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Exceptionally Fast Heterogeneous Catalysis Using Perovskite Nanocrystals for Hydrocarbon Aromatization
Melad Shaikh1, Nhu Dang1, Jericho Reyes1
1Department of Chemistry and Biochemistry, San Diego State University, San Diego, California 92182, United States.
None:
Heterogeneous catalysis, though often slower than homogeneous catalysis due to mass transfer and adsorption limitations, is favored in industry for its facile separation, reusability, and scalability. Overcoming heterogeneous limitations demands innovative catalyst architectures and reaction designs. Here we report a lead halide perovskite CsPbBr3 nanocrystal (NC) heterogeneous catalytic system that achieves exceptionally fast hydrocarbon aromatization, with turnover frequencies (TOFs) up to 6.5 s-1 per Cs, or up to 11.1 mol/kg/s, enabling kilograms of benzene formation from cyclohexene with milligrams of catalyst loading under ambient condition. Driven by a radical chain mechanism with over 848% quantum yield under visible-light, this system exhibits broad functional group tolerance, aromatizes substituted cyclohexenes with high selectivity, and extends to acyclic olefins via a photocatalytic [4 + 2] aromatization route. Our perovskite catalysis approach thus offers a transformative highly reactive avenue to complex arenes and heteroarenes, bridging gaps between hetero- and homogeneous catalysis.
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