Tuning the selectivity of catalytic hydrogenation of fumaric acid with supercritical CO2

IF 3.4 3区工程技术 Q2 CHEMISTRY, PHYSICAL

Journal of Supercritical Fluids Pub Date : 2024-10-09 DOI:10.1016/j.supflu.2024.106424

Adolfo L. Figueredo , Carolina S. Costa , Maitê L. Gothe , Reinaldo C. Bazito , Pedro Vidinha , Camila G. Pereira

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Abstract

The catalytic hydrogenation of fumaric acid, a prominent bioplatform molecule, was evaluated over PdRe/SiO₂ within a variety of reaction media compositions comprising methanol, water, supercritical CO₂, and their assorted combinations with H₂, across a range of temperature and pressure regimes. Meticulous manipulation of the reaction media composition facilitated the precise modulation of catalytic activity to favor specific hydrogenation products. For instance, within a water-saturated supercritical CO₂ medium, γ-butyrolactone exhibited a noteworthy 89 % selectivity at 188°C under 250 bar total pressure, whereas in the methanol-containing supercritical CO₂ system, hydrogenation displayed a remarkable 91 % selectivity towards tetrahydrofuran at 175°C and 250 bar. This investigation underscores the multifaceted influence of CO₂, extending beyond its pressure-derived effects - it functions as a solvent, selectively favoring catalytic pathways and enhancing product selectivity.

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调整超临界二氧化碳催化富马酸加氢的选择性

在各种反应介质组成（包括甲醇、水、超临界 CO2 以及它们与 H2 的各种组合）中，通过 PdRe/SiO2 在一定温度和压力范围内对富马酸（一种重要的生物平台分子）的催化氢化进行了评估。对反应介质成分的精心操作有助于精确调节催化活性，以获得特定的氢化产物。例如，在水饱和的超临界二氧化碳介质中，γ-丁内酯在 188 摄氏度、总压 250 巴的条件下表现出 89% 的选择性，而在含甲醇的超临界二氧化碳体系中，氢化反应在 175 摄氏度、总压 250 巴的条件下对四氢呋喃表现出 91% 的选择性。这项研究强调了二氧化碳的多方面影响，它不仅具有压力效应，还具有溶剂功能，可选择性地促进催化途径并提高产品选择性。

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

Journal of Supercritical Fluids 工程技术-工程：化工

CiteScore

7.60

自引率

10.30%

发文量

236

审稿时长

56 days

期刊介绍： The Journal of Supercritical Fluids is an international journal devoted to the fundamental and applied aspects of supercritical fluids and processes. Its aim is to provide a focused platform for academic and industrial researchers to report their findings and to have ready access to the advances in this rapidly growing field. Its coverage is multidisciplinary and includes both basic and applied topics. Thermodynamics and phase equilibria, reaction kinetics and rate processes, thermal and transport properties, and all topics related to processing such as separations (extraction, fractionation, purification, chromatography) nucleation and impregnation are within the scope. Accounts of specific engineering applications such as those encountered in food, fuel, natural products, minerals, pharmaceuticals and polymer industries are included. Topics related to high pressure equipment design, analytical techniques, sensors, and process control methodologies are also within the scope of the journal.