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Manganese-Catalyzed Upgrading of Ethanol into 1-Butanol

2017; American Chemical Society; Volume: 139; Issue: 34 Linguagem: Inglês

10.1021/jacs.7b05939

1943-2984

Shaomin Fu, Zhihui Shao, Yujie Wang, Qiang Liu,

Catalysis and Hydrodesulfurization Studies

Biomass-derived ethanol is an important renewable feedstock. Its conversion into high-quality biofuels is a promising route to replace fossil resources. Herein, an efficient manganese-catalyzed Guerbet-type condensation reaction of ethanol to form 1-butanol was explored. This is the first example of upgrading ethanol into higher alcohols using a homogeneous non-noble-metal catalyst. This process proceeded selectively in the presence of a well-defined manganese pincer complex at the parts per million (ppm) level. The developed reaction represents a sustainable synthesis of 1-butanol with excellent turnover number (>110 000) and turnover frequency (>3000 h-1). Moreover, mechanistic studies including control experiments, NMR spectroscopy, and X-ray crystallography identified the essential role of the "N-H moiety" of the manganese catalysts and the major reaction intermediates related to the catalytic cycle.