Solid-phase synthesis of titanium-oxo clusters and their unprecedented catalytic performance in oxidative desulfurization of fuel oil†

IF 9.3 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Green Chemistry Pub Date : 2025-02-11 DOI:10.1039/D4GC05728G

Xinchun Liu, Yanpeng Yuan, Jiawei Fu, Yuqing Kong, Yinyong Sun, Xiaolin Li and Nan Qu

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引用次数: 0

Abstract

Titanium-oxo clusters (TOCs) have attracted much attention due to their diversity of structure and composition in recent years. Currently, such materials are synthesized by the solvothermal method. In this work, we report that a series of TOCs involving Ti₂₉KO₃₉(OEt)₃₈, Ti₆O₆(4-tbbz)₆(OⁱPr)₆, Ti₆O₆(abz)₆(OⁱPr)₆ and Ti₆O₆(4-tbbz)₁₀(OⁱPr)₂ have successfully been prepared by the solid-phase method. The structure of obtained materials was solved by the single-crystal X-ray diffraction technique. Furthermore, the performance of these TOCs was evaluated by the oxidative desulfurization (ODS) reactions of a model fuel oil. It was found that Ti₆O₆(4-tbbz)₁₀(OⁱPr)₂ exhibited unprecedented catalytic activity with a turnover frequency (TOF) of 729 h⁻¹ and mass activity of 1919 mmol h⁻¹ g⁻¹. The results from the experiments and theoretical calculations reveal that the Ti-hydroperoxo five-membered ring intermediates formed by the combination of binuclear titanium sites in Ti₆O₆(4-tbbz)₁₀(OⁱPr)₂ clusters with H₂O₂ play a key role in the oxidation of sulfur compounds. In addition, it is demonstrated that such TOCs can be utilized as precursors for the synthesis of Ti-MOFs.

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来源期刊

Green Chemistry 化学-化学综合

CiteScore

16.10

自引率

7.10%

发文量

677

审稿时长

1.4 months

期刊介绍： Green Chemistry is a journal that provides a unique forum for the publication of innovative research on the development of alternative green and sustainable technologies. The scope of Green Chemistry is based on the definition proposed by Anastas and Warner (Green Chemistry: Theory and Practice, P T Anastas and J C Warner, Oxford University Press, Oxford, 1998), which defines green chemistry as the utilisation of a set of principles that reduces or eliminates the use or generation of hazardous substances in the design, manufacture and application of chemical products. Green Chemistry aims to reduce the environmental impact of the chemical enterprise by developing a technology base that is inherently non-toxic to living things and the environment. The journal welcomes submissions on all aspects of research relating to this endeavor and publishes original and significant cutting-edge research that is likely to be of wide general appeal. For a work to be published, it must present a significant advance in green chemistry, including a comparison with existing methods and a demonstration of advantages over those methods.