MXene (Ti <inf>3</inf> C <inf>2</inf> ) Vacancy-Confined Single-Atom Catalyst for Efficient Functionalization of CO <inf>2</inf>
- Publication Type:
- Journal Article
- Journal of the American Chemical Society, 2019, 141 (9), pp. 4086 - 4093
- Issue Date:
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© Copyright 2019 American Chemical Society. A central topic in single-atom catalysis is building strong interactions between single atoms and the support for stabilization. Herein we report the preparation of stabilized single-atom catalysts via a simultaneous self-reduction stabilization process at room temperature using ultrathin two-dimensional Ti 3-x C 2 T y MXene nanosheets characterized by abundant Ti-deficit vacancy defects and a high reducing capability. The single atoms therein form strong metal-carbon bonds with the Ti 3-x C 2 T y support and are therefore stabilized onto the sites previously occupied by Ti. Pt-based single-atom catalyst (SAC) Pt 1 /Ti 3-x C 2 T y offers a green route to utilizing greenhouse gas CO 2 , via the formylation of amines, as a C 1 source in organic synthesis. DFT calculations reveal that, compared to Pt nanoparticles, the single Pt atoms on Ti 3-x C 2 T y support feature partial positive charges and atomic dispersion, which helps to significantly decrease the adsorption energy and activation energy of silane, CO 2 , and aniline, thereby boosting catalytic performance. We believe that these results would open up new opportunities for the fabrication of SACs and the applications of MXenes in organic synthesis.
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