Solvent-free room-temperature oxidative desulfurization enabled by superhydrophobic Mo/SBA-15 catalysts

IF 4.7 3区 材料科学 Q1 CHEMISTRY, APPLIED
Robert E. Mustakimov, Nina V. Arzyaeva, Gleb V. Nikolaevich, Matvei D. Sukmanov, Anna V. Vutolkina, Argam V. Akopyan
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引用次数: 0

Abstract

Developing low-energy and waste-minimizing desulfurization technologies is essential for cleaner fuel production. Here, we report superhydrophobic molybdenum catalysts based on SBA-15, prepared by grafting octyltriethoxysilane (up to 20 mass %) while preserving the mesoporous framework. The hydrophobic surface significantly improves interfacial mass transfer and suppresses catalyst deactivation by excess aqueous H2O2 adsorption, enabling oxidative desulfurization (ODS) at room temperature without any organic co-solvents. Characterization (elemental analysis, TGA, N2 physisorption, FTIR, SEM/TEM, contact-angle measurements) confirms successful modification and enhanced stability.
The catalyst 20oct/Mo/SBA under optimized solvent-free conditions allows to achieve 99 % conversion for a high-sulfur model fuel (8000 ppmS) at 2 mass % dosage, representing the first demonstration of complete ODS of such sulfur-rich feed at ambient temperature. The catalyst also showed sufficient activity to oxidize straight-run diesel under mild, co-solvent-free conditions. These results establish hydrophobic Mo/SBA-15 catalysts as an energy-efficient and environmentally benign platform for deep oxidative desulfurization.

Abstract Image

超疏水Mo/SBA-15催化剂实现无溶剂室温氧化脱硫
开发低能耗和减少废物的脱硫技术对清洁燃料生产至关重要。在这里,我们报道了基于SBA-15的超疏水钼催化剂,该催化剂通过接枝辛基三乙基氧基硅烷(高达20%质量%)制备而成,同时保留了介孔框架。疏水表面显著改善了界面传质,抑制了过量H2O2吸附引起的催化剂失活,实现了室温氧化脱硫(ODS),无需任何有机共溶剂。表征(元素分析,TGA, N2物理吸附,FTIR, SEM/TEM,接触角测量)证实了成功的改性和增强的稳定性。催化剂20oct/Mo/SBA在优化的无溶剂条件下,可以在2质量%的用量下对高硫模型燃料(8000 ppmS)实现99%的转化率,这是这种富硫饲料在室温下完全ODS的首次演示。该催化剂在温和、无助溶剂的条件下也表现出足够的氧化直馏柴油的活性。这些结果表明,疏水Mo/SBA-15催化剂是一种节能环保的深度氧化脱硫平台。
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来源期刊
Microporous and Mesoporous Materials
Microporous and Mesoporous Materials 化学-材料科学:综合
CiteScore
10.70
自引率
5.80%
发文量
649
审稿时长
26 days
期刊介绍: Microporous and Mesoporous Materials covers novel and significant aspects of porous solids classified as either microporous (pore size up to 2 nm) or mesoporous (pore size 2 to 50 nm). The porosity should have a specific impact on the material properties or application. Typical examples are zeolites and zeolite-like materials, pillared materials, clathrasils and clathrates, carbon molecular sieves, ordered mesoporous materials, organic/inorganic porous hybrid materials, or porous metal oxides. Both natural and synthetic porous materials are within the scope of the journal. Topics which are particularly of interest include: All aspects of natural microporous and mesoporous solids The synthesis of crystalline or amorphous porous materials The physico-chemical characterization of microporous and mesoporous solids, especially spectroscopic and microscopic The modification of microporous and mesoporous solids, for example by ion exchange or solid-state reactions All topics related to diffusion of mobile species in the pores of microporous and mesoporous materials Adsorption (and other separation techniques) using microporous or mesoporous adsorbents Catalysis by microporous and mesoporous materials Host/guest interactions Theoretical chemistry and modelling of host/guest interactions All topics related to the application of microporous and mesoporous materials in industrial catalysis, separation technology, environmental protection, electrochemistry, membranes, sensors, optical devices, etc.
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