射流搅拌反应器（JSR）氧化N，N-二甲基甲酰胺（DMF）过程中含氮产物生成的实验与模型研究

IF 5.8 2区工程技术 Q2 ENERGY & FUELS

Combustion and Flame Pub Date : 2025-04-16 DOI:10.1016/j.combustflame.2025.114188

Su Zhang, Fuheng Xia, Meijun Fan, Yixiang Zhang, Guan Wang, Bin Liu, Yongqiang Chen, Yili Zhang, Renhui Ruan, Xuebin Wang

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引用次数: 0

摘要

对N， N-二甲基甲酰胺（DMF）的氧化进行了实验和数值研究。实验在熔融石英喷射搅拌反应器（JSR）中进行，在常压下，温度范围为T = 500-900℃，不同的等效比（φ=0.5、0.7、0.9和1.2）。对主要含氮产物和中间体进行了详细的分析，并用改进的动力学模型解释了结果，描述了DMF的氧化机理和氮转化路径。测量结果表明，DMF氧化的主要含氮产物是HCN、NO和N2O，其中HCN被确定为关键中间体。动力学分析表明，温度升高促进H2CN的分解，促进HCN的生成，而O2水平升高促进OH自由基的生成，促进HCN向NO和N2O的转化。在750°C时，通量分析阐明了NO和N2O的主要转化途径，为优化燃烧和排放控制过程提供了有价值的信息。NO的主要转化途径为燃料- n→CH3N(CH2)CHO→CH3NCH2→CH2NCH2→H2CN→HCN→NCO→HNCO→NH2→H2NO→HNO→NO， N2O的主要转化途径为燃料- n→CH3N(CH2)CHO→CH3NCH2→CH2NCH2→H2CN→HCN→NCO→N2O。研究结果为减少工业应用中的氮基污染物提供了重要意义，为DMF氧化提供了更可持续的方法。

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Experimental and modeling investigation of nitrogen-containing product formation during N,N-dimethylformamide (DMF) oxidation in a jet-stirred reactor (JSR)

The oxidation of N, N-dimethylformamide (DMF) was investigated both experimentally and numerically. Experiments were carried out in a fused silica jet-stirred reactor (JSR) under atmospheric pressure covering a temperature range of T = 500–900 °C with different equivalence ratio (φ=0.5, 0.7, 0.9 and 1.2). A detailed analysis of the main nitrogen-containing products and intermediates was performed, and the results were interpreted with an improved kinetic model, describing the oxidation mechanism of DMF and the nitrogen conversion path. The measurements suggest that the primary nitrogen-containing products of DMF oxidation are HCN, NO, and N₂O, with HCN identified as a key intermediate. Kinetic analysis shows that higher temperatures promote H₂CN decomposition to stimulates the production of HCN, while increased O₂ levels enhance OH radical production, which facilitates the conversion of HCN to NO and N₂O. At 750 °C, flux analysis elucidated the main conversion pathways for NO and N₂O, providing valuable information for optimizing combustion and emissions control processes. The main conversion pathway of NO is Fuel-N→CH₃N(CH₂)CHO→CH₃NCH₂→CH₂NCH₂→H₂CN→HCN→NCO→HNCO→NH₂→H₂NO→HNO→NO, while the main conversion pathway of N₂O is Fuel-N→CH₃N(CH₂)CHO→CH₃NCH₂→CH₂NCH₂→H₂CN→HCN→NCO→N₂O. The findings offer important implications for reducing nitrogen-based pollutants in industrial applications, contributing to a more sustainable approach to DMF oxidation.

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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.