氧合物
合成气
化学
二氧化碳重整
甲烷
离解(化学)
氧气
催化作用
焦炭
化学工程
有机化学
工程类
作者
Shangkun Li,Jintao Sun,Yury Gorbanev,Kevin van’t Veer,Björn Loenders,Yanhui Yi,Thomas Kenis,Qi Chen,Annemie Bogaerts
出处
期刊:ACS Sustainable Chemistry & Engineering
[American Chemical Society]
日期:2023-10-06
卷期号:11 (42): 15373-15384
被引量:2
标识
DOI:10.1021/acssuschemeng.3c04352
摘要
Plasma-based dry reforming of methane (DRM) into high-value-added oxygenates is an appealing approach to enable otherwise thermodynamically unfavorable chemical reactions at ambient pressure and near room temperature. However, it suffers from coke deposition due to the deep decomposition of CH4. In this work, we assess the DRM performance upon O2 addition, as well as varying temperature, CO2/CH4 ratio, discharge power, and gas residence time, for optimizing oxygenate production. By adding O2, the main products can be shifted from syngas (CO + H2) toward oxygenates. Chemical kinetics modeling shows that the improved oxygenate production is due to the increased concentration of oxygen-containing radicals, e.g., O, OH, and HO2, formed by electron impact dissociation [e + O2 → e + O + O/O(1D)] and subsequent reactions with H atoms. Our study reveals the crucial role of oxygen-coupling in DRM aimed at oxygenates, providing practical solutions to suppress carbon deposition and at the same time enhance the oxygenates production in plasma-assisted DRM.
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