Peng Liu, You Zhang, Junjun Guo, Adamu Alfazazi, Carson Chu, Raul Serrano-Bayona, Faruk Aydin, Et-touhami Es-sebbar, Hong G. Im, Bassam Dally, Xiang Gao, William L. Roberts
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In this study, the effects of CO/CH ratio on the profiles of temperature, OH radical, light gas products, large polycyclic aromatic hydrocarbons (PAHs), and soot were investigated for CH-CO-O laminar inverse diffusion flames near ATR conditions, using the combined non-intrusive and intrusive diagnostic methods. Pure O as oxidizer was fed through the central nozzle of the burner surrounded by CH fuel diluted with CO. The experimental results revealed that the formation of soot and PAHs was greatly suppressed with a higher CO/CH ratio. The PAHs and soot loading followed exponential function as CO/CH mole ratio, regardless of pressure, O mole fraction, and burner size. The flame height was found to increase linearly with CO dilution, and the high temperature region (> 1000 K) shifts downstream. The H production decreased with CO/CH ratio, while CO production is less sensitive to CO dilution. The importance of radical species during soot formation is confirmed based on the comprehensive data set. Moreover, five well-known chemical-kinetic mechanisms were evaluated against experimental datasets. The comparisons indicate that the flame temperature and concentration trends of investigated species are well predicted, but future work is needed to improve the prediction accuracy of amplitude and spatial distribution, especially for CH, PAHs and soot. 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引用次数: 0
摘要
甲烷的自热转化(ATR)具有较高的二氧化碳捕集效率(>95%)和成本优势,是一种前景广阔的低碳氢气生产技术。特别是,将 CO+CH 温室气体转化为有价值的 CO+H 气体是碳中和能源系统的可行解决方案。火焰温度、重整气体成分和浓度以及烟尘负荷是决定后续催化剂区 H 生产效率的主要因素。本研究采用非侵入式和侵入式相结合的诊断方法,研究了在 ATR 条件下,CH-CO-O 层流反向扩散火焰中 CO/CH 比率对温度、OH 自由基、轻气体产物、大型多环芳烃 (PAH) 和烟尘的影响。纯 O 作为氧化剂通过燃烧器的中央喷嘴送入,周围是用 CO 稀释的 CH 燃料。实验结果表明,CO/CH 比值越高,烟尘和多环芳烃的形成就越受抑制。多环芳烃和烟尘的负荷随 CO/CH 摩尔比呈指数函数变化,与压力、O 摩尔分数和燃烧器大小无关。火焰高度随着 CO 的稀释而线性增加,高温区(> 1000 K)向下游移动。H 生成量随 CO/CH 比率的增加而减少,而 CO 生成量对 CO 稀释的敏感性较低。基于综合数据集,证实了自由基物种在烟尘形成过程中的重要性。此外,还根据实验数据集评估了五种著名的化学动力学机制。比较结果表明,所研究物种的火焰温度和浓度趋势得到了很好的预测,但还需要进一步提高对振幅和空间分布的预测精度,尤其是对 CH、PAHs 和烟尘的预测精度。所报告的实验和模拟结果可为 ATR 模型的验证、开发、缩减和应用提供有价值的指导。
Characterization of CH4-CO2-O2 diffusion flames near autothermal reforming condition
Autothermal reforming (ATR) of methane is a promising technology for low-carbon H production due to its high CO capture efficiency (>95 %) and cost advantage. Especially, reforming CO+CH greenhouse gases to valuable CO+H gases is a feasible solution for carbon-neutral energy systems. Flame temperature, reforming gas composition and concentration, and soot loading are major factors determining the efficiency of H production in the subsequent catalyst region. In this study, the effects of CO/CH ratio on the profiles of temperature, OH radical, light gas products, large polycyclic aromatic hydrocarbons (PAHs), and soot were investigated for CH-CO-O laminar inverse diffusion flames near ATR conditions, using the combined non-intrusive and intrusive diagnostic methods. Pure O as oxidizer was fed through the central nozzle of the burner surrounded by CH fuel diluted with CO. The experimental results revealed that the formation of soot and PAHs was greatly suppressed with a higher CO/CH ratio. The PAHs and soot loading followed exponential function as CO/CH mole ratio, regardless of pressure, O mole fraction, and burner size. The flame height was found to increase linearly with CO dilution, and the high temperature region (> 1000 K) shifts downstream. The H production decreased with CO/CH ratio, while CO production is less sensitive to CO dilution. The importance of radical species during soot formation is confirmed based on the comprehensive data set. Moreover, five well-known chemical-kinetic mechanisms were evaluated against experimental datasets. The comparisons indicate that the flame temperature and concentration trends of investigated species are well predicted, but future work is needed to improve the prediction accuracy of amplitude and spatial distribution, especially for CH, PAHs and soot. The reported experiment and simulation results can provide valuable guidance for ATR model validation, development, reduction, and application.
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.