Bifunctional Rh/Al-SBA-15 catalysed cascade hydroformylation and hydroxyalkylation of alkenes to fuel precursors†

IF 4.4 3区化学 Q2 CHEMISTRY, PHYSICAL

Catalysis Science & Technology Pub Date : 2025-04-15 DOI:10.1039/d5cy00171d

Krishnan Ravi , Hanuman Kachgunde , Venkata D. B. C. Dasireddy , Jim Mensah , Adam F. Lee , Ankush V. Biradar , Karen Wilson

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Abstract

Decarbonisation of hard-to-abate liquid transport fuels, notably used in the aviation and shipping sectors, requires new catalytic routes to valorise waste feedstocks. Here we report a bifunctional Rh/Al-SBA-15 catalyst for the one-pot, two step cascade hydroformylation of 1-alkenes with CO/H₂ to form linear and branched aldehydes, and their subsequent hydroxyalkylation (HAA) with 2-methylfuran to form oxygenated jet fuel precursors. A strong synergy between Rh and Al-SBA-15 is observed for hydroformylation, with the bifunctional catalyst significantly more active than Rh/SBA-15 for the first step of the cascade. Superior yields of desired HAA products are observed over Rh/Al-SBA-15 relative to a physical mixture of Rh/SBA-15 and Al-SBA-15. Under syngas (CO/H₂) at 30 bar and 80 °C, alkenes undergo Rh catalysed hydroformylation to aldehydes, and in a subsequent step under N₂, HAA of aldehydes over the solid acid sites of Al-SBA-15 gives an overall ∼60% yield of fuel range precursors.

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双功能Rh/Al-SBA-15催化级联氢甲酰化和羟烷基化烯烃燃料前体†

难以减排的液体运输燃料的脱碳，特别是在航空和航运部门使用的燃料，需要新的催化途径来使废物原料增值。本文报道了一种双功能的Rh/Al-SBA-15催化剂，用于1-烯烃与CO/H2的一锅两步级联氢甲酰化反应，形成线性和支化醛，然后与2-甲基呋喃进行羟基烷基化反应，形成含氧的喷气燃料前体。Rh和Al-SBA-15在氢甲酰化过程中具有很强的协同作用，在级联反应的第一步，双功能催化剂的活性明显高于Rh/SBA-15。相对于Rh/Al-SBA-15和Al-SBA-15的物理混合物，在Rh/Al-SBA-15上观察到所需的HAA产物的产率更高。在30 bar和80°C的合成气（CO/H2）下，烯烃经过Rh催化的氢甲酰化反应生成醛，在N2下的后续步骤中，醛在Al-SBA-15的固体酸位点上的HAA得到燃料范围前体的总体产率为60%。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Catalysis Science & Technology CHEMISTRY, PHYSICAL-

CiteScore

8.70

自引率

6.00%

发文量

587

审稿时长

1.5 months

期刊介绍： A multidisciplinary journal focusing on cutting edge research across all fundamental science and technological aspects of catalysis. Editor-in-chief: Bert Weckhuysen Impact factor: 5.0 Time to first decision (peer reviewed only): 31 days