Vacancy-cluster-mediated surface activation for boosting CO₂ chemical fixation

Area of Science:

• Materials Science
• Catalysis
• Chemical Engineering

Background:

• Cycloaddition of carbon dioxide (CO2) with epoxides to form cyclic carbonates is a key strategy for CO2 utilization.
• Efficient catalysis requires active sites that promote epoxide adsorption and C-O bond cleavage.
• Two-dimensional materials offer unique properties for catalytic applications.

Purpose of the Study:

• To design and synthesize novel catalysts for enhanced CO2 cycloaddition with epoxides.
• To investigate the role of vacancy engineering in activating catalytic surfaces.
• To improve the generation of cyclic carbonates through CO2 utilization.

Main Methods:

• Utilizing two-dimensional FeOCl as a model material.
• Employing vacancy-cluster engineering to create electron-donor and -acceptor units.
• Combining theoretical simulations with in situ diffuse reflectance infrared Fourier-transform spectroscopy (in situ DRIFTS).

Main Results:

• Introduction of Fe-Cl vacancy clusters activates the FeOCl surface.
• Vacancy clusters provide reactive sites with electron-donor and -acceptor characteristics.
• Enhanced epoxide adsorption and accelerated C-O bond cleavage were observed.
• FeOCl nanosheets with vacancy clusters demonstrated superior cyclic carbonate generation.

Conclusions:

• Vacancy-cluster engineering is an effective strategy for designing advanced catalysts.
• Activated FeOCl nanosheets show significant potential for CO2 utilization via cycloaddition reactions.
• The developed catalytic system offers a promising route for sustainable chemical synthesis.