Plasma technology is a promising method for activating small molecules. Propane (C₃H₈) dehydrogenation (PDH) is a strong endothermic reaction that faces thermodynamic limitations, which is expected to be addressed by plasma technology. Investigating the interplay of the plasma and catalysts, as well as its impact on PDH, is significant for designing efficient plasma mediated PDH systems. Herein, we report a strong interplay between plasma and catalysts during the PDH reaction, which determines the enhancement performance. It was observed that the consumption rate of C₃H₈ can be greatly boosted in plasma-mediated conditions over three representative metal oxide catalysts, i.e., Co/Al₂O₃, Ga/Al₂O₃, and V/Al₂O₃. Discharge power calculations suggest that the activation of C₃H₈ by nonthermal plasma is primarily in the form of vibrational excitation, which reduces the activation energy required for the PDH and thus enhances the consumption rate of C₃H₈. A systematic study of the metal oxide catalysts by manipulating the number of active sites and the molecules of the vibrational excited state of C₃H₈ revealed a strong interplay between plasma and catalysts. For plasma-mediated PDH reactions, the rate increases with the loading of metal oxides, followed by a constant value in high-loading regions. In contrast, the values increased monotonically under the same conditions under pure thermal conditions. This suggests that the PDH performance in plasma-mediated conditions is determined by both the number of active sites and the amount of vibrationally excited molecules, while that for the pure thermal reaction is solely dictated by the number of active sites. This work is expected to advance the rational design of plasma-assisted systems with the optimal performance for more sustainable catalysis.

中文翻译：

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揭示丙烷脱氢反应中非热等离子体和金属氧化物催化剂之间的相互作用


等离子体技术是一种很有前途的激活小分子的方法。丙烷 （C₃H₈） 脱氢 （PDH） 是一种强吸热反应，面临热力学限制，有望通过等离子体技术来解决。研究等离子体和催化剂的相互作用及其对 PDH 的影响，对于设计高效的等离子体介导的 PDH 系统具有重要意义。在此，我们报道了 PDH 反应过程中等离子体和催化剂之间的强相互作用，这决定了增强性能。据观察，在等离子体介导的条件下，C₃H₈ 的消耗率可以大大提高三种代表性金属氧化物催化剂，即 Co/Al₂O₃、Ga/Al₂O₃ 和 V/Al₂O₃。放电功率计算表明，非热等离子体对 C₃H₈ 的活化主要以振动激发的形式出现，这降低了 PDH 所需的活化能，从而提高了 C₃H₈ 的消耗率。通过操纵 C₃H₈ 的活性位点和分子的数量对金属氧化物催化剂进行系统研究，揭示了等离子体和催化剂之间的强相互作用。对于等离子体介导的 PDH 反应，速率随着金属氧化物的负载而增加，随后在高负载区域保持恒定值。相比之下，在纯热条件下，在相同条件下，这些值单调增加。 这表明，在等离子体介导的条件下，PDH 性能由活性位点的数量和振动激发的分子的数量决定，而纯热反应的性能完全由活性位点的数量决定。这项工作有望推进等离子体辅助系统的合理设计，并为更可持续的催化提供最佳性能。