturity distributions were broadly similar. These results provide high-fidelity data for model validation and emphasize the need to account for wavelength-dependent optical properties when quantifying soot at elevated pressures.
Novelty and significance statement
This study provides the first multi-parameter characterization of synergistic soot formation in ethylene/propane diffusion flames at elevated pressures. By introducing a wavelength-dependent absorption function, E(m), it captures spatial variation in soot maturity and improves quantification. The results demonstrate persistent synergistic effects across pressures and yield novel mechanistic insights, including rate-limiting steps, with direct relevance to predictive soot models for high-pressure combustion systems using blended fuels.
本文研究了压力对乙烯/丙烷共流层流扩散火焰(1 - 6atm)中协同烟灰形成的影响。利用三色视距衰减和光谱烟尘发射技术,获得了烟尘体积分数、温度和烟尘吸收函数E(m)的径向分解场。在所有压力下均观察到协同促进烟灰的形成,但其强度随压力而变化:在1atm时,烟灰体积分数峰值从纯乙烯的1.24 ppm增加到5%丙烷碳的1.52 ppm,而在6atm时,它仅从86.4 ppm略微增加到90.3 ppm。归一化烟灰产率在2 atm时非线性最强,3 atm次之,然后是1 atm、4 atm、5 atm和6 atm。在给定压力下,不同混合物的温度是相似的,并且主要由烟尘负荷和相关的辐射损失控制。测量结果表明,E(m)在光谱和空间上都有变化;在靠近火焰底部的新生烟尘区域,数值明显低于通常假设的0.26,而在其他地方则更高。这种变化表明,恒定的E(m)可能会根据位置和波长错误地估计烟灰体积分数。尽管不同混合物的烟灰浓度存在很大差异,但烟灰成熟度分布大致相似。这些结果为模型验证提供了高保真度的数据,并强调了在量化高压下煤烟时需要考虑波长相关的光学特性。本研究首次提供了高压下乙烯/丙烷扩散火焰中协同烟灰形成的多参数表征。通过引入波长相关的吸收函数E(m),该方法捕获了煤烟成熟度的空间变化,提高了量化。结果表明,跨压力的持续协同效应,并产生了新的机制见解,包括限速步骤,与使用混合燃料的高压燃烧系统的预测烟灰模型直接相关。
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引用次数: 0
Flue gas to mitigate explosions: The diluting effect and mechanism of inert gases on hydrogen explosion in confined space 缓解爆炸的烟气:惰性气体对密闭空间氢气爆炸的稀释作用和机理
IF 6.2 2区 工程技术 Q2 ENERGY & FUELS Pub Date : 2025-12-27 DOI: 10.1016/j.combustflame.2025.114736
Xinyu Ma , Baisheng Nie , Weili Wang , Yushu Zhang , Dan Zhao , Li Chang , Xianfeng Liu
The efficient utilization of flue gas has strategic value in alleviating environmental pressure and promoting sustainable development. This study investigated the explosion characteristics of hydrogen under inert conditions and analyzed the difference in inerting effects between single gas dilution (CO₂, N₂) and multi-component synergistic control (flue gas)using a 20 L spherical explosion test system. The Chemkin simulation software was applied to reveal the microscopic reaction mechanism of different inert gases in hydrogen explosions. The findings indicate that the addition of inert gases lowers the flame temperature of hydrogen explosion and thus the Pmax, (dP/dt)max and KG, while tb and tc raise parabolically. The critical inhibition concentrations of the three diluents are 50 % flue gas, 40 % N2 and 30 % CO2. For a given dilution ratio, the KG of N2 and flue gas in suppressing hydrogen explosion are higher than those for CO2. The explosion suppression effect of flue gas is not a linear superposition of single CO2 and N2. The different heat capacities of the inert gases and the regulation mechanism on the chain reactions fundamentally determine the severity of hydrogen explosion. Sensitivity analysis reveals that free radicals are primarily sensitive to the intermediate reaction R26 (forward direction) and R15 (reverse direction). The research results provide a scientific basis for improving disaster prevention systems and developing efficient explosion suppressants.
