2025-12-17 分子科学研究所
＜関連情報＞
マルチモーダルオペランド解析により明らかにされたメタンの直流促進乾式改質における非熱触媒的起源 Nonthermal Catalytic Origin in DC-Enhanced Dry Reforming of Methane Unveiled by Multimodal Operando Analyses
Harunobu Tedzuka,Hikaru Saito,Nobuki Matsumoto,Masanari Nagasaka,Hiromasa Sato,Yasushi Sekine,and Toshiki Sugimoto
The Journal of Chemistry Letters Published: December 11, 2025
DOI:https://doi.org/10.1021/acs.jpclett.5c03159
Abstract
Catalytic dry reforming of methane (DRM) is a key reaction for the sustainable utilization of major greenhouse gases, CO2 and CH4. However, conventional DRM often suffers from severe catalyst deactivation due to high temperature requirements. Applying direct current (DC) to catalysts has emerged as a promising strategy to overcome these limitations, yet the underlying DC-enhanced catalytic mechanisms remain elusive. Here, we unveil the nonthermal catalytic origin of DC-applied DRM over Pd/CeO2 through multimodal operando analyses. Spatially resolved operando infrared measurements revealed that key reaction intermediates specific to nonthermal DRM exclusively emerge on current-carrying regions of the catalyst surface under DC bias. Furthermore, operando infrared and visible absorption spectroscopy detected the trapped electrons and holes generated in CeO2 during DC application and revealed a clear correlation between the density of injected charges and the DRM activity. Soft X-ray spectroscopic analysis uncovers an unconventional pathway of hole generation in nominally n-type CeO2 under DC bias. These observations demonstrate that DC application induces distinct molecular and electronic species that promote CO2 reduction and CH4 oxidation in DRM via nonthermal pathways.
