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

Rahul Gautam, Neeraj Sharma, Kanika Saini, Shunmugavel Saravanamurugan

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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 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