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Highly selective hydrogenation of CO₂ into C₂₊ alcohols by homogeneous catalysis.

ABSTRACT: The hydrogenation of CO₂ to produce alcohols with two or more carbons (C₂₊ alcohols) is of great importance, but is challenging. In this work, we found that a Ru₃(CO)₁₂/Rh₂(CO)₄Cl₂-LiI system could catalyze the reaction effectively in 1,3-dimethyl-2-imidazolidinone (DMI) under mild conditions. Methanol, ethanol, propanol, 2-methyl propanol, butanol, and 2-methyl butanol were produced in the homogeneous catalytic reaction. The C₂₊ alcohols could be generated at 160 °C, which is the lowest temperature reported so far for producing C₂₊ alcohols via CO₂ hydrogenation. The selectivity for the C₂₊ alcohols could be as high as 96.4% at the optimized conditions, which is higher than those reported in the literature. In addition, the catalytic system could be easily recycled. The route of the reaction for forming the C₂₊ alcohols was discussed on the basis of control experiments.

SUBMITTER: Qian Q

PROVIDER: S-EPMC5947507 | biostudies-literature | 2015 Oct

REPOSITORIES: biostudies-literature

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Highly selective hydrogenation of CO2 into C2+ alcohols by homogeneous catalysis.

Qian Qingli Q Cui Meng M He Zhenhong Z Wu Congyi C Zhu Qinggong Q Zhang Zhaofu Z Ma Jun J Yang Guanying G Zhang Jingjing J Han Buxing B

Chemical science 20150710 10

The hydrogenation of CO2 to produce alcohols with two or more carbons (C2+ alcohols) is of great importance, but is challenging. In this work, we found that a Ru3(CO)12/Rh2(CO)4Cl2-LiI system could catalyze the reaction effectively in 1,3-dimethyl-2-imidazolidinone (DMI) under mild conditions. Methanol, ethanol, propanol, 2-methyl propanol, butanol, and 2-methyl butanol were produced in the homogeneous catalytic reactio ...[more]

PMID: 29861902

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Project description:BackgroundReplacing fossil fuels as energy carrier requires alternatives that combine sustainable production, high volumetric energy density, easy and fast refueling for mobile applications, and preferably low risk of hazard. Molecular hydrogen (H2) has been considered as promising alternative; however, practical application is struggling because of the low volumetric energy density and the explosion hazard when stored in large amounts. One way to overcome these limitations is the transient conversion of H2 into other chemicals with increased volumetric energy density and lower risk hazard, for example so-called liquid organic hydrogen carriers such as formic acid/formate that is obtained by hydrogenation of CO2. Many homogenous and heterogenous chemical catalysts have been described in the past years, however, often requiring high pressures and temperatures. Recently, the first biocatalyst for this reaction has been described opening the route to a biotechnological alternative for this conversion.ResultsThe hydrogen-dependent CO2 reductase (HDCR) is a highly active biocatalyst for storing H2 in the form of formic acid/formate by reversibly catalyzing the hydrogenation of CO2. We report the identification, isolation, and characterization of the first thermostable HDCR operating at temperatures up to 70 °C. The enzyme was isolated from the thermophilic acetogenic bacterium Thermoanaerobacter kivui and displays exceptionally high activities in both reaction directions, substantially exceeding known chemical catalysts. CO2 hydrogenation is catalyzed at mild conditions with a turnover frequency of 9,556,000 h-1 (specific activity of 900 µmol formate min-1 mg-1) and the reverse reaction, H2?+?CO2 release from formate, is catalyzed with a turnover frequency of 9,892,000 h-1 (930 µmol H2 min-1 mg-1). The HDCR of T. kivui consists of a [FeFe] hydrogenase subunit putatively coupled to a tungsten-dependent CO2 reductase/formate dehydrogenase subunit by an array of iron-sulfur clusters.ConclusionsThe discovery of the first thermostable HDCR provides a promising biological alternative for a chemically challenging reaction and might serve as model for the better understanding of catalysts able to efficiently reduce CO2. The catalytic activity for reversible CO2 hydrogenation of this enzyme is the highest activity known for bio- and chemical catalysts and requiring only ambient temperatures and pressures. The thermostability provides more flexibility regarding the process parameters for a biotechnological application.

Dataset Information

Highly selective hydrogenation of CO₂ into C₂₊ alcohols by homogeneous catalysis.

Publications

Highly selective hydrogenation of CO<sub>2</sub> into C<sub>2+</sub> alcohols by homogeneous catalysis.

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