Toward Carbon Monoxide Methanation at Mild Conditions on Dual- Site Catalysts

The catalytic carbon monoxide (CO) methanation is an ideal model reaction for the fundamental understanding of catalysis on the gas-solid interface and is crucial for various industrial processes. However, the harsh operating conditions make the reaction unsustainable, and the limitations set by the scaling relations between the dissociation energy barrier and dissociative binding energy of CO further increase the difficulty in designing high-performance methanation catalysts operating under milder conditions. Herein, we proposed a theoretical strategy to circumvent the limitations elegantly and achieve both facile CO dissociation and C/O hydrogenation on the catalyst containing a confined dual site. The DFT-based microkinetic modeling (MKM) reveals that the designed Co-Cr2/G dual-site catalyst could provide 4-6 orders of magnitude higher turnover frequency for CH4 production than the cobalt step sites. We believe that the proposed strategy in the current work will provide essential guidance for designing state-of-the-art methanation catalysts under mild conditions.

Automated summary

In this study, a new theoretical strategy was proposed to achieve both facile CO dissociation and C/O hydrogenation on a catalyst by introducing confined dual active sites. The DFT-based microkinetic modeling showed that the designed Co-Cr2/G dual-site catalyst provided 4-6 orders of magnitude higher turnover frequency for CH4 production compared to cobalt step sites. We believe that this strategy will provide essential guidance for designing state-of-the-art methanation catalysts under mild conditions.