| Ti-MWW分子筛催化硫醚氧化反应的机理 |
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| 引用本文： | 卞贺,张健,高志杰,张会明,徐斌,张士国,夏道宏.Ti-MWW分子筛催化硫醚氧化反应的机理[J].石油学报(石油加工),2019,35(5):874-882. |
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| 作者姓名： | 卞贺 张健 高志杰 张会明 徐斌 张士国 夏道宏 |
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| 作者单位： | 1滨州学院 化工与安全学院,山东 滨州 256603；2中国石油大学(华东) 重质油国家重点实验室，山东 青岛 266580 |
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| 基金项目： | 山东省自然科学基金项目(ZR2015BL012, ZR2018QB007,ZR2016BL09)、滨州市科技发展计划项目(2014ZC0321)、滨州学院科研基金项目(BZXYG1607)资助 |
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| 摘 要： | 采用密度泛函理论的B3LYP D3方法，在6 31G(d,p)基组水平上研究了钛硅分子筛(Ti MWW)/过氧化氢(H2O2)体系T3位点活性中心上二甲基硫醚(DMS)氧化反应的微观机理，并考察了不同溶剂分子对Ti MWW分子筛催化性能的影响。结果表明：不同溶剂分子在活性中心上的吸附能力由强到弱依次为CH3COCH3、CH3OH、H2O、CH3CN；钛 氧活性中间体的催化活性由大到小依次为Ti η2 OOH CH3OH、Ti η2 OOH CH3COCH3、Ti η2 OOH H2O、Ti η2 OOH CH3CN、Ti η2 OOH、Ti η1 OOH。Ti MWW分子筛作为催化剂显著降低了二甲基硫醚与过氧化氢氧化反应的能垒，有利于反应的发生。
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| 关 键 词： | 密度泛函理论 钛硅分子筛(Ti-MWW) 二甲基硫醚 氧化脱硫 |
| 收稿时间： | 2018-10-08 |
Mechanism of Catalyzed Oxidation of Thioether by Ti-MWW Zeolite |
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| BIAN He,ZHANG Jian,GAO Zhijie,ZHANG Huiming,XU Bin,ZHANG Shiguo,XIA Daohong.Mechanism of Catalyzed Oxidation of Thioether by Ti-MWW Zeolite[J].Acta Petrolei Sinica (Petroleum Processing Section),2019,35(5):874-882. |
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| Authors: | BIAN He ZHANG Jian GAO Zhijie ZHANG Huiming XU Bin ZHANG Shiguo XIA Daohong |
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| Affiliation: | 1Department of Chemical Engineering and Safety, Binzhou University, Binzhou 256603, China;
2China State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Qingdao 266580, China |
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| Abstract: | The oxidative reaction mechanism of dimethyl sulfide on the T3 site in titanium silicalite Ti MWW/H2O2 system was studied at the B3LYP D3/6 31G (d,p) level of theory as well as effects of solvents on the catalytic performance. The results show that the adsorption capacity of solvents on active centers follows the descend order: CH3COCH3, CH3OH, H2O, CH3CN, and the catalytic activity follows the descend order: Ti η2 OOH CH3OH, Ti η2 OOH CH3COCH3, Ti η2 OOH H2O,Ti η2 OOH CH3CN, Ti η2 OOH, Ti η1 OOH. Moreover, it is found that Ti MWW zeolite significantly reduces the energy barrier for the reaction between DMS and H2O2, which makes the reaction occur more easily. |
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| Keywords: | density functional theory titanium silicalite (Ti-MWW) zeolite dimethyl sulfide oxidative desulfurization |
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