摘要
The metal species embedded in specific positions within the zeolite framework and their unique microenvironment exhibit fascinating effects on catalytic performance. Herein, we incorporated tetrahedrally coordinated Co 2+ into the framework of hollow silicate-1 zeolite and investigated the influence of halogen anions (Cl - , Br - and F - ) in the synthesized gel on the distribution of cobalt species in the channels. The addition of an appropriate amount of inorganic ammonium salts and seeds was found to be a necessary condition for cobalt incorporated into the framework. Notably, the Cl - anions present in the synthesis gel can induce more cobalt species located at the intersection cavity of silicate-1 (β-type). Comprehensive characterization results indicate that the tetrahedrally coordinated Co 2+ in the intersecting cavities of hollow zeolite appears to exhibit more efficient styrene epoxidation performance. This work presents a simple and cost-effective method to synthesize hollow cobalt-based zeolite with adjustable metal distribution in channels. By regulating the spatial distribution of cobalt species with halogens, the CS-0.1–0.5-Cl catalyst enhanced activity and selectivity in the epoxidation reaction of styrene to styrene oxide. Specifically, at a temperature of 80 °C after a reaction time of 6 h, the catalyst demonstrated a styrene oxide yield of 42.47 % and a excellent styrene oxide selectivity of 82.29 %.
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