Promoted catalytic performance from furfural to isopropyl levulinate by Zr loaded on defective nanosponge zeolites

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED Microporous and Mesoporous Materials Pub Date : 2024-02-21 DOI:10.1016/j.micromeso.2024.113061

Longbin Deng , Shuaishuai Zhou , Congzhen Qiao , Xin Yu , Yutong Wang , Yajie Tian

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Abstract

Production of alkyl levulinate (AL) from bio-derived furfural (FUR) is environmental-friendly and sustainable. During such process, bifunctional Zr/zeolite catalyst has been demonstrated highly efficient, in which synergism of metal-zeolite and porous structure of catalysts play important roles. In this work, a defective nanoaponge ZSM-5 zeolite loading Zr catalyst is prepared for conversion of FUR to produce isopropyl levulinate (IPL). The defective nanosponge zeolite is hydrothermally synthesized sequenced by acid treatment (NP-A). Then the Zr species were introduced in the as-synthesized NP-A zeolite by impregnation and calcination (Zr/NP-A). The NP zeolite composed of nano-crystalline aggregates deliver hierarchical pores, which promotes adsorption and activation of isopropanol. And the generation of framework Zr accelerates the adsorption of FUR. The as-synthesized Zr/NP-A catalyst give IPL yield up of 77.8 mol% after 3 h reaction at 200 °C with turnover frequency of 8.3 mmol g⁻¹ h⁻¹, which provides an efficient catalyst for production of AL through bio-route.

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缺陷纳米海绵沸石上负载的锆促进了从糠醛到乙酰丙酸异丙酯的催化性能

利用生物衍生糠醛（FUR）生产乙酰丙酸烷基酯（AL）既环保又可持续。在此过程中，双功能锆/沸石催化剂被证明具有很高的效率，其中金属-沸石的协同作用和催化剂的多孔结构发挥了重要作用。在这项工作中，制备了一种缺陷纳米皂基 ZSM-5 沸石负载 Zr 催化剂，用于将 FUR 转化为生产乙酰丙酸异丙酯（IPL）。缺陷纳米海绵沸石是通过酸处理（NP-A）水热合成的。然后通过浸渍和煅烧（Zr/NP-A）在合成的 NP-A 沸石中引入 Zr 物种。由纳米晶体聚集体组成的 NP 沸石提供了分层孔隙，促进了异丙醇的吸附和活化。框架 Zr 的生成加速了对 FUR 的吸附。所合成的 Zr/NP-A 催化剂在 200 °C 下反应 3 小时后，IPL 产率达到 77.8 摩尔%，周转频率为 8.3 毫摩尔/克-1 小时-1，为通过生物途径生产 AL 提供了一种高效催化剂。

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来源期刊

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.