Influence of Soot Particles on the Gas-Phase Methane Conversion into Synthesis Gas: The Role of H2O and CO2 Additives

IF 1.3 4区 化学 Q4 CHEMISTRY, PHYSICAL
A. R. Akhunyanov, P. A. Vlasov, V. N. Smirnov, A. V. Arutyunov, D. I. Mikhailov, V. S. Arutyunov
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Abstract

The influence of the formation of microheterogeneous soot particles on the gas-phase conversion of rich mixtures of methane with oxygen into synthesis gas in a temperature range from 1500 to 1800 K under the conditions of an adiabatic reactor was studied by kinetic modeling. The effect of CO2 and H2O additives on this process was studied. The appearance of soot particles was observed in rich mixtures, starting from the fuel excess factor ϕ = 3.33. At relatively low temperatures of ~1500 K, a small amount of microheterogeneous soot particles was formed, which did not significantly affect other components of the reacting system. A noticeable effect of soot particles at this temperature was observed at a higher value of ϕ = 8.0. This was most clearly manifested in the temperature profile of the process, in which two maximums were observed at times of about 0.01 and 0.1 s upon the addition of water to the reacting mixture. In the case of CO2 additions, the second maximum in the temperature profile was almost not pronounced. A complex temperature profile led to the appearance of the second concentration maximum of hydroxyl radicals OH at times of ~0.1 s. The addition of H2O and CO2 made it possible to vary the H2/CO ratio in the synthesis gas over a wide range, which is necessary for the synthesis of various products. Because the added CO2 under these conditions was actually involved in the chemical process of obtaining synthesis gas, its partial recirculation from the conversion products made it possible to reduce its emission in the production of synthesis gas.

Abstract Image

Abstract Image

煤烟颗粒对气相甲烷转化为合成气的影响:H2O 和 CO2 添加剂的作用
摘要 通过动力学模型研究了在绝热反应器条件下,在 1500 至 1800 K 的温度范围内,微异质烟尘颗粒的形成对甲烷与氧气的富混合物气相转化为合成气的影响。研究了 CO2 和 H2O 添加剂对这一过程的影响。从燃料过剩系数 ϕ = 3.33 开始,在富混合物中观察到烟尘颗粒的出现。在相对较低的温度(约 1500 K)下,形成了少量的微异质烟尘颗粒,但对反应体系中的其他成分没有明显影响。在这个温度下,当 ϕ = 8.0 的值较高时,煤烟颗粒会产生明显的影响。这在反应过程的温度曲线中表现得最为明显,在向反应混合物中加水时,在大约 0.01 秒和 0.1 秒的时间内出现了两个最大值。在加入二氧化碳的情况下,温度曲线上的第二个最大值几乎不明显。复杂的温度曲线导致羟基自由基 OH 的第二个浓度最大值出现在约 0.1 秒时。由于在这些条件下添加的 CO2 实际上参与了获得合成气的化学过程,因此其从转化产物中的部分再循环可以减少其在合成气生产过程中的排放。
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来源期刊
Kinetics and Catalysis
Kinetics and Catalysis 化学-物理化学
CiteScore
2.10
自引率
27.30%
发文量
64
审稿时长
6-12 weeks
期刊介绍: Kinetics and Catalysis Russian is a periodical that publishes theoretical and experimental works on homogeneous and heterogeneous kinetics and catalysis. Other topics include the mechanism and kinetics of noncatalytic processes in gaseous, liquid, and solid phases, quantum chemical calculations in kinetics and catalysis, methods of studying catalytic processes and catalysts, the chemistry of catalysts and adsorbent surfaces, the structure and physicochemical properties of catalysts, preparation and poisoning of catalysts, macrokinetics, and computer simulations in catalysis. The journal also publishes review articles on contemporary problems in kinetics and catalysis. The journal welcomes manuscripts from all countries in the English or Russian language.
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