Room temperature aerobic oxidation of thiophenes catalyzed by silver 5-atoms clusters

IF 5.3 2区 化学 Q1 CHEMISTRY, APPLIED Catalysis Today Pub Date : 2025-04-01 Epub Date: 2025-01-03 DOI:10.1016/j.cattod.2025.115184
K. Jori , M. Mizrahi , L.J. Giovanetti , J.M. Ramallo-López , D. Buceta , I.R. Arias , J.M. Blanco Trillo , M.A.López Quintela , F.G. Requejo
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Abstract

To produce an impact in the reduction of sulfur derivatives on the environment it is essential to further eliminate the sulfur content in fuels. Although oxidative desulfurization using low temperatures and atmospheric pressure is a very appealing alternative to the currently used, and highly energy demanding, hydrodesulfurization method, it suffers from the use of high amounts of oxidizing agents such as NO2, H2O2, and tert-butyl-hydro-peroxide, especially for the oxidation of highly oxidation-resistant compounds as thiophens. Using X-ray absorption near edge structure (XANES) spectroscopy, we show that Ag clusters of 5 atoms (Ag5) have high catalytic activities to achieve the complete oxidation (S−2 to S+6) of highly oxidation-resistant compounds, such as dibenzothiophene, tetraphenyl thiophene and asphaltene, under ambient conditions in a simple and efficient process. Additionally, an analysis regarding the effect of Ag5 concentration for possible oxidation routes for dibenzothiophene is shown. These results can open a new avenue to face the challenge of reducing the presence of sulfur compounds in fuels using simple and green approaches.
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银5原子团簇催化噻吩的室温好氧氧化研究
为了减少硫衍生物对环境的影响,必须进一步消除燃料中的硫含量。虽然低温常压氧化脱硫是目前使用的高能耗加氢脱硫方法的一种非常有吸引力的替代方法,但它需要使用大量的氧化剂,如NO2, H2O2和叔丁基过氧化氢,特别是对于高抗氧化性化合物如硫芬的氧化。利用x射线吸收近边结构(XANES)光谱,我们发现5个原子的银簇(Ag5)具有很高的催化活性,可以在环境条件下以简单高效的过程实现高抗氧化化合物,如二苯并噻吩、四苯基噻吩和沥青烯的完全氧化(S−2到S+6)。此外,还分析了Ag5浓度对二苯并噻吩可能氧化途径的影响。这些结果可以开辟一条新的途径,以面对使用简单和绿色的方法减少燃料中硫化合物的存在的挑战。
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来源期刊
Catalysis Today
Catalysis Today 化学-工程:化工
CiteScore
11.50
自引率
3.80%
发文量
573
审稿时长
2.9 months
期刊介绍: Catalysis Today focuses on the rapid publication of original invited papers devoted to currently important topics in catalysis and related subjects. The journal only publishes special issues (Proposing a Catalysis Today Special Issue), each of which is supervised by Guest Editors who recruit individual papers and oversee the peer review process. Catalysis Today offers researchers in the field of catalysis in-depth overviews of topical issues. Both fundamental and applied aspects of catalysis are covered. Subjects such as catalysis of immobilized organometallic and biocatalytic systems are welcome. Subjects related to catalysis such as experimental techniques, adsorption, process technology, synthesis, in situ characterization, computational, theoretical modeling, imaging and others are included if there is a clear relationship to catalysis.
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