杂多酸及其铯盐用于噻吩氧化脱硫反应的研究  

Oxidative desulfurization of thiophene using H202 as oxidant over Keggin-type heteropolyacids and cesium salts

作　　者：李新华[1] 丁孝涛[1] 金明善[1] 索掌怀[1] 

机构地区：[1]烟台大学应用催化研究所,山东烟台264005

出　　处：《Journal of Environmental Science and Engineering》2008年第4期5-9,共5页环境科学与工程（英文版）

基　　金：本文得到国家自然科学基金（项目编号：20473070）资助.

摘　　要：制备了钒取代磷铂杂多酸及杂多酸铯盐。X-光粉末衍射及IR光谱分析表明制备的杂多化合物均具有原有杂多酸的Keggin结构。以磷钨酸、磷钼酸、硅钨酸、磷钒铂酸及其铯盐为催化剂，H2O2为氧化剂考察了噻吩氧化脱硫的催化活性。发现对不同的杂多酸催化剂，其活性次序为：H3PW12O40〉H5PV2Mo10O40〉H6PV3Mo9O40〉H4VMo11O40〉H3PMo12O40〉〉H4SiW12O40。而杂多酸铯盐中Cs原子的数目对脱硫活性也有显着的影响。随CS原子数目的增加，CsxH3-xPW12O40的脱硫活性持续下降，CsxH3-xPMo12O40的活性变化并不明显，而CsxH5-xPV2Mo10O40的活性变化与Cs／H比有关。提高反应温度，可以显着提高其脱硫活性。Vanadium-substituted heteropolymolybdates （H4PVMo11O40, HsPV2MO10O40 and H6PV3Mo9040） and cesium salts of various heteropolyacids （CsxH3-xPW12O40, CsxH3-xPMo12O40 and CsxH5-xPV2Mo10O40） were prepared. The results from XRD and IR spectroscopy that these samples have Keggin structure. Oxidative desulfurization activity of thiophene using H2O2 as oxidant at mild conditions over these catalysts was evaluated. The activities are found to follow the order of H3PW12040 〉 H5PV2M10O40〉 H6PW3Mo9O40〉 H4PVMo11O40〉 H3PMo12O40 〉〉 H4SiW12O40. The desulfurization activities decrease with Cs number for CsxH3-xPW12O40 but slightly change for CsxH3-xPMo12O40. However, the desulfurization activities depend on Cs/H ratio in CsxH5-xPV2Mo10O40 and the maximal activity is observed at x=3.0. When the reaction temperature rises, higher activity is also found.

关 键 词：杂多酸 杂多酸绝盐 噻吩 氧化脱硫 

分 类 号：X51[环境科学与工程—环境工程]