3 years ago

Manganese-Catalyzed Sequential Hydrogenation of CO2 to Methanol via Formamide

Manganese-Catalyzed Sequential Hydrogenation of CO2 to Methanol via Formamide
Jotheeswari Kothandaraman, Sayan Kar, G. K. Surya Prakash, Alain Goeppert
Mn(I)-PNP pincer catalyzed sequential one-pot homogeneous CO2 hydrogenation to CH3OH by molecular H2 is demonstrated. The hydrogenation consists of two parts—N-formylation of an amine utilizing CO2 and H2, and subsequent formamide reduction to CH3OH, regenerating the amine in the process. A reported air-stable and well-defined Mn-PNP pincer complex was found active for the catalysis of both steps. CH3OH yields up to 84% and 71% (w.r.t amine) were obtained, when benzylamine and morpholine were used as amines, respectively; and a TON of up to 36 was observed. In our opinion, this study represents an important development in the nascent field of base-metal-catalyzed homogeneous CO2 hydrogenation to CH3OH.

Publisher URL: http://dx.doi.org/10.1021/acscatal.7b02066

DOI: 10.1021/acscatal.7b02066

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