Abstract
Catalyst immobilization in decane and repetitive hydrogenation of CO2 to HCOOH-amine with subsequent reactive distillation of the resulting methanolic solution.
Highlights
The first step comprises the hydrogenation of CO2 to formic acid (FA) in the presence of an amine and has been realized using a biphasic system with methanol as the product phase and n-decane as the catalyst phase allowing efficient immobilization of alkyl-tagged ruthenium phosphine complexes
The second step comprises the esterification of formic acid and methanol via reactive distillation directly from the product mixture of the first step
Repetitive batch experiments demonstrated the suitability of the biphasic system to generate a suitable feed for the second step with excellent catalyst retention
Summary
The interest in the utilization of CO2 as readily available feedstock is experiencing a growing momentum in both academia and industry.[1,2,3,4,5,6] Carbon dioxide can be “harvested” in high concentration at numerous point sources worldwide facilitating the implementation of carbon capture and utilization (CCU) concepts,[7,8] including the use of CO2 as C1-building block for chemical synthesis as an attractive and challenging option.[9,10,11,12,13] These strategies can contribute to the goal of “defossilization” of the chemical value chain, in particular when combined with energy input from renewable resources.[14]Catalytic hydrogenation of CO2 using transition metal complexes has evolved as a promising valorization strategy providing a range of differently functionalized products.[9,15,16,17,18] In a “drop-in” approach, CO2-based products can replace chemical commodities usually produced by the refinement of fossil carbon and eventually lead to a more closed carbon cycle, which is the ultimate goal of a sustainable economy. An integrated two-step process was developed for the production of methylformate (MF) from carbon dioxide, hydrogen and methanol.
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