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- W2776831209 abstract "Compared to homogeneous catalysis, heterogeneous catalysis allows for ready separation of products from the catalyst and thus reuse of the catalyst. C-C coupling is typically performed on a molecular catalyst which is mixed with reactants in liquid phase during catalysis. This homogeneous mixing at a molecular level in the same phase makes separation of the molecular catalyst extremely challenging and costly. Here we demonstrated that a TiO2-based nanoparticle catalyst anchoring singly dispersed Pd atoms (Pd1/TiO2) is selective and highly active for more than 10 Sonogashira C-C coupling reactions (R≡CH + R'X → R≡R'; X = Br, I; R' = aryl or vinyl). The coupling between iodobenzene and phenylacetylene on Pd1/TiO2 exhibits a turnover rate of 51.0 diphenylacetylene molecules per anchored Pd atom per minute at 60 °C, with a low apparent activation barrier of 28.9 kJ/mol and no cost of catalyst separation. DFT calculations suggest that the single Pd atom bonded to surface lattice oxygen atoms of TiO2 acts as a site to dissociatively chemisorb iodobenzene to generate an intermediate phenyl, which then couples with phenylacetylenyl bound to a surface oxygen atom. This coupling of phenyl adsorbed on Pd1 and phenylacetylenyl bound to Oad of TiO2 forms the product molecule, diphenylacetylene." @default.
- W2776831209 created "2018-01-05" @default.
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- W2776831209 date "2018-01-11" @default.
- W2776831209 modified "2023-10-12" @default.
- W2776831209 title "C–C Coupling on Single-Atom-Based Heterogeneous Catalyst" @default.
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- W2776831209 doi "https://doi.org/10.1021/jacs.7b09314" @default.
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