烟气的高效利用对缓解环境压力、促进可持续发展具有战略价值。本研究利用20 L球形爆炸试验系统,研究了氢气在惰性条件下的爆炸特性,分析了单一气体稀释(CO₂、N₂)与多组分协同控制(烟气)的惰性效果差异。利用Chemkin模拟软件揭示了不同惰性气体在氢气爆炸中的微观反应机理。结果表明:惰性气体的加入降低了氢爆炸火焰温度,从而降低了Pmax、(dP/dt)max和KG,而tb和tc呈抛物线上升。三种稀释剂的临界抑制浓度分别为50%烟气、40% N2和30% CO2。在一定稀释比下,N2和烟气抑制氢气爆炸的KG均高于CO2。烟气的抑爆效果不是单一CO2和N2的线性叠加。惰性气体的不同热容和对链式反应的调控机理从根本上决定了氢气爆炸的严重程度。敏感性分析表明,自由基主要对中间反应R26(正向)和R15(反向)敏感。研究结果为完善防灾系统、开发高效防爆药剂提供了科学依据。
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引用次数: 0
Study on powder–gas “hybrid” combustion: Its mechanism to achieve variable burning velocities 粉末-气体“混合”燃烧的研究:实现变燃烧速度的机理
IF 6.2 2区 工程技术 Q2 ENERGY & FUELS Pub Date : 2025-12-27 DOI: 10.1016/j.combustflame.2025.114730
Yuyang Jiang, Ryoki Okada, Akito Tayama, Daiki Matsugi, Yuji Nakamura
This study investigates a low-carbon combustion method based on powder-gas “hybrid” flames, in which ultra-lean methane–air mixtures are assisted by biomass powder (Lycopodium spores) to achieve continuous “weak explosions”. This approach offers a solution to achieving stable combustion of low-calorific gaseous fuels with a small amount of combustible powder. In this hybrid fuel, both the powder concentration and the gas-phase equivalence ratio are below their respective flammability limits. A stagnation-point flame was employed, and the burning velocity was determined from particle image velocimetry (PIV) measurements. The results showed that an increase in powder loading rate leads to an increase in burning velocity. A qualitative analysis was conducted to assess the mechanisms controlling the burning velocity; namely, effects of pyrolysis-induced increases in the equivalence ratio and flame surface area, as well as the influence of radiative preheating on the burning velocity. This work offers a new pathway for the combustion of low-calorific gaseous fuels and biomass-based wastes, contributing to carbon neutrality through the utilization of renewable solid fuels. It may represent a promising direction for future developments in sustainable combustion technologies.
本研究研究了一种基于粉末-气体“混合”火焰的低碳燃烧方法,其中超稀薄甲烷-空气混合物在生物质粉末(石松孢子)的辅助下实现连续“弱爆炸”。这种方法提供了一种用少量可燃粉末实现低热量气体燃料稳定燃烧的解决方案。在该混合燃料中,粉末浓度和气相当量比均低于各自的可燃性极限。采用静止点火焰,用粒子图像测速法测定燃烧速度。结果表明,装粉率的增加导致燃烧速度的增加。定性分析了控制燃烧速度的机理;即热解引起的等效比和火焰表面积增加的影响,以及辐射预热对燃烧速度的影响。这项工作为低热量气体燃料和生物质废物的燃烧提供了一条新的途径,通过利用可再生固体燃料为碳中和做出贡献。它可能代表了可持续燃烧技术未来发展的一个有希望的方向。
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引用次数: 0
Effects of steam dilution on flame characteristics and vortex field mechanisms in normal and inverse diffusion Hydrogen-Oxygen flames 水蒸气稀释对正扩散和逆扩散氢氧火焰火焰特性的影响及涡场机制
IF 6.2 2区 工程技术 Q2 ENERGY & FUELS Pub Date : 2025-12-26 DOI: 10.1016/j.combustflame.2025.114722
Jinqi Zhu, Xiaopeng Jiang, Yu Zhang, Wenda Zhang, Penghua Qiu, Yijun Zhao
Steam-diluted hydrogen-oxygen combustion is a key technology for future hydrogen utilization. Steam dilution significantly affects heat release and mixing, altering flame characteristics. Normal diffusion flames (NDFs) and inverse diffusion flames (IDFs) in coaxial jets exhibit distinct flame evolution patterns under steam influence. To elucidate the coupling between combustion mode and steam dilution, this study combines experiments and numerical simulations to clarify the distinct mechanisms of steam dilution on NDFs and IDFs. Static characterization shows that steam dilution significantly alters the unfiltered broadband flame emission structure and OH* distribution near the flame root in NDFs. When the steam dilution exceeds 40 %, the emission peak shifts downstream, while the spatial distribution in IDFs remains stable. Dynamic analysis demonstrates that steam dilution intensifies transient flame front wrinkling and shortens the OH* oscillation period in NDFs. In contrast, IDFs dynamics are less sensitive to dilution, with minimal disruption to the transient flame front structure. Multiphysics analysis of combustion reveals that near-field vortex evolution in NDFs is governed by viscous diffusion, vortex stretching and tilting, volume expansion, and baroclinic torque, with viscous diffusion dominating downstream. In IDFs, viscous diffusion controls near-field dynamics, while vortex stretching and tilting, volume expansion, and viscous diffusion jointly influence the downstream region. Steam dilution enhances the misalignment between density and pressure gradients within the flame, thereby amplifying the baroclinic torque effect in NDFs. Conversely, the baroclinic torque mechanism is negligible in IDFs.
