Tailoring Zeolite L-Supported-Cu Catalysts for CO₂ Hydrogenation: Insights into the Mechanism of CH₃OH and CO Formation

Abstract

The utilization of Cu-based catalysts in CO 2 conversion into valuable chemicals is of significant interest due to their potential in mitigating greenhouse gas emissions. However, the controllable design of Cu-based catalysts and the regulation of their mechanism remain challenging. In this study, a series of efficient Cu/L catalysts were prepared for this process, and the intrinsic influencing factors on the reaction routes were systematically revealed. Various techniques revealed that Cu particles in Lsupported catalysts exhibited higher dispersion and formed Cu− O(OH)−K interfacial sites. However, with increasing Cu loading, the dispersion of Cu particles and the percentage of Cu−O(OH)− K interfaces decreased. Kinetic investigations revealed that the adsorption configuration and electronic structure of Cu species codetermined the reaction pathways and resulting selectivity. Cu/L catalysts possessing Cu−O(OH)−K interfaces and small particles demonstrated the preferential formation of formate species, promoting methanol formation. However, larger Cu particles generated carboxylate intermediates, resulting in higher CO selectivity..

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