Tailoring the preparation of USY zeolite with uniform mesoporosity for improved catalytic activity in phenol/isopropanol alkylation

IF 4.8 3区 材料科学 Q1 CHEMISTRY, APPLIED
C. Molina , A. Abdrassilova , M.I. Ávila , M.M. Alonso-Doncel , J. Cueto , G. Gómez-Pozuelo , L. Briones , J.A. Botas , D.P. Serrano , A. Peral , J.M. Escola
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Abstract

The preparation of hierarchical USY zeolite, exhibiting uniform mesoporosity and high Si/Al atomic ratio (48–52), has been investigated by means of a surfactant/ammonia post-treatment applied to a commercial USY sample. The procedure involved the use of temperatures within 40–135 °C, a low ammonia concentration solution (0.05 N) and hydrothermal synthesis times of 20 h. When working at 40–80 °C, the obtained USY samples exhibit enhanced intraparticular mesoporosity (324–418 m2 g−1), showing increasingly uniform mesopores around 4.0 nm, while holding a remarkable zeolitic microporosity (413–363 m2 g−1). In contrast, higher temperatures resulted in a steady abatement of crystalline zeolitic domains, with a total collapse of the zeolite structure at 135 °C. These hierarchical USY materials were tested in the alkylation of phenol with isopropanol, wherein one of the obtained products, e.g. 2,6-diisopropylphenol (Propofol), is the most important intravenous anaesthetic in the market. Interestingly, the generation of the uniform mesoporosity in USY samples led to an enhancement of both the phenol conversion and the selectivity towards C-alkylation products. Thus, the sample treated at 60 °C (USY-60) gave rise to the highest selectivity towards C-alkylation products (84 %) and poly-alkylphenols formation (72 %), with an encouraging selectivity towards 2,6-diisopropylphenol (43 %).

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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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