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Πέμπτη 24 Ιανουαρίου 2019

Metal–Organic‐Framework‐Derived Hollow N‐Doped Porous Carbon with Ultrahigh Concentrations of Single Zn Atoms for Efficient Carbon Dioxide Conversion

Metal–Organic‐Framework‐Derived Hollow N‐Doped Porous Carbon with Ultrahigh Concentrations of Single Zn Atoms for Efficient Carbon Dioxide Conversion:

Angewandte Chemie International Edition Metal–Organic‐Framework‐Derived Hollow N‐Doped Porous Carbon with Ultrahigh Concentrations of Single Zn Atoms for Efficient Carbon Dioxide Conversion
Hollow porous carbons (HPC), featuring hierarchical pores and uniform dopants of nitrogen and ultrahigh content (11.3 wt %) of single‐atom Zn, are fabricated by the pyrolysis of template‐directed hollow ZIF‐8 spheres. Thanks to the Zn/N sites and the photothermal effect endowed by those features, the optimized HPC‐800 efficiently catalyzes CO2 cycloaddition with epoxides under light irradiation at ambient temperature.





Abstract

The development of efficient and low energy‐consumption catalysts for CO2 conversion is desired, yet remains a great challenge. Herein, a class of novel hollow porous carbons (HPC), featuring well dispersed dopants of nitrogen and single Zn atoms, have been fabricated, based on the templated growth of a hollow metal–organic framework precursor, followed by pyrolysis. The optimized HPC‐800 achieves efficient catalytic CO2 cycloaddition with epoxides, under light irradiation, at ambient temperature, by taking advantage of an ultrahigh loading of (11.3 wt %) single‐atom Zn and uniform N active sites, high‐efficiency photothermal conversion as well as the hierarchical pores in the carbon shell. As far as we know, this is the first report on the integration of the photothermal effect of carbon‐based materials with single metal atoms for catalytic CO2 fixation.

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