Plasma-Derived Atomic Hydrogen Enables Eley–Rideal-Type CO2 Methanation at Low Temperatures

作者：Dae-Yeong Kim, Yoshinobu Inagaki, Tsukasa Yamakawa, Bang Lu, Yoshiaki Sato, Naoki Shirai, Shinya Furukawa, Hyun‐Ha Kim, Satoru Takakusagi, Koichi Sasaki, Tomohiro Nozaki · 发表于：JACS Au · 年份：2024 · DOI：10.1021/jacsau.4c00857 · 被引用次数：19 · 研究领域：Catalytic Processes in Materials Science、Carbon dioxide utilization in catalysis、Ammonia Synthesis and Nitrogen Reduction

High Resolution Image Download MS PowerPoint Slide Activating H 2 molecules into atomic hydrogen and utilizing their intrinsic chemical reactivity are important processes in catalytic hydrogenation. Here, we have developed a plasma-catalyst combined system that directly provides atomic hydrogen from the gas phase to the catalytic reaction to utilize the high energy and translational freedom of atomic hydrogen. In this system, we show that the temperature of CO 2 methanation over Ni/Al 2 O 3 can be dramatically lower compared to thermal catalysis. Using a detailed mechanistic study with kinetic studies, laser plasma diagnostics, in situ plasma surface characterization, and theoretical calculations, we revealed that plasma-derived atomic hydrogen (PDAH) plays a crucial role in reaction promotion. In particular, PDAH effectively lowers the energy barrier of bidentate formate hydrogenation by translating from the Langmuir–Hinshelwood to the Eley–Rideal-type reaction.