Department of Mechanical and Aerospace Engineering, Princeton University, Princeton, New Jersey 08544, USA; email:
Annu Rev Chem Biomol Eng. 2019 Jun 7;10:199-217. doi: 10.1146/annurev-chembioeng-060718-030141. Epub 2019 Mar 22.
This article reviews recent theoretical developments on incipient ignition induced by radical runaway in systems described by detailed chemistry. Employing eigenvalue analysis, we first analyze the canonical explosion limits of mixtures of hydrogen and oxygen, yielding explicit criteria that well reproduce their characteristic Z-shaped response in the pressure-temperature plot. Subsequently, we evaluate the role of hydrogen addition to the explosion limits of mixtures of oxygen with either carbon monoxide or methane, demonstrating and quantifying its strong catalytic effect, especially for the carbon monoxide cases. We then discuss the role of low-temperature chemistry in the autoignition of large hydrocarbon fuels, with emphasis on the first-stage ignition delay and the associated negative-temperature coefficient phenomena. Finally, we extend the analysis to problems of nonhomogeneous ignition in the presence of convective-diffusive transport, using counterflow as an example, demonstrating the canonical similarity between homogeneous and nonhomogeneous systems. We conclude with suggestions for potential directions for future research.
本文综述了详细化学反应体系中自由基失控引发初始点火的最新理论进展。采用特征值分析,我们首先分析了氢氧混合物的典型爆炸极限,得到了明确的判据,很好地再现了它们在压力-温度图中的特征 Z 形响应。随后,我们评估了向一氧化碳或甲烷与氧的混合物中添加氢气对爆炸极限的影响,证明并量化了其对爆炸极限的强烈催化作用,特别是对一氧化碳情况的影响。然后,我们讨论了低温化学在大型碳氢燃料自燃中的作用,重点关注第一阶段点火延迟和相关的负温度系数现象。最后,我们将分析扩展到存在对流-扩散输运的非均相点火问题,以逆流为例,证明了均相和非均相系统之间的典型相似性。最后,我们对未来研究的潜在方向提出了建议。