期刊
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
卷 8, 期 17, 页码 6622-6633出版社
AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.9b07212
关键词
Metal-organic frameworks; MoS2; Visible light; Photocatalysis; Cyclohexane oxidation
资金
- National Key Research and Development Plan [2016YFC0303704]
- National Natural Science Foundation of China [21676296]
Selective oxidation of cyclohexane to KA oil (cyclohexanol and cyclohexanone) is one of the most important industrial procedure. In this study, we reported a remarkably enhanced cyclohexane oxidation under visible-light irradiation by a novel MoS(2)pCu/Cu(2)OpC composite photocatalyst with multilevel hierarchy, which was prepared by immersing (NH4)(2)MoS4 guest into Cumetal-organic framework (MOF) polyhedra host and subsequently pyrolyzing the Cu-MOF-guest polyhedra to encapsulate MoS2 into Cu/Cu2O@C. Importantly, the composite photocatalyst showed much better photocatalytic cydohexane oxidation performance than that of the simple mechanical mixture of MoS2 and Cu/Cu2O@C. The distinct photocatalytic performance of MoS(2)pCu/Cu(2)OpC composite can be ascribed to its heterojunction band reconstruction and unique multilevel architecture to facilitate the separation of photoinduced electrons and holes and generation reactive species during photoirradiation. The Cu nanoparticles in the MoS(2)pCu/Cu2O@C composite also effectively capture electrons and prevent electron-hole recombination due to the surface plasmon resonance (SPR). The photogenerated holes (h(+)) and center dot OH radical were supposed to be predominant components of the valence band (VB) and oxidize cyclohexane (C6H12) to produce cyclohexyl radical (C6H11 center dot), which can be further oxidized to cyclohexanol and cyclohexanone. According to the above results, a possible photocatalytic mechanism was proposed.
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