Abstract:

Non-thermal plasma (NTP) activated heterogeneous catalyst (i.e. NTP-catalysis) systems have many advantages, such as mild reaction conditions, faster response, and possible compact reactor configuration, presenting wide application foreground in the catalytic transformation of single-carbon (C₁) molecules [CO₂ hydrogenation, methane activation, water-gas shift (WGS) reaction, and methanol-reforming for hydrogen (H₂) production]. In detail, the high energy electron of plasma can quickly activate C₁ molecules in the gas-phase to generate reactive species, which will interact with the heterogeneous catalyst to ignite surface chemical reaction, and hence efficiently catalytic conversion of C₁ molecules under mild conditions. However, the synergic mechanism between plasma and catalyst, as well as relevant catalytic reaction mechanisms, are highly complex, which require further investigation. This review briefly presents the state-of-the-art of NTP-catalysis for catalytic conversion of C₁ molecules. Specific attention focuses on ①the design and development of bespoke heterogeneous catalysts for NTP-catalytic conversions of C₁ molecules and ② mechanistic investigations of catalytic conversions of C₁ molecules under NTP conditions using advanced in situ characterization methods. Additionally, future perspectives of NTP-catalysis are also proposed in this review including ① the design and development of tailor-made catalysts for NTP-catalysis, and study their structure-reactivity relationships, ② the development of advanced in situ characterization techniques for gaining further insights into the function mechanisms of active species and the catalytic reaction mechanisms, ③ the design and development of highly efficient plasma catalytic reactor, and the development of theoretical model and numerical simulation method for developed reactor, providing the scientific guidance of the design, optimization and scaling-up of plasma catalytic reactor.

Key words: non-thermal plasma (NTP), catalyst, C₁ molecule, catalytic mechanism, in situ characterization

摘要：

非热等离子体催化具有反应条件温和、启动快和反应器结构紧凑等特点，在C₁分子催化转化领域（如CO₂加氢、甲烷活化、水煤气变换反应和甲醇重整制氢）有着广阔的应用前景。具体来说，等离子体特有的高能电子可在气相中快速活化稳定性极强的C₁分子并生成活性物质，接着与催化剂结合发生表面化学反应，从而实现常温常压下C₁分子的高效转化。然而，等离子体与催化剂之间的协同作用机制以及催化机理极为复杂，仍有待进一步研究。本综述简单介绍了非热等离子体催化转化C₁分子的近期研究进展，重点探讨了适用于非热等离子 体的催化剂研究以及催化机理的高级原位表征。最后，提出了非热等离子体催化转化C₁分子的未来发展方向：①设计并构筑适用于非热等离子体催化的高效催化剂，并研究其构效关系；②发展高级原位表征技术，揭示活性物质的作用机理以及催化机理；③设计并构建高效的等离子体催化反应器，并建立反应器的理论模型和数值模拟方法，科学指导等离子体反应器的设计、优化和放大。

关键词: 非热等离子体, 催化剂, C₁分子, 催化机理, 原位表征