Experimental study demonstrates high light olefin yield using surface-engineered ZnZrOx and SAPO-34, indicating a scalable pathway for carbon dioxide utilization.
Key Points
To develop a high-surface-area ZnZrOx solid-solution catalyst with enriched surface active sites to overcome the kinetic and adsorption limitations of conventional catalysts in converting CO2 to light olefins.
Synthesized a ZnZrOx solid-solution catalyst using a kinetics-controlled precipitation method driven by slow ammonia gas diffusion.
Coupled the surface-engineered ZnZrOx catalyst with a SAPO-34 zeolite to form a bifunctional catalytic system for methanol-mediated CO2 hydrogenation.
Investigated reaction mechanisms and surface intermediates using in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and evaluated catalytic stability over 100 hours.
The gas diffusion strategy produced a ZnZrOx catalyst with a specific surface area of 89.4 m2·g–1, surface Zn enrichment, and increased density of Zn–O–Zr sites and oxygen vacancies.
Coupled with SAPO-34, the catalyst achieved a CO2 conversion of 28.2%, light olefin selectivity of 86.6%, and light olefin yield of 13.5%.
Demonstrated durable stability with less than a 0.4 percentage point drop in light olefin yield over 100 hours of continuous operation.