Designing a Ru/TiO2 Catalyst with Ru Flat Island for Hydrogenation of Aromatic Compounds

IF 13.1 1区 化学 Q1 CHEMISTRY, PHYSICAL
Jingrong Li, Ying Wang, Tingting Xiao, Xinluona Su, Haiyang Cheng* and Fengyu Zhao, 
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Abstract

Hydrogenation of aromatic molecules is a crucial industrial process that has been extensively employed in the synthesis of fundamental chemicals. In this work, the hydrogenation of bisphenol A (BPA) was studied over a kind of Ru/TiO2 catalyst. The catalytic activity of Ru/TiO2 was adjusted via manipulation of the metal–support interaction (MSI) by thermal treatment. The Ru/TiO2 exhibited a volcano-shaped dependence on calcination temperature, with the highest activity presented at 300 °C for the hydrogenation of BPA at mild conditions, produced 4,4′-isopropylidenedicyclohexanol (HBPA) with a yield of 99% at 80 °C, 4 MPa H2. The MSI could be adjusted by varying the calcination temperature, and flat Ru islands were formed at elevated temperatures, which facilitate the adsorption of the benzene ring of BPA. However, small-sized and electron-deficient Ru species prefer to adsorb H2. The Ru/TiO2-300 catalyst contains an appropriate composition of Ru nanoparticles and Ru flat islands, effectively balancing the competitive adsorption of H2 and BPA molecules, and thus exhibits high catalytic performance. Moreover, the Ru/TiO2-300 catalyst is highly efficient for a variety of aromatic compounds, producing the desired products selectively under mild conditions. Furthermore, it presented high stability without any loss in activity after 10 recycles. This work developed an efficient catalyst for the hydrogenation of aromatic compounds, and the insights into the catalytic mechanism will provide useful information to researchers in wide fields.

Abstract Image

Abstract Image

带Ru平岛的Ru/TiO2催化剂的设计及其在芳香化合物加氢中的应用
芳香族分子的氢化反应是一个重要的工业过程,已广泛应用于基础化学品的合成。本文研究了双酚A (BPA)在Ru/TiO2催化剂上的加氢反应。通过热处理金属-载体相互作用(MSI)调节Ru/TiO2的催化活性。Ru/TiO2对煅烧温度呈火山状的依赖性,在300℃温和条件下对BPA的加氢反应活性最高,在80℃、4 MPa H2条件下生成4,4′-异丙基二环己醇(HBPA),产率达99%。MSI可以通过改变煅烧温度来调节,在高温下形成扁平的Ru岛,有利于BPA对苯环的吸附。然而,小尺寸和缺电子的Ru更倾向于吸附H2。Ru/TiO2-300催化剂含有适当的Ru纳米颗粒和Ru扁平岛组成,有效平衡H2和BPA分子的竞争吸附,从而表现出较高的催化性能。此外,Ru/TiO2-300催化剂对多种芳香族化合物具有很高的催化效率,在温和的条件下选择性地生成所需的产物。此外,它具有高稳定性,在10次循环后没有任何活性损失。本研究开发了一种高效的芳香族化合物加氢催化剂,对其催化机理的深入研究将为广大领域的研究人员提供有用的信息。
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来源期刊
ACS Catalysis
ACS Catalysis CHEMISTRY, PHYSICAL-
CiteScore
20.80
自引率
6.20%
发文量
1253
审稿时长
1.5 months
期刊介绍: ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.
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