Enhanced Lewis acidity on modified H-ZSM-5 catalysed 5-hydroxymethylfurfural oxidation in aqueous solvent

IF 3.9 2区 化学 Q2 CHEMISTRY, PHYSICAL Molecular Catalysis Pub Date : 2024-10-17 DOI:10.1016/j.mcat.2024.114610
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Abstract

The primary focus of the present study is to develop a zeolite-based catalyst that enhances Lewis acidity for catalysing 5-hydroxymethylfurfural (HMF) oxidation. The study modifies the parent H-ZSM-5 (H-Z) via desilication followed by Ru impregnation. The results show that RuZS90 (Ru impregnated on desilicated H-Z for 90 min) exhibits higher catalytic activity for the HMF oxidation than Ru impregnated on parent H-Z. NH3-temperature programmed desorption (TPD) results indicate that RuZS90 possesses more than 2.6 and 2.3 times higher total acidity than H-Z and RuH-Z, contributing to the higher catalytic activity. A poisoning study with potassium thiocyanate (KSCN), which passivates Lewis acidic sites, suggests that RuZS90 yields no considerable oxidised furanic products, confirming the crucial role of Lewis acidic sites. The NH3-DRIFT study further corroborates that RuZS90 contains more enhanced Lewis acidic sites than the parent H-Z, playing a vital role in the oxidation of HMF.

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改性 H-ZSM-5 在水性溶剂中催化 5- 羟甲基糠醛氧化时增强的路易斯酸性
本研究的主要重点是开发一种沸石基催化剂,以提高催化 5-羟甲基糠醛(HMF)氧化的路易斯酸度。研究通过脱硅后浸渍 Ru 的方法对母体 H-ZSM-5 (H-Z) 进行改性。结果表明,与浸渍在母体 H-Z 上的 Ru 相比,浸渍在脱硅 H-Z 上 90 分钟的 RuZS90 对 HMF 氧化具有更高的催化活性。NH3-温度编程解吸(TPD)结果表明,RuZS90 的总酸度分别是 H-Z 和 RuH-Z 的 2.6 倍和 2.3 倍,这也是其催化活性更高的原因。硫氰酸钾(KSCN)会钝化路易斯酸位点,而中毒研究表明,RuZS90 不会产生大量氧化呋喃产物,这证实了路易斯酸位点的关键作用。NH3-DRIFT 研究进一步证实,与母体 H-Z 相比,RuZS90 含有更多增强的路易斯酸位点,在 HMF 的氧化过程中发挥了重要作用。
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来源期刊
Molecular Catalysis
Molecular Catalysis Chemical Engineering-Process Chemistry and Technology
CiteScore
6.90
自引率
10.90%
发文量
700
审稿时长
40 days
期刊介绍: Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are: Heterogeneous catalysis including immobilized molecular catalysts Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis Photo- and electrochemistry Theoretical aspects of catalysis analyzed by computational methods
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