首页|Engineering surface framework Ti06 single sites for unprecedented deep oxidative desulfurization

Engineering surface framework Ti06 single sites for unprecedented deep oxidative desulfurization

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Catalytic oxidative desulfurization(ODS)using titanium silicate catalysts has emerged as an efficient technique for the complete removal of organosulfur compounds from automotive fuels.However,the precise control of highly accessible and stable-framework Ti active sites remains highly challenging.Here we reveal for the first time by using density functional theory calculations that framework hexa-coordinated Ti(TiO6)species of mesoporous titanium silicates are the most active sites for ODS and lead to a lower-energy pathway of ODS.A novel method to achieve highly accessible and homogeneously distributed framework TiO6 active single sites at the mesoporous surface has been developed.Such surface framework TiO6 species exhibit an exceptional ODS performance.A removal of 920 ppm of benzothiophene is achieved at 60℃ in 60 min,which is 1.67 times that of the best catalyst reported so far.For bulky molecules such as 4,6-dimethyldibenzothiophene(DMDBT),it takes only 3 min to remove 500 ppm of DMDBT at 60℃ with our catalyst,which is five times faster than that with the current best catalyst.Such a catalyst can be easily upscaled and could be used for concrete industrial application in the ODS of bulky organosulfur compounds with minimized energy consumption and high reaction efficiency.

electrostatic interactionsframework hexa-coordinated Ti siteoxidative desulfurizationmesoporous materialsself-assembly

Shen Yu、Zhan Liu、Jia-Min Lyu、Chun-Mu Guo、Xiao-Yu Yang、Peng Jiang、Yi-Long Wang、Zhi-Yi Hu、Ming-Hui Sun、Yu Li、Li-Hua Chen、Bao-Lian Su

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Laboratory of Living Materials at the State Key Laboratory of Advanced Technology for Materials Synthesis and Processing,Wuhan University of Technology,Wuhan 430070,China

Nanostructure Research Center,Wuhan University of Technology,Wuhan 430070,China

School of Chemistry,Chemical Engineering and Life Science,Wuhan University of Technology,Wuhan 430070,China

Laboratory of Inorganic Materials Chemistry,University of Namur,Namur B-5000,Belgium

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国家重点研发计划国家自然科学基金国家自然科学基金国家自然科学基金国家自然科学基金Program of Introducing Talents of Discipline to Universities-Plan 111 from the Ministry of Science and Technology and the MiEuropean Commission Interreg Ⅴ France-Wallonie-Vlaanderen Project'DepollutAirProgram Win2WalWallonia Region of Belgium and the National Key Research and Development Program Intergovernmental Technological Innovation

2022YFB3504000U20A201222229302222302152U22B6011B20002TCHARBONACTIF:2110120SUB/2021/IND493971/524448

2024

10.1093/nsr/nwae085

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年,卷(期)：2024.11(5)
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