4.8 Article

Designing Heteroatom-Codoped Iron Metal-Organic Framework for Promotional Photoreduction of Carbon Dioxide to Ethylene

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WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202216232

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C2H4; CO2 Reduction; Doping; Metal-Organic Frameworks; Photocatalysis

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In this study, a N,S-doped Fe-based MIL-88B catalyst with a well-defined hexagonal prism morphology was designed and synthesized. The catalyst showed a high yield of C2H4 evolution under simulated solar irradiation, which was due to the synergistic effect of Fe-N coordinated sites and reasonable defects in the N,S-doped photocatalyst, facilitating the formation and dimerization of C-C coupling intermediates.
Rational engineering active sites and vantage defects of catalysts are promising but grand challenging task to enhance photoreduction CO2 to high value-added C2 products. In this study, we designed an N,S-codoped Fe-based MIL-88B catalyst with well-defined bipyramidal hexagonal prism morphology via a facile and effective process, which was synthesized by addition of appropriate 1,2-benzisothiazolin-3-one (BIT) and acetic acid to the reaction solution. Under simulated solar irradiation, the designed catalyst exhibits high C2H4 evolution yield of 17.7 mu mol g(-1)center dot h, which has been rarely achieved in photocatalytic CO2 reduction process. The synergistic effect of Fe-N coordinated sites and reasonable defects in the N,S-codoped photocatalyst can accelerate the migration of photogenerated carriers, resulting in high electron density, and this in turn helps to facilitate the formation and dimerization of C-C coupling intermediates for C2H4 effectively.

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