Experimental and kinetic modeling study of ammonia/dimethoxymethane oxidation in a jet-stirred reactor using SVUV-PIMS

IF 6.2 2区工程技术 Q2 ENERGY & FUELS

Combustion and Flame Pub Date : 2025-10-10 DOI:10.1016/j.combustflame.2025.114525

Tenglong Lv , Yifeng Wang , Xin Zhong , Qiang Xu , Jinyang Zhang , Zhandong Wang , Zunqing Zheng , Hu Wang

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引用次数: 0

Abstract

This study investigates the oxidation characteristics of NH₃/DMM₁ (dimethoxymethane, CH₃OCH₂OCH₃) blended fuels at ND-75(1.5 % NH₃: 0.5 % DMM₁) and ND-50 (1 % NH₃: 1 % DMM₁ (balance O₂/Ar, φ =1)) mixing ratios across a temperature range of 550–1100 K, employing experimental and numerical approaches to elucidate their interaction mechanisms. Experiments were conducted in a jet-stirred reactor (JSR) coupled with synchrotron vacuum ultraviolet photoionization mass spectrometry (SVUV-PIMS), enabling the online detection and quantification of 17 products, including C₀–C₃ small molecules, NH₃, nitrogen oxides, and four rarely reported carbon-nitrogen (C–N) intermediates: HCN, HNCO, CH₃CN, and CH₃NO₂. A detailed kinetic model, comprising 210 species and 1595 elementary reactions, was developed based on experimental data and validated against measured species profiles, demonstrating good predictive accuracy for ignition delay times and intermediate evolution. The results reveal that DMM₁ oxidation generates reactive radicals (e.g., OH, HO₂, CH₃) that enhance NH₃ reactivity, with temperature-dependent shifts in C–N bond formation pathways—favoring CH₃+NO₂=CH₃NO₂ at 870 K and CH₃+NH₂=CH₃NH₂ at 1010 K. These intermediates play a crucial role in shaping the reaction network, providing new insights into the coupled nitrogen-carbon chemistry relevant to low-emission combustion technologies.

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基于SVUV-PIMS的射流搅拌反应器氨/二甲氧基甲烷氧化实验及动力学建模研究

本研究研究了NH₃/DMM₁（二甲氧基甲烷，CH3OCH2OCH3）混合燃料在ND-75（1.5% NH₃：0.5% DMM₁）和ND-50 （1% NH₃：1% DMM₁（平衡O₂/Ar， φ =1））混合比例下在550-1100 K温度范围内的氧化特性，采用实验和数值方法阐明了它们的相互作用机理。实验在喷气搅拌反应器（JSR）和同步加速器真空紫外光电离质谱（SVUV-PIMS）上进行，实现了17种产品的在线检测和定量，包括C₀C₃小分子、NH₃、氮氧化物和四种很少报道的碳氮（C -n）中间体：HCN、HNCO、CH₃CN和CH₃NO₂。基于实验数据，建立了包含210种物质和1595种基本反应的详细动力学模型，并与测量的物质特征进行了验证，证明了点火延迟时间和中间进化的良好预测准确性。结果表明，DMM₁氧化产生反应性自由基（例如OH、HO₂、CH₃），增强了NH₃的反应性，C-N键形成路径的温度依赖变化有利于870 K时CH₃+NO₂=CH₃NO₂，1010 K时CH₃+NH₂=CH₃NH₂。这些中间体在形成反应网络中起着至关重要的作用，为与低排放燃烧技术相关的氮碳耦合化学提供了新的见解。

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来源期刊

Combustion and Flame 工程技术-工程：化工

CiteScore

9.50

自引率

20.50%

发文量

631

审稿时长

3.8 months

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.