Green catalytic oxidation of ethylbenzene to acetophenone over modified TS-1 zeolite supported cobalt oxide

IF 4.8 3区 材料科学 Q1 CHEMISTRY, APPLIED
Zhimei Song , Jinhong Li , Kaikai Cui , Mei Han , Dan Fang , Chang Cai , Nan Zhao , Jinge Wang , Lidong Chen
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Abstract

The development of catalysts and processes with high activity, good selectivity and easy reproducibility and regeneration is the core of the solution for the oxidation of ethylbenzene to acetophenone. In this paper, the catalyst of cobalt metal oxide supported on TS-1 zeolite co-modified by alkali treatment and titanium silicon composite oxide was prepared. The catalysts were characterized by XRD, Raman, N2 adsorption-desorption, SEM, TEM, XPS, FT-IR and UV–vis techniques to establish the correlation between physical and chemical properties and catalytic performance. Among the prepared catalysts, SiO2 and TiO2 co-coated TS-1 supported 3.75 wt % Co3O4 catalyst showed better oxidation activity. Under the optimized reaction conditions: T = 80 °C, t = 8 h, mcat = 0.03 g, nEB: nHAC: nKBr: nH2O2 = 1 : 21: 0.1 : 16, the conversion of ethylbenzene was as high as 86.7 % and the selectivity of acetophenone was 85.6 %. After repeated tests, it showed good cycle and regeneration reaction performance. The high activity of this catalyst is attributed to the synergistic effect of cobalt oxide and TS-1 zeolite, and the mesoporous structure of titanium-silicon composite oxide is conducive to the adsorption and diffusion of reactants, intermediates and products.

Abstract Image

改性 TS-1 沸石支撑氧化钴催化乙苯氧化为苯乙酮的绿色催化反应
开发活性高、选择性好、易于重现和再生的催化剂和工艺是解决乙苯氧化为苯乙酮问题的核心。本文制备了以碱处理和钛硅复合氧化物共同改性的 TS-1 沸石为载体的金属氧化钴催化剂。通过 XRD、拉曼、N2 吸附-解吸、扫描电镜、TEM、XPS、傅立叶变换红外光谱和紫外可见光等技术对催化剂进行了表征,以确定催化剂的物理和化学性质与催化性能之间的相关性。在制备的催化剂中,SiO2 和 TiO2 共包覆的 TS-1 支承 3.75 wt % Co3O4 催化剂表现出更好的氧化活性。在优化的反应条件下T = 80 °C,t = 8 h,mcat = 0.03 g,nEB: nHAC: nKBr: nH2O2 = 1 : 21: 0.1 :16 时,乙苯的转化率高达 86.7%,对苯乙酮的选择性为 85.6%。经过反复试验,该催化剂显示出良好的循环和再生反应性能。该催化剂的高活性得益于氧化钴和 TS-1 沸石的协同作用,钛硅复合氧化物的介孔结构有利于反应物、中间产物和产物的吸附和扩散。
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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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