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The sequestration of atmospheric CO2 into value-added products is of great interest from economic and environmental perspectives. The tetra-shelled Cr1.3Fe0.7O3 hollow sphere as a heterogeneous catalyst was synthesized by a simple hydrothermal method followed by calcination at 600 °C. The synthesized tetra-shelled hollow spheres were characterized by several effective tools. The catalytic performance was studied for the cycloaddition reaction of CO2 with epoxides under solvent-free conditions. The reaction time, reaction temperature, CO2 pressure, and the catalyst amount were systematically studied. Under the best-experimented condition (0.02 g of the catalyst, 80 °C, 6 h, and 4 bar CO2 pressure), the catalyst demonstrated a broad substrate scope and functional group tolerance. Besides, the catalyst showed high recycling efficiency for five consecutive reaction cycles with no significant decline in activity. [ABSTRACT FROM AUTHOR]