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Sustainable Catalytic Synthesis for a Bio‐Based Alternative to the Reach‐Restricted N‐Methyl‐2‐Pyrrolidone
Advanced Sustainable Systems ( IF 7.1 ) Pub Date : 2020-02-19 , DOI: 10.1002/adsu.201900117
Pierluigi Barbaro 1 , Francesca Liguori 1 , Claudio Oldani 2 , Carmen Moreno‐Marrodán 1
Affiliation  

The catalytic conversion of biomass and its derivatives into valuable chemicals requires efficient, energy saving, and sustainable technologies. In this work, a variety of bifunctional catalysts are prepared combining immobilized metal nanoparticles and acid solid materials featuring Lewis or Brønsted acidity. The catalytic systems are tested in the reductive amination of bio‐derived levulinates with primary amines, using hydrogen as clean reducing agent, to obtain N‐substituted‐5‐methyl‐2‐pyrrolidones, which are proposed as substitutes for the widely used, REACH‐restricted solvent N‐methyl‐2‐pyrrolidone. The overall process is studied in depth to identify the best combination of metal and acid functionalities to be used in one‐pot and one stage. Pt immobilized onto the Brønsted solid acid Aquivion is shown to be the most efficient catalyst, with a productivity of N‐heptyl‐5‐methyl‐2‐pyrrolidone of 7.9 mmolgcat−1 h−1 reached at full conversion and 98.6% selectivity, under 120 °C, 4 bar H2 pressure and solvent‐free conditions.

中文翻译:

可持续的催化合成技术,可替代受限的N-甲基-2-吡咯烷酮

生物质及其衍生物催化转化为有价值的化学品需要高效,节能和可持续的技术。在这项工作中,结合了固定化的金属纳米粒子和具有路易斯或布朗斯台德酸度的酸性固体材料,制备了多种双功能催化剂。使用氢作为清洁的还原剂,在生物衍生的乙酰丙酸酯与伯胺的还原胺化反应中,测试了催化体系,以获得N取代的5-甲基-2-吡咯烷酮,被提议作为广泛使用的REACH的替代品限制溶剂N甲基-2-吡咯烷酮 对整个过程进行了深入研究,以确定一锅一阶段中使用的金属和酸官能度的最佳组合。固定在Brønsted固体酸Aquivion上的Pt是最有效的催化剂,全转化率下N-庚基-5-甲基-2-吡咯烷酮的生产率为7.9 mmolg cat -1 h -1,选择性为98.6%,在120°C,4 bar H 2压力和无溶剂条件下。
更新日期:2020-02-19
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