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Influence of ionic conductivity and dielectric constant of the catalyst on DBD plasma-assisted CO2 hydrogenation into methanol
Journal of Physics D: Applied Physics ( IF 3.4 ) Pub Date : 2021-06-04 , DOI: 10.1088/1361-6463/abfddd
Maxwell Quezada Feliz 1, 2 , Isabelle Polaert 2 , Alain Ledoux 2 , Christian Fernandez 1 , Federico Azzolina-Jury 1
Affiliation  

Dielectric barrier discharge (DBD) plasma technology is a promising method for producing methanol from CO2 hydrogenation as the reaction can be run at atmospheric pressure and temperatures below 100 C. The choice of the catalyst is crucial and has to be made not only according to its activity and selectivity towards the desired product, but its effect on plasma properties. In this work, the influence of several important catalytic properties of DBD plasma such as the dielectric constant of the catalyst and ionic conductivity is studied. The effects of the catalyst support and the addition of promoters on CO2 hydrogenation under DBD plasma are also studied. To this end, Cu and Cu–ZnO catalysts supported on γ-Al2O3 and a template-free seedless ZSM-5 (Si/Al molar ratio of 23) were prepared to study their catalytic performance on CO2 hydrogenation into methanol under DBD plasma. These catalysts were fully characterized by XRD, SEM, N2 physisorption, temperature programmed reduction and in situ FTIR CO adsorption. The relative complex permittivity of the catalysts was measured and the ionic conductivity was estimated using a modified Debye model. In this paper, the role of the ionic conductivity of the catalyst was identified as a crucial parameter in plasma-assisted CO2 hydrogenation. It was found that the lower the value of the ionic conductivity, the better the CO2 conversion. Indeed, high ionic conductivity reduces the density of the plasma and decreases the dissociation of CO2. The highest CO2 conversion value (34.0%) was observed for the nonconductive alumina support, whereas the highest methanol yield (0.5%) was observed for the zeolite-supported Cu–ZnO catalyst.



中文翻译:

催化剂离子电导率和介电常数对DBD等离子体辅助CO2加氢制甲醇的影响

介质阻挡放电 (DBD) 等离子体技术是一种有前景的从 CO 2加氢生产甲醇的方法,因为该反应可以在大气压和低于 100°C 的温度下进行。催化剂的选择至关重要,不仅要根据它对所需产物的活性和选择性,但它对等离子体特性的影响。在这项工作中,研究了 DBD 等离子体的几个重要催化性能,如催化剂的介电常数和离子电导率的影响。还研究了催化剂载体和助催化剂的加入对DBD等离子体下CO 2加氢的影响。为此,负载在γ -Al 2 O 3上的 Cu 和 Cu-ZnO 催化剂制备无模板无籽ZSM-5(Si/Al摩尔比为23)以研究其在DBD等离子体下CO 2加氢制甲醇的催化性能。这些催化剂通过XRD、SEM、N 2物理吸附、程序升温还原和原位FTIR CO吸附进行了充分表征。测量催化剂的相对复介电常数并使用改进的德拜模型估计离子电导率。在本文中,催化剂离子电导率的作用被确定为等离子体辅助 CO 2氢化中的关键参数。发现离子电导率值越低,CO 2越好转换。事实上,高离子电导率降低了等离子体的密度并减少了 CO 2的离解。对于非导电氧化铝载体观察到最高的 CO 2转化值 (34.0%),而在沸石负载的 Cu-ZnO 催化剂中观察到最高的甲醇产率 (0.5%)。

更新日期:2021-06-04
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