Engineering surface framework TiO_(6) single sites for unprecedented deep oxidative desulfurization  

作　　者：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 

机构地区：[1]Laboratory of Living Materials at the State Key Laboratory of Advanced Technology for Materials Synthesis and Processing,Wuhan University of Technology,Wuhan 430070,China [2]Nanostructure Research Center,Wuhan University of Technology,Wuhan 430070,China [3]School of Chemistry,Chemical Engineering and Life Science,Wuhan University of Technology,Wuhan 430070,China [4]Laboratory of Inorganic Materials Chemistry,University of Namur,Namur B-5000,Belgium

出　　处：《National Science Review》2024年第5期296-307,共12页国家科学评论（英文版）

基　　金：supported by the National Key R&D Program of China(2022YFB3504000);the National Natural Science Foundation of China(U20A20122,22293022,22302152 and U22B6011);the Program of Introducing Talents of Discipline to Universities-Plan 111(B20002)from the Ministry of Science and Technology and the Ministry of Education of China.This work was also supported by the European Commission Interreg V France-Wallonie-Vlaanderen Project‘DepollutAir’,the Program Win2Wal(TCHARBONACTIF:2110120);the Wallonia Region of Belgium and the National Key R&D Program Intergovernmental Technological Innovation Special Cooperation Project Wallonia-Brussels/China(MOST)(SUB/2021/IND493971/524448).

摘　　要：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(TiO_(6))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 TiO_(6) active single sites at the mesoporous surface has been developed.Such surface framework TiO_(6) 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.

关 键 词：electrostatic interactions framework hexa-coordinated Ti site oxidative desulfurization mesoporous materials SELF-ASSEMBLY 

分 类 号：TQ426[化学工程]