Magnetic Ru nanocatalysts for green solvent-free oxidation reactions of aromatic alcohols

IF 2.1 3区化学 Q3 CHEMISTRY, INORGANIC & NUCLEAR Journal of Organometallic Chemistry Pub Date : 2024-09-03 DOI:10.1016/j.jorganchem.2024.123354

Haijiao Jia , Yuchen Cui , Xiaoqian Yuan , Yanmei Xu , Youxin Li

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Abstract

A kind of magnetic hybrid organic-inorganic nanoparticles containing Ru metal (Fe₃O₄@SiO₂-FPBA-Ru) was prepared. It was spherical with the characteristic lattice fringe of ruthenium atom. The size was in the range of 5–15 nm and it contained 0.30 mmol/g Ru. Its saturation magnetization value was 15.95 emu/g, which could be easily and efficiently recovered from solution through an external magnet. It was also stable below 240°C and hot filtration experiment proved Ru wasn't leaked from Fe₃O₄@SiO₂-FPBA-Ru in 70°C oxidation reaction. It could be recovered and reused at least 7 cycles. The low amount of Fe₃O₄@SiO₂-FPBA-Ru (75 mmol%) could convert the 99 % of 1-phenylethanol to acetophenone under solvent-free system, which verified its green and environment-friendly properties. The yield was exceed that of homogeneous (RuCl₃, 85 %). Beside this, the TON (5181), TOF (7430 h⁻¹) in oxidation of 1-phenylethanol and high conversion yields for a series of oxidation reactions of aromatic secondary alcohols proved the high catalytic ability of Fe₃O₄@SiO₂-FPBA-Ru. These laid a foundation for its industrial applications.

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用于芳香醇绿色无溶剂氧化反应的磁性纳米 Ru 催化剂

制备了一种含金属 Ru 的磁性有机无机杂化纳米粒子（Fe3O4@SiO2-FPBA-Ru）。它呈球形，带有钌原子特有的晶格边缘。其尺寸范围为 5-15 nm，含钌量为 0.30 mmol/g。它的饱和磁化值为 15.95 emu/g，可通过外置磁铁轻松有效地从溶液中回收。它在 240°C 以下也很稳定，热过滤实验证明，在 70°C 的氧化反应中，Fe3O4@SiO2-FPBA-Ru 中的 Ru 没有泄漏。它可以回收并重复使用至少 7 次。低用量的 Fe3O4@SiO2-FPBA-Ru（75 mmol%）可在无溶剂体系中将 99% 的 1-苯基乙醇转化为苯乙酮，验证了其绿色环保的特性。收率超过了均相物（RuCl3，85%）。此外，Fe3O4@SiO2-FPBA-Ru 在氧化 1-苯基乙醇时的 TON（5181）和 TOF（7430 h-1）以及在一系列芳香族仲醇氧化反应中的高转化率也证明了它的高催化能力。这些都为其工业应用奠定了基础。

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来源期刊

Journal of Organometallic Chemistry 化学-无机化学与核化学

CiteScore

4.40

自引率

8.70%

发文量

221

审稿时长

36 days

期刊介绍： The Journal of Organometallic Chemistry targets original papers dealing with theoretical aspects, structural chemistry, synthesis, physical and chemical properties (including reaction mechanisms), and practical applications of organometallic compounds. Organometallic compounds are defined as compounds that contain metal - carbon bonds. The term metal includes all alkali and alkaline earth metals, all transition metals and the lanthanides and actinides in the Periodic Table. Metalloids including the elements in Group 13 and the heavier members of the Groups 14 - 16 are also included. The term chemistry includes syntheses, characterizations and reaction chemistry of all such compounds. Research reports based on use of organometallic complexes in bioorganometallic chemistry, medicine, material sciences, homogeneous catalysis and energy conversion are also welcome. The scope of the journal has been enlarged to encompass important research on organometallic complexes in bioorganometallic chemistry and material sciences, and of heavier main group elements in organometallic chemistry. The journal also publishes review articles, short communications and notes.