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在CO-可切换溶剂体系中的自动串联催化还原氢甲酰化反应

Auto-Tandem Catalytic Reductive Hydroformylation in a CO-Switchable Solvent System.

作者信息

Püschel Sebastian, Sadowski Jan, Rösler Thorsten, Ehmann Kira Ruth, Vorholt Andreas J, Leitner Walter

机构信息

Max Planck Institute for Chemical Energy Conversion, 45470 Mülheim an der Ruhr, Germany.

Institute for Technical and Macromolecular Chemistry, RWTH Aachen University, 52074 Aachen, Germany.

出版信息

ACS Sustain Chem Eng. 2022 Mar 21;10(11):3749-3756. doi: 10.1021/acssuschemeng.2c00419. Epub 2022 Mar 8.

Abstract

Upgradation of olefin-enriched Fischer-Tropsch cuts by the synthesis of alcohols leads to drop-in-capable biosynthetic fuels with low carbon emissions. As an alternative to the conventional two-step production of long-chain alcohols, tandem catalytic systems improve the energy and resource efficiency. Herein, we present an auto-tandem catalytic system for the production of alcohols from olefin-paraffin mixtures. By utilization of a tertiary alkanolamine as the ligand as well as the switchable component in the solvent system, a lean reaction system capable of catalyst recycling was developed. The system was characterized with regard to the switchable solvent separation approach and reaction parameters, resulting in alcohol yields of up to 99.5% and turnover frequencies of up to 764 h. By recycling the catalyst in 10 consecutive reactions, a total turnover number of 2810 was achieved.

摘要

通过醇合成对富含烯烃的费托馏分进行升级可得到具有低碳排放的可直接替代的生物合成燃料。作为传统长链醇两步法生产的替代方法,串联催化系统提高了能源和资源效率。在此,我们展示了一种用于从烯烃 - 石蜡混合物生产醇的自动串联催化系统。通过使用叔烷醇胺作为配体以及溶剂体系中的可切换组分,开发了一种能够进行催化剂循环的贫反应体系。该系统在可切换溶剂分离方法和反应参数方面进行了表征,醇产率高达99.5%,周转频率高达764 h⁻¹。通过在10次连续反应中循环使用催化剂,实现了总计2810的总周转数。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/aed6/8942186/4b6fe6648ba1/sc2c00419_0002.jpg

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