CO2/CH4辉光放电等离子体。第二部分:等离子体催化氧化铈相互作用机理的研究

IF 2.6 3区 物理与天体物理 Q3 ENGINEERING, CHEMICAL Plasma Chemistry and Plasma Processing Pub Date : 2023-11-17 DOI:10.1007/s11090-023-10419-7
Carolina A. Garcia-Soto, Edmond Baratte, Tiago Silva, Vasco Guerra, Vasile I. Parvulescu, Olivier Guaitella
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引用次数: 0

摘要

为了研究表面等离子体与氧化铈(\(\hbox {CeO}_2\))作为催化表面的相互作用,对\(\hbox {CO}_2\)和\(\hbox {CO}_2\) - \(\hbox {CH}_4\)等离子体进行了原位红外透射实验。利用直流辉光放电等离子体反应器,在低压下观察到\(\hbox {CO}_2\)气体在表面吸附形成三齿碳酸盐和碳酸盐。当\(\hbox {CO}_2\) - \(\hbox {CH}_4\)等离子体被点燃时,甲酸类物质形成,而碳酸盐类物质从表面消失。\(\hbox {CeO}_2\)颗粒也被放置在等离子体的下游,以便在\(\hbox {CeO}_2\)上没有任何加热或强电场的情况下观察\(\hbox {CO}_2\) - \(\hbox {CH}_4\)等离子体出口处气体成分的作用。此外,还研究了水对几种表面现象的影响。氢氧基在等离子体下与三叉戟碳酸盐生成甲酸酯的反应中起着重要作用。这里使用的\(\hbox {CO}_2\) - \(\hbox {CH}_4\)等离子体的气相化学已在本工作的第一部分中详细描述。关于气相的结论有助于理解\(\hbox {CeO}_2\)上观察到的现象。这些结果揭示了在\(\hbox {CO}_2\) - \(\hbox {CH}_4\)表面等离子体反应过程中发生的复杂机制,有助于改善\(\hbox {CO}_2\)的回收利用。
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CO2/CH4 Glow Discharge Plasma. Part II: Study of Plasma Catalysis Interaction Mechanisms on CeO2

In situ FTIR transmission experiments for \(\hbox {CO}_2\) and \(\hbox {CO}_2\)\(\hbox {CH}_4\) plasma were performed for a fundamental study of surface plasma interaction with cerium oxide (\(\hbox {CeO}_2\)) as catalytic surface. Utilizing a DC glow discharge plasma reactor at low pressure, it was observed that \(\hbox {CO}_2\) gas adsorbs in the surface forming tridentate carbonates and hydrogen carbonates. When \(\hbox {CO}_2\)\(\hbox {CH}_4\) plasma is ignited, formate species were formed while carbonate species disappeared from the surface. The \(\hbox {CeO}_2\) pellet has also been placed downstream the plasma in order to observe the role of the gas composition at the exit of \(\hbox {CO}_2\)\(\hbox {CH}_4\) plasma on \(\hbox {CeO}_2\) without any heating or strong electric field. In addition, the effect of water was investigated in several surface phenomena. OH groups play an important role in the reaction with tridentate carbonates to generate formates under plasma. The gas phase chemistry of the \(\hbox {CO}_2\)\(\hbox {CH}_4\) plasma used here has been described in details in the part I of this work. The conclusions drawn on the gas phase contribute to the understanding of the observed phenomena on \(\hbox {CeO}_2\). These results enlighten the complex mechanisms occurring during \(\hbox {CO}_2\)\(\hbox {CH}_4\) plasma reactions on surfaces that could help in the improvement of \(\hbox {CO}_2\) recycling.

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来源期刊
Plasma Chemistry and Plasma Processing
Plasma Chemistry and Plasma Processing 工程技术-工程:化工
CiteScore
5.90
自引率
8.30%
发文量
73
审稿时长
6-12 weeks
期刊介绍: Publishing original papers on fundamental and applied research in plasma chemistry and plasma processing, the scope of this journal includes processing plasmas ranging from non-thermal plasmas to thermal plasmas, and fundamental plasma studies as well as studies of specific plasma applications. Such applications include but are not limited to plasma catalysis, environmental processing including treatment of liquids and gases, biological applications of plasmas including plasma medicine and agriculture, surface modification and deposition, powder and nanostructure synthesis, energy applications including plasma combustion and reforming, resource recovery, coupling of plasmas and electrochemistry, and plasma etching. Studies of chemical kinetics in plasmas, and the interactions of plasmas with surfaces are also solicited. It is essential that submissions include substantial consideration of the role of the plasma, for example, the relevant plasma chemistry, plasma physics or plasma–surface interactions; manuscripts that consider solely the properties of materials or substances processed using a plasma are not within the journal’s scope.
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