Cu-Based Catalysts for the One-Pot Condensation–Hydrogenation of Cyclopentanone to Produce Valuable SAF Precursors

IF 3.9 3区 化学 Q2 CHEMISTRY, PHYSICAL ChemCatChem Pub Date : 2024-11-04 DOI:10.1002/cctc.202401586
Dr. Nicola Schiaroli, Dr. Lorenzo Scaglione, Dr. Riccardo Mandioni, Dr. Francesca Foschi, Prof. Sandro Recchia, Prof. Carlo Lucarelli
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Abstract

A process combining aldol condensation and hydrogenation of bio-based cyclopentanone (CPO) in a one-pot reaction is proposed. Cu-based bifunctional catalysts obtained from hydrotalcite-type precursors were found highly active in mild reaction conditions (i.e., 130–170 °C), producing valuable bicyclic (C10) and tricyclic (C15) aliphatic alcohols/ketones with interesting application as sustainable aviation fuel (SAF) precursors with enhanced properties. The presence of surficial strong basic sites active in aldol condensation, together with the formation of highly dispersed copper nanoparticles able to catalyze C═C and C═O hydrogenation (TOF of 0.06–0.16 s−1), assured high catalytic efficiency and fine control of the products nature and distribution. From the optimization of both catalysts formulation and reaction conditions it was found that, properly tuning the Cu content, it is possible to drive products distribution towards the production of bicyclic (C10) aliphatic alcohol with high selectivity (75% at total CPO conversion, when Cu = 10 wt %, at 170 °C, 1.0 MPa of H2) and short reaction time (4 h). The optimized catalyst formulation showed impressive stability over multiple reaction/regeneration cycles, demonstrating the high potential of the proposed catalytic process for future applications in sustainable biofuels production.

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铜基催化剂用于环戊酮一锅缩合加氢制有价值的SAF前驱体
提出了一种醇缩加氢合成生物基环戊酮(CPO)的一锅反应工艺。从水滑石型前驱体中获得的铜基双功能催化剂在温和的反应条件下(即130-170°C)具有很高的活性,可以产生有价值的双环(C10)和三环(C15)脂肪醇/酮,作为具有增强性能的可持续航空燃料(SAF)前驱体有很好的应用前景。在醛醇缩合反应中活性的表面强碱位的存在,以及形成的高度分散的铜纳米粒子能够催化C = C和C = O加氢(TOF为0.06-0.16 s−1),保证了高催化效率和对产物性质和分布的精细控制。从催化剂配方和反应条件的优化中发现,适当调整Cu含量,可以推动产物分布向生产双环(C10)脂肪醇的方向发展,具有高选择性(当Cu = 10 wt %,在170°C, 1.0 MPa H2下,总CPO转化率为75%)和短反应时间(4 h)。优化后的催化剂配方在多次反应/再生循环中表现出令人满意的稳定性。展示了所提出的催化过程在未来可持续生物燃料生产中的应用潜力。
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来源期刊
ChemCatChem
ChemCatChem 化学-物理化学
CiteScore
8.10
自引率
4.40%
发文量
511
审稿时长
1.3 months
期刊介绍: With an impact factor of 4.495 (2018), ChemCatChem is one of the premier journals in the field of catalysis. The journal provides primary research papers and critical secondary information on heterogeneous, homogeneous and bio- and nanocatalysis. The journal is well placed to strengthen cross-communication within between these communities. Its authors and readers come from academia, the chemical industry, and government laboratories across the world. It is published on behalf of Chemistry Europe, an association of 16 European chemical societies, and is supported by the German Catalysis Society.
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