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>Photocatalytic C–H activation for C–C/CN/C–S bond formation over CdS: effect of morphological regulation and S vacancies
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Photocatalytic C–H activation for C–C/CN/C–S bond formation over CdS: effect of morphological regulation and S vacancies
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机译：Photocatalytic C–H activation for C–C/CN/C–S bond formation over CdS: effect of morphological regulation and S vacancies
The construction of C–X (X = C, N, S) bonds through C–H activation is one of the most challenging, important and rapidly developing fields in recent years. Herein, CdS with different morphologies (nanorods, nanospheres, nanosheets) was prepared by a thermal solvent method, and CdS enriched with S vacancies was constructed through simple calcination. The as-prepared heterogeneous CdS catalytic materials were utilized to fabricate C–C, CN and C–S bonds for the manufacture of drug intermediates or other value-added products through high bond energy, low polarity and strong inertia C–H bond activation. For example, the direct activation of sp3 C–H chemical bonds of tetrahydrofuran (THF) to form THF free radical and the free radical addition with olefins/alkynes could be achieved with various CdS catalytic materials without a base additive and oxidant. The CdS morphology improved the photocatalytic performance through the effective photogenerated carrier separation and transformation enhancement caused by the formation of hexagonal-phase CdS along with a certain degree of lattice distortion induced polarization dipole moment and internal polarization electric field. Furthermore, the S-vacancy-enriched CdS nanorods provided more active sites for THF capture and tetrahydrofuran free radical generation, so that the THF sp3 C–H direct activation to construct C–C bonds became more feasible. DMF and toluene sp3 C–H could also be activated to form C–C bonds; benzylamine sp3 C–H could be activated to construct CN bonds accompanied by H2 generation; benzyl mercaptan S–H bonds and phenylacetylene/styrene C–H bonds could be activated to build C–S bonds; and benzene/toluene C–H bonds could be activated in the presence of CO2 to produce carboxylic acid. Compared with the method requiring a stoichiometric oxidant in previous studies, the C–H activation of THF and the construction of other inert chemical structures could be mildly realized over S-vacancy-enriched hexagonal CdS nanorods.
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