Molecularly Defined Manganese Catalyst for Low-Temperature Hydrogenation of Carbon Monoxide to Methanol

Pavel Ryabchuk, Kenta Stier, Kathrin Junge, Marek P. Checinski, Matthias Beller

Publikation: Beitrag in FachzeitschriftArtikelBegutachtung

63 Zitate (Scopus)

Abstract

Methanol synthesis from syngas (CO/H2 mixtures) is one of the largest manmade chemical processes with annual production reaching 100 million tons. The current industrial method proceeds at high temperatures (200-300 °C) and pressures (50-100 atm) using a copper-zinc-based heterogeneous catalyst. In contrast, here, we report a molecularly defined manganese catalyst that allows for low-temperature/low-pressure (120-150 °C, 50 bar) carbon monoxide hydrogenation to methanol. This new approach was evaluated and optimized by quantum mechanical simulations virtual high-throughput screenings. Crucial for this achievement is the use of amine-based promoters, which capture carbon monoxide to give formamide intermediates, which then undergo manganese-catalyzed hydrogenolysis, regenerating the promoter. Following this conceptually new approach, high selectivity toward methanol and catalyst turnover numbers (up to 3170) was achieved. The proposed general catalytic cycle for methanol synthesis is supported by model studies and detailed spectroscopic investigations.

OriginalspracheEnglisch
Seiten (von - bis)16923-16929
Seitenumfang7
FachzeitschriftJournal of the American Chemical Society
Jahrgang141
Ausgabenummer42
DOIs
PublikationsstatusVeröffentlicht - 23 Okt. 2019
Extern publiziertJa

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