坡缕石负载钌催化剂高效选择性氧化5-羟甲基糠醛制备2,5-二甲酰基呋喃

IF 5.3 2区 地球科学 Q2 CHEMISTRY, PHYSICAL Applied Clay Science Pub Date : 2023-09-15 DOI:10.1016/j.clay.2023.107023
Xuemin Zhong , Peng Yuan , Samahe Sadjadi , Dong Liu , Yanfu Wei
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引用次数: 3

摘要

5-羟甲基糠醛(HMF)氧化生成2,5 -二甲酰呋喃(DFF)是将可再生生物质转化为原料化学品的重要反应。在本研究中,我们开发了坡高岭土(Pal)负载的钌(Ru)催化剂,用于HMF的高效选择性氧化成DFF。以天然粘土矿物坡缕石为载体,实现了钌纳米颗粒的固定化和分散。以Ru(III)/Pal为催化剂,在110℃、10 bar O2的甲苯反应条件下,反应4.5 h后,HMF转化率为100%,DFF收率为98%,DFF选择性为98%。钌纳米颗粒与坡缕石协同作用,实现了催化剂优异的催化性能。钌金属活性位点促进了反应物或中间体的活化,加速了DFF的形成。此外,由于Ru(III)/Pal催化剂的粒径和钌种类不同,Ru(III)/Pal催化剂对HMF氧化成DFF的催化活性高于Ru(0)/Pal催化剂。坡缕石对Ru纳米颗粒的分散作用增强了催化活性。此外,坡齿石负载的Ru催化剂表现出良好的稳定性,并且可以连续重复使用至少5次,而不会显著降低其催化活性。
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Palygorskite-supported ruthenium catalysts for the efficient selective oxidation of 5-hydroxymethylfurfural to 2, 5-diformylfuran

The oxidation of 5-hydroxymethylfurfural (HMF) to 2, 5-diformylfuran (DFF) is an important reaction for the conversion of renewable biomass into feedstock chemicals. In this work, palygorskite (Pal)-supported ruthenium (Ru) catalysts were developed for the efficient selective oxidation of HMF to DFF. Using natural clay mineral palygorskite as the support enabled the immobilization and dispersion of Ru nanoparticles. A 100% HMF conversion, 98% DFF yield, and 98% DFF selectivity were obtained over Ru(III)/Pal catalyst after 4.5 h under the optimal reaction conditions at 110 °C and 10 bar of O2 in toluene. Ru nanoparticles and palygorskite synergistically achieve the excellent catalytic performance of the catalyst. The Ru metal active sites facilitate the activation of the reactants or intermediates, accelerating the formation of DFF. Furthermore, due to their different particle sizes and Ru species, the Ru(III)/Pal catalyst exhibits higher catalytic activity than the Ru(0)/Pal catalyst for the oxidation of HMF to DFF. The palygorskite-enhanced dispersion effect on Ru nanoparticles augments the catalytic activity. Moreover, the palygorskite-supported Ru catalyst showed good stability and was reused for at least five times consecutive cycles without significant loss of its catalytic activity.

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来源期刊
Applied Clay Science
Applied Clay Science 地学-矿物学
CiteScore
10.30
自引率
10.70%
发文量
289
审稿时长
39 days
期刊介绍: Applied Clay Science aims to be an international journal attracting high quality scientific papers on clays and clay minerals, including research papers, reviews, and technical notes. The journal covers typical subjects of Fundamental and Applied Clay Science such as: • Synthesis and purification • Structural, crystallographic and mineralogical properties of clays and clay minerals • Thermal properties of clays and clay minerals • Physico-chemical properties including i) surface and interface properties; ii) thermodynamic properties; iii) mechanical properties • Interaction with water, with polar and apolar molecules • Colloidal properties and rheology • Adsorption, Intercalation, Ionic exchange • Genesis and deposits of clay minerals • Geology and geochemistry of clays • Modification of clays and clay minerals properties by thermal and physical treatments • Modification by chemical treatments with organic and inorganic molecules(organoclays, pillared clays) • Modification by biological microorganisms. etc...
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