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

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Rare Metals 2024年第1期43卷 236-246页

作者： Lin Yang Zhong Zhang Chao-Nan Zhang Xiu-Li Wang College of Chemistry and Materials Engineering Bohai UniversityJinzhou 121013China Professional Technology Innovation Center of Liaoning Province for Conversion Materials of Solar Cell Bohai UniversityJinzhou 121013China

The design and synthesis of catalysts for the oxidation desulfurization and production of hydrogen are extremely important for solving environmental pollution and energy ***,a novel bifunctional [α-Mo_(8)O_(26)]^(4-)/[β-Mo_(8)O_(26)]^(4-)-based Cu-viologen complex H_(4)[Cu_(2)~ⅠCl_(2)(Hbcbpy)_(4)] [α-Mo_(8)O_(26)] [β-Mo8O_(26)]·H_(2)O(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) *** structural characteristic of BHU-2 is the presence of two types of octamolybdate clusters [α-Mo_(8)O_(26)]^(4-)/[β-Mo_(8)O_(26)]^(4-)and a new binuclear Cu~Ⅰ-Hbcbpy complex linked by Cl-bridges[Cu_(2)ⅠCl_(2)(Hbcbpy)_(4)]^(4+).BHU-2 as a heterogeneous catalyst exhibits excellent activities to the oxidation desulfurization and photocatalytic hydrogen *** 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 *** 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 ***,BHU-2 shows a high catalytic activity for visible-light-driven hydrogen evolution with an H_(2) evolution rate of 1677.85 μmol·g^(-1)·h^(-1) within 10 ***,the catalytic activities do not decrease evidently after three cycles,revealing the prominent structural stability and recyclability.

关键词： Polyoxometalate Metal-organic complex Viologen oxidation desulfurization Photocatalytic hydrogen production

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oxidation Reactivities of Organic Sulfur Compounds in Fuel Oil Using Immobilized Heteropoly Acid as Catalyst

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Journal of Wuhan University of Technology(Materials Science) 2007年第2期22卷 320-324页

作者：颜学敏雷家珩 Department of Applied Chemistry Wuhan University of Technology

Heteropoly acid of Keggin structure phosphotungstic（HPW） and phosphomolybdic（HPMo） were chemically anchored to the modified SBA-15 channel. The materials were used as catalyst for oxidative desulfurization of organic sulfur compounds including benzothiophene （BT）, dibenzothiophene （DBT） and 4,6-dimethydibenzothiophene （4,6-DMDBT）. The experimental results show that the catalysts are efficient and reusable, the catalytic activity is hardly reduced even in the 5th cycle of use.

关键词： SBA-15 phosphotungstic phosphomolybdic oxidation desulfurization

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