在纳米海绵 MFI 沸石上支撑的磷酸锆催化下,通过催化转移加氢从糠醛制备乙酰丙酸异丙酯

IF 4.8 3区 材料科学 Q1 CHEMISTRY, APPLIED Microporous and Mesoporous Materials Pub Date : 2024-06-20 DOI:10.1016/j.micromeso.2024.113226
Tiantian Wang , Longbin Deng , Shuaishuai Zhou , Zhenheng Diao , Hongyan Wang , Congzhen Qiao , Yajie Tian
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引用次数: 0

摘要

乙酰丙酸烷基酯是一种从生物质中提取的高价值化学品。本文制备了一种纳米海绵 ZSM-5 支承磷酸锆(ZrPO/NPZ)催化剂,并将其用于以异丙醇为 H-载体催化糠醛(FUR)转移加氢生成左旋丙酸异丙酯(IPL)。ZrPO 种类提供了路易斯酸位点,ZSM-5 沸石还提供了额外的布伦斯特酸位点。使用具有暴露表面积的分层 ZSM-5 作为支撑,ZrPO 活性物质的分散性增加,从而促进了 FUR 的吸附和转化,生成 2-(异丙氧基甲基)呋喃(IPMF)。沸石上适度的布氏酸位点促进了异丙醇的吸附和活化,从而提高了中间 IPMF 的转化率,并形成了 IPL。此外,随着所制备催化剂中 P/Zr 比率的增加,发现 Brønsted/Lewis 的比例有所提高,这对 FUR 的转化不利。P/Zr 为 1 的优化 ZrPO/NPZ 催化剂具有最佳的催化性能,在 200 °C 下反应 3 小时后,其 IPL 产率为 ∼69 wt%(TOF 为 6.98 mmol g-1 h-1),为从 FUR 生产 IPL 提供了一种重要的催化剂。
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Production of isopropyl levulinate from furfural catalyzed by zirconium phosphate supported on nanosponge MFI zeolite through catalytic transfer hydrogenation

Alkyl levulinate is a kind of high value chemicals derived from biomass. Here, a nanosponge ZSM-5 supporting zirconium phosphate (ZrPO/NPZ) catalyst is prepared and used for catalytic transfer hydrogenation of furfural (FUR) to produce isopropyl levulinate (IPL) using isopropanol as H-donor. ZrPO specie provides Lewis acid sites together with additional Brønsted acid sites by ZSM-5 zeolite. Using the hierarchical ZSM-5 with exposed surface area as support, the dispersion of ZrPO active species increases, which facilitates the adsorption and conversion of FUR with the generation of 2-(isopropoxymethyl)furan (IPMF). The moderate Brønsted acid sites by zeolite promote the adsorption and activation of isopropanol, thus increasing the conversion rates of intermediate IPMF with formation of IPL. Furthermore, improved proportions of Brønsted/Lewis was detected with the increase of P/Zr ratios in the prepared catalysts, which is adverse for conversion of FUR. The optimized ZrPO/NPZ catalyst with P/Zr of 1 gives the best catalytic performance with IPL yield of ∼69 wt% after 3 h reaction at 200 °C (TOF of 6.98 mmol g−1 h−1), which provides an essential catalyst to produce IPL from FUR.

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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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