Density Functional Theory Study of Synthesis of Oxygenates and Higher Hydrocarbons from Methane and Carbon Dioxide Using Cold Plasmas
Density Functional Theory Study of Synthesis of Oxygenates and Higher Hydrocarbons from Methane and Carbon Dioxide Using Cold Plasmas
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DOI：
10.1021/ef0300949
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发表时间：
2004
期刊：
影响因子：
5.3
通讯作者：
Jian‐guo Wang;Chang-jun Liu;Baldur Eliassion
中科院分区：
文献类型：
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作者：
Jian‐guo Wang;Chang-jun Liu;Baldur Eliassion
采用密度泛函理论（DFT）方法研究了冷等离子体条件下甲烷（CH4）和二氧化碳（CO2）合成含氧化合物和高级烃的反应机理.分析了反应物的主要解离途径。讨论了各种产物，包括合成气、高级烃和含氧化合物的形成的可行性。DFT研究证实，合成的主要障碍是反应物CH 4和CO 2的解离。在冷等离子体已经提供了解离CH4和CO2所需的能量之后，可以容易地产生合成气、高级烃和含氧化合物。本DFT研究还表明，等离子体合成通常会导致形成合成气，高级烃，和含氧化合物的混合物。
A density functional theory (DFT) study has been conducted in this work to investigate the reaction mechanism of synthesis of oxygenates and higher hydrocarbons from methane (CH4) and carbon dioxide (CO2), using cold plasmas. The main dissociation routes of the reactants were analyzed. The feasibility of the formation of various products, including syngas, higher hydrocarbons, and oxygenates, was discussed. The DFT study confirmed that the major obstacle of the synthesis is the dissociation of the reactants CH4 and CO2. After the cold plasma has supplied the necessary energy for the dissociation of CH4 and CO2, syngas, higher hydrocarbons, and oxygenates can be then easily produced. The present DFT study also demonstrates that the plasma synthesis will normally lead to a formation of a mixture of syngas, higher hydrocarbons, and oxygenates.