Issue 13, 2024

Liquid-phase hydrogenation of carbon monoxide to methanol using a recyclable manganese-based catalytic system

Abstract

A simple and recyclable homogeneous catalytic system for the hydrogenation of carbon monoxide to methanol was established. The reaction is catalyzed by a molecular manganese complex using a high-boiling alcohol as the solvent for catalyst immobilization. The CO hydrogenation is assisted by the product itself and the solvent through the formation of a methyl or dodecyl formate ester intermediate mediated by catalytic amounts of NaOMe as the base. This allows the catalytic formation of methanol in alcohols combined with facile product separation and catalyst recycling via distillation. Initial turnover frequencies (TOF) of 2250 h−1 were reached under optimized conditions in 1-dodecanol/methanol as the reaction medium (T = 160 °C, p(H2/CO) = 80/10 bar). The performance was stabilized in batch-wise recycling over 6 runs achieving a total turnover number (TTON) of >12 000 corresponding to an enhancement of more than five times compared to single batch operation under identical conditions. Minimal leaching of the components of the organometallic catalyst was observed during distillative product separation and catalyst activity could be fully restored by re-addition of the base NaOMe.

Graphical abstract: Liquid-phase hydrogenation of carbon monoxide to methanol using a recyclable manganese-based catalytic system

Supplementary files

Article information

Article type
Paper
Submitted
01 Mar 2024
Accepted
21 May 2024
First published
07 Jun 2024
This article is Open Access
Creative Commons BY license

Green Chem., 2024,26, 7799-7805

Liquid-phase hydrogenation of carbon monoxide to methanol using a recyclable manganese-based catalytic system

S. Stahl, N. Wessel, A. J. Vorholt and W. Leitner, Green Chem., 2024, 26, 7799 DOI: 10.1039/D4GC01050G

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