Betsy Kurisingal Joseph, Pablo Doménech, Leonhard Schill, Anders Riisager
{"title":"Exploring Heterogeneous Pd Nanocatalysts for Upgrading Acetone-Butanol Mixtures to Sustainable Aviation Fuel Precursors","authors":"Betsy Kurisingal Joseph, Pablo Doménech, Leonhard Schill, Anders Riisager","doi":"10.1021/acssuschemeng.5c02948","DOIUrl":null,"url":null,"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, C<sub>11</sub>(═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 MgKPO<sub>4</sub> in the presence of the K<sub>3</sub>PO<sub>4</sub> 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.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"266 1","pages":""},"PeriodicalIF":7.1000,"publicationDate":"2025-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Sustainable Chemistry & Engineering","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acssuschemeng.5c02948","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
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.
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.