xPd100-xCu/UiO-66-NH2 catalysts for selective 5-hydroxymethylfurfural reduction

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED Microporous and Mesoporous Materials Pub Date : 2024-11-22 DOI:10.1016/j.micromeso.2024.113432

Denis P. Morilov , Konstantin L. Timofeev , Aleksandra G. Golubovskaya , Olga A. Stonkus , Tamara S. Kharlamova

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Abstract

The present work is focused on a strategy to regulate the properties of monometallic Pd and bimetallic PdCu catalysts for selective 5-hydroxymethylfurfural (HMF) reduction via the interaction with the functional groups of the NH₂-modified Zr-based metal-organic frameworks (Zr-MOFs). xPd100-xCu/UiO-66-NH₂-X catalysts with different fractions of amino terephthalate linkers as well as Pd and Cu metals (x and 100-x, respectively) in bimetallic composition are prepared with impregnation reduction technique. The obtained samples are studied using a complex of methods, including XRD, low-temperature nitrogen adsorption, IR spectroscopy, and CO pulsed chemisorption. The effect of NH₂ groups on the adsorption properties of the Zr-MOFs towards Pd and Cu precursors and on Pd and PdCu species formation in xPd100-xCu/UiO-66-NH₂-X catalysts is considered. The formation of active particles at various stages of catalyst formation is studied in detail. 50 % fraction of NH₂ linkers is found optimal for the formation of active and selective mono- and bimetallic CuPd catalysts, while 100 % fraction significantly reduces the activity of the samples due to the strong interaction of active Pd species with the support and does not allow the formation of bimetallic catalysts.

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用于选择性还原 5-羟甲基糠醛的 xPd100-xCu/UiO-66-NH2 催化剂

本研究的重点是通过与 NH2 改性 Zr 基金属有机框架（Zr-MOFs）官能团的相互作用，调节用于选择性还原 5-羟甲基糠醛（HMF）的单金属 Pd 和双金属 PdCu 催化剂的性能。采用浸渍还原技术制备了 xPd100-xCu/UiO-66-NH2-X 催化剂，其中含有不同比例的对苯二甲酸氨基连接体以及双金属成分中的钯和铜金属（分别为 x 和 100-x）。研究采用了多种方法，包括 XRD、低温氮吸附、红外光谱和 CO 脉冲化学吸附。研究考虑了 NH2 基团对 Zr-MOFs 对 Pd 和 Cu 前驱体的吸附特性以及对 xPd100-xCu/UiO-66-NH2-X 催化剂中 Pd 和 PdCu 物种形成的影响。详细研究了催化剂形成过程中各个阶段活性颗粒的形成。研究发现，50% 的 NH2 链接剂是形成活性和选择性单金属和双金属铜钯催化剂的最佳成分，而 100% 的 NH2 链接剂会显著降低样品的活性，因为活性钯物种会与载体发生强烈的相互作用，并且无法形成双金属催化剂。

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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.