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Overcoming the Activity-CH4 Reducibility Trade-off in Dry Reforming of Methane via Spatially Separated Rh1 and
Wenjie Guo1, Wenbin Li1,2, Jiyun Ren1
1School of Chemistry and Chemical Engineering, Northwestern Polytechnical University, Xi'an, 710072, China.
Abstract:
Achieving high CO2 conversion with minimal reductant input is essential for enabling a sustainable carbon cycle. Dry reforming of methane (DRM) represents a key pathway toward this goal, yet it is typically limited by CH4 reducibility (moles of CO2 consumed per mole of CH4) of 1 molCO2 molCH4 -1, and temperatures >700 °C. These limitations arise from an inherent trade-off between catalytic activity and CH4 reducibility, imposed by thermodynamic and kinetic constraints. Herein, we report a catalyst comprising spatially isolated Rh atoms (Rh1) and frustrated Lewis pairs (FLPs) on porous CeO2 nanorods, which decouples the DRM process into two elemental steps: CO2 reduction and CH4 partial oxidation. This spatial separation enables simultaneous high activity and exceptional CH4 reducibility by facilitating *O migration form FLPs (for CO2 reduction and *O storage) to Rh1 (for CH4 partial oxidation). The optimized catalyst exhibits a CO production rate of 83.4 mol gRh -1 h-1 at 450 °C, surpassing state-of-the-art catalysts, while achieving a CH4 reducibility of 2.54 molCO2 molCH4 -1, significantly exceeding the conventional DRM limit. Furthermore, the catalyst demonstrates outstanding stability over 350 h. This work offers a robust strategy for overcoming classical trade-off in DRM, rendering it a promising candidate for industrial application.
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