Abstract
Selective oxygenation of alkanes via CH bond activation still remains a challenge because the oxygen-containing products are more active than the substrates. Here, we develop a new concept of eco-friendly zeolite-fixed photocatalyst to impart catalytic performance via loading CuCl2 upon visible-light irradiation. Complete selectivity in terms of the final oxidation product KA-oil was obtained with 24% conversion in the application of cyclohexane oxidation. After optimization, the desired ketones and alcohols were also obtained in good to excellent selectivities with broad substrate scope. Multiple experimental studies combined with theoretical calculations demonstrate that the formation of the unique CuCl2/TS-1 hollow structure with isolated CuCl2 species anchored onto the inner and outer surface of TS-1 shells: the function of the major tetrahedral Ti–O4 sites in heterojunctions to isolate energy levels near the conduction and valence bands. In photocatalysis, the presence of Cu–O–Ti–O3 heterojunctions facilitates separation and transfer of photogenerated electrons and holes
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