Exploring Heterogeneous Pd Nanocatalysts for Upgrading Acetone-Butanol Mixtures to Sustainable Aviation Fuel Precursors

IF 7.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Betsy Kurisingal Joseph, Pablo Doménech, Leonhard Schill, Anders Riisager
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Abstract

The catalytic conversion of fermentation-derived short-chained oxygenates into longer-chained hydrocarbons offers a promising solution to obtain sustainable aviation fuel (SAF) with a low carbon footprint and maximum utilization of renewable resources. This study explores the alkylation of acetone-butanol (AB) mixtures using Pd supported on high-surface area materials with varying inherent properties, aiming to optimize selectivity toward higher ketones. To elucidate the nature of the active catalyst, all synthesized catalysts were thoroughly characterized and tested under the optimized reaction conditions for the AB alkylation. A 5 wt % Pd/MgO-HS (HS: high surface) catalyst was found to exhibit the highest selectivity (81%) for 6-undecanone, C11(═O), which was attributed to an optimal balance of catalytically active sites and surface properties. Despite the absence of Pd leaching, the catalyst showed reduced activity in consecutive reaction runs. Comprehensive analysis of the spent catalyst identified the primary cause to be a transformation of the MgO support to MgKPO4 in the presence of the K3PO4 base additive under the reaction conditions. The restructuring of the catalyst support led to entrapment of the accessible Pd sites, reducing their availability for catalytic reactions. The insights from the study provide a robust framework for future SAF development, particularly in the design and optimization of catalysts for higher ketone production from renewable resources.

Abstract Image

探索丙酮-丁醇混合物转化为可持续航空燃料前驱体的多相钯纳米催化剂
发酵衍生的短链含氧化合物催化转化为长链碳氢化合物,为获得低碳足迹和最大限度利用可再生资源的可持续航空燃料(SAF)提供了一种有前途的解决方案。本研究探讨了在具有不同固有性质的高表面积材料上负载Pd对丙酮-丁醇(AB)混合物的烷基化反应,旨在优化对高级酮的选择性。为了阐明活性催化剂的性质,在优化的AB烷基化反应条件下,对所有合成的催化剂进行了全面的表征和测试。发现5 wt % Pd/MgO-HS (HS:高表面)催化剂对6-十一酮C11(= O)具有最高的选择性(81%),这归因于催化活性位点和表面性质的最佳平衡。尽管没有钯浸出,催化剂在连续反应中表现出活性降低。对废催化剂的综合分析表明,在反应条件下,在K3PO4碱添加剂的存在下,MgO载体转化为MgKPO4是主要原因。催化剂载体的重组导致可接近的Pd位点被困住,降低了它们在催化反应中的可用性。该研究的见解为未来SAF的发展提供了一个强有力的框架,特别是在设计和优化催化剂以从可再生资源中生产更高的酮。
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来源期刊
ACS Sustainable Chemistry & Engineering
ACS Sustainable Chemistry & Engineering CHEMISTRY, MULTIDISCIPLINARY-ENGINEERING, CHEMICAL
CiteScore
13.80
自引率
4.80%
发文量
1470
审稿时长
1.7 months
期刊介绍: ACS Sustainable Chemistry & Engineering is a prestigious weekly peer-reviewed scientific journal published by the American Chemical Society. Dedicated to advancing the principles of green chemistry and green engineering, it covers a wide array of research topics including green chemistry, green engineering, biomass, alternative energy, and life cycle assessment. The journal welcomes submissions in various formats, including Letters, Articles, Features, and Perspectives (Reviews), that address the challenges of sustainability in the chemical enterprise and contribute to the advancement of sustainable practices. Join us in shaping the future of sustainable chemistry and engineering.
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