蒸汽稀释氢氧燃烧是未来氢利用的关键技术。蒸汽稀释显著影响热量释放和混合,改变火焰特性。同轴射流中正扩散火焰(ndf)和逆扩散火焰(IDFs)在蒸汽作用下表现出不同的火焰演化模式。为了阐明燃烧方式与蒸汽稀释之间的耦合关系,本研究将实验与数值模拟相结合,阐明蒸汽稀释对ndf和IDFs的不同机理。静态表征表明,蒸汽稀释显著改变了ndf中未过滤的宽带火焰发射结构和火焰根部附近OH*的分布。当蒸汽稀释度超过40%时,排放峰向下游移动,而idf的空间分布保持稳定。动力学分析表明,蒸汽稀释加剧了瞬态火焰锋面起皱,缩短了ndf中的OH*振荡周期。相比之下,idf动力学对稀释不太敏感,对瞬态火焰前缘结构的破坏最小。燃烧多物理场分析表明,ndf内近场涡演化主要受粘性扩散、涡旋拉伸和倾斜、体积膨胀和斜压转矩控制,以粘性扩散为主。在idf中,粘性扩散控制着近场动力学,而旋涡拉伸和倾斜、体积膨胀和粘性扩散共同影响下游区域。蒸汽稀释增强了火焰内密度梯度和压力梯度之间的不对准,从而放大了ndf中的斜压扭矩效应。相反,斜压转矩机制在idf中可以忽略不计。
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引用次数: 0
Three- versus two-dimensional numerical simulation of distorted tulip flame in stoichiometric hydrogen-air mixture 化学计量氢-空气混合物中扭曲郁金香火焰的三维与二维数值模拟
IF 6.2 2区 工程技术 Q2 ENERGY & FUELS Pub Date : 2025-12-26 DOI: 10.1016/j.combustflame.2025.114733
Jumeng Fan , Xiangyu Zhang , Huahua Xiao , Longhua Hu , Luqing Wang , Honghao Ma , Xinming Qin , Yundong Zhang , Chao Wu
Numerical simulation of the formation and evolution of distorted tulip flame (DTF) requires solving the three-dimensional (3D), fully-compressible, and reactive Navier-Stokes equations using a high-order numerical method and adaptive mesh refinement. In this work, a dynamically thickened flame model coupled with a chemical-diffusive model was employed to achieve efficient and accurate resolution of 3D DTF structures. Validation against prior experiments, theories, and simulations confirms the numerical method’s reliability. The 3D results reveal noteworthy differences from two-dimensional (2D) simulations in flame evolution and pressure dynamics. A key observation in 3D simulation is the progressive shallowing of the primary central cusp without collapse, contrasting with the collapse-regeneration cycles observed in 2D During exponential flame acceleration, the acceleration rate is proportional to the ratio of flame surface area to the burned volume, leading to higher propagation speed and reduced distortion frequency. While both 2D and 3D models predict the same peak pressure, the 2D case underestimates the pressure growth rate due to slower flame acceleration. Linear Rayleigh-Taylor instability (RTI) analysis indicates that the larger RTI growth rate and time-scale in 3D leads to greater flame distortions and deeper cusps, and consequently larger flame surface area that causes higher flame speed and pressure growth rate in the later stage.
变形郁金香火焰(DTF)的形成和演化的数值模拟需要使用高阶数值方法和自适应网格细化来求解三维(3D)、完全可压缩和反应性的Navier-Stokes方程。本文采用动态增厚火焰模型与化学扩散模型相结合的方法,实现了三维DTF结构的高效精确分辨率。通过先前的实验、理论和仿真验证了数值方法的可靠性。三维结果显示,在火焰演化和压力动力学方面与二维(2D)模拟有显著差异。在三维模拟中,一个关键的观察结果是初级中心尖头逐渐变浅而不坍塌,与二维中观察到的坍塌-再生周期形成对比。在指数火焰加速过程中,加速度与火焰表面积与燃烧体积的比例成正比,从而导致更高的传播速度和更低的失真频率。虽然2D和3D模型预测的峰值压力相同,但由于火焰加速度较慢,2D模型低估了压力增长率。线性瑞利-泰勒不稳定性(RTI)分析表明,越大的RTI生长速率和时间尺度在三维空间中导致越大的火焰畸变和更深的尖点,从而导致越大的火焰表面积,导致后期火焰速度和压力增长速率越高。
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引用次数: 0
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