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Selective Ruthenium-Catalyzed Transformation of Carbon Dioxide: An Alternative Approach toward Formaldehyde

Author:
Siebert, Max, Seibicke, Max, Siegle, Alexander F., Kräh, Sabrina, Trapp, Oliver
Source:
Journal of the American Chemical Society 2018 v.141 no.1 pp. 334-341
ISSN:
1520-5126
Subject:
carbon dioxide, catalysts, formaldehyde, formates, hydrogen, methanol, oxidation, ruthenium, screening, temperature
Abstract:
Formaldehyde is an important precursor to numerous industrial processes and is produced in multimillion ton scale every year by catalytic oxidation of methanol in an energetically unfavorable and atom-inefficient industrial process. In this work, we present a highly selective one-step synthesis of a formaldehyde derivative starting from carbon dioxide and hydrogen gas utilizing a homogeneous ruthenium catalyst. Here, formaldehyde is obtained as dimethoxymethane, its dimethyl acetal, by selective reduction of carbon dioxide at moderate temperatures (90 °C) and partial pressures (90 bar H₂/20 bar CO₂) in the presence of methanol. Besides the desired product, only methyl formate is formed, which can be transformed to dimethoxymethane in a consecutive catalytic step. By comprehensive screening of the catalytic system, maximum turnover numbers of 786 for dimethoxymethane and 1290 for methyl formate were achieved with remarkable selectivities of over 90% for dimethoxymethane.
Agid:
6271555