A bifunctional POM-based Cu-viologen complex with mixed octamolybdate clusters for rapid oxidation desulfurization and effective photogeneration of hydrogen AITranslate

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Chinese Library Classification Number:O641.4[理学—物理化学];O643.36[理学—物理化学]

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The design and synthesis of catalysts for the oxidation desulfurization and production of hydrogen are extremely important for solving environmental pollution and energy shortage.Herein,a novel bifunctional [α-Mo₈O₂₆]^4-/[β-Mo₈O₂₆]^4--based Cu-viologen complex H₄[Cu₂~ⅠCl₂(Hbcbpy)₄] [α-Mo₈O₂₆] [β-Mo8O₂₆]·H₂O(BHU-2,Hbcbpy=1-(4-carboxybenzyl)-4,4'-bipyridinium) was synthesized and characterized by single-crystal X-ray diffraction(XRD),infrared radiation spectra,powder X-ray diffraction(PXRD) and X-ray photoelectron spectroscopy(XPS) spectra.The structural characteristic of BHU-2 is the presence of two types of octamolybdate clusters [α-Mo₈O₂₆]^4-/[β-Mo₈O₂₆]^4-and a new binuclear Cu~Ⅰ-Hbcbpy complex linked by Cl-bridges[Cu₂ⅠCl₂(Hbcbpy)₄]⁴⁺.BHU-2 as a heterogeneous catalyst exhibits excellent activities to the oxidation desulfurization and photocatalytic hydrogen production.At room temperature,BHU-2 can catalyze 96% conversion of methyl phenyl sulfide with 98% selectivity,and the process obeys the pseudo-first-order reaction kinetic with the half-life of9.6 min.The notorious 2-chloroethyl ethyl sulfide can achieve 99% conversion with 98% selectivity within only1 min at the presence of BHU-2,and the turnover frequency(TOF) is up to 7400 h^-1.BHU-2 also exhibits high catalytic activity for the oxidation of other aromatic and aliphatic thioethers within short time at room temperature.Furthermore,BHU-2 shows a high catalytic activity for visible-light-driven hydrogen evolution with an H₂ evolution rate of 1677.85 μmol·g^-1·h^-1 within 10 h.Moreover,the catalytic activities do not decrease evidently after three cycles,revealing the prominent structural stability and recyclability.