141
views
0
recommends
+1 Recommend
0 collections
    0
    shares
      • Record: found
      • Abstract: found
      • Article: found
      Is Open Access

      Direct synthesis of formic acid from carbon dioxide by hydrogenation in acidic media

      research-article
      1 , 1 , a , 1
      Nature Communications
      Nature Pub. Group

      Read this article at

      Bookmark
          There is no author summary for this article yet. Authors can add summaries to their articles on ScienceOpen to make them more accessible to a non-specialist audience.

          Abstract

          The chemical transformation of carbon dioxide into useful products becomes increasingly important as CO 2 levels in the atmosphere continue to rise as a consequence of human activities. In this article we describe the direct hydrogenation of CO 2 into formic acid using a homogeneous ruthenium catalyst, in aqueous solution and in dimethyl sulphoxide (DMSO), without any additives. In water, at 40 °C, 0.2 M formic acid can be obtained under 200 bar, however, in DMSO the same catalyst affords 1.9 M formic acid. In both solvents the catalysts can be reused multiple times without a decrease in activity. Worldwide demand for formic acid continues to grow, especially in the context of a renewable energy hydrogen carrier, and its production from CO 2 without base, via the direct catalytic carbon dioxide hydrogenation, is considerably more sustainable than the existing routes.

          Abstract

          The conversion of carbon dioxide into formic acid is attractive for energy storage and chemical production, but the typical use of bases or other additives make isolation of the free acid difficult. Here, the authors report the catalytic conversion of carbon dioxide into formic acid without the need for any additives.

          Related collections

          Most cited references15

          • Record: found
          • Abstract: found
          • Article: not found

          Utilisation of CO2 as a chemical feedstock: opportunities and challenges.

          The need to reduce the accumulation of CO(2) into the atmosphere requires new technologies able to reduce the CO(2) emission. The utilization of CO(2) as a building block may represent an interesting approach to synthetic methodologies less intensive in carbon and energy. In this paper the general properties of carbon dioxide and its interaction with metal centres is first considered. The potential of carbon dioxide as a raw material in the synthesis of chemicals such as carboxylates, carbonates, carbamates is then discussed. The utilization of CO(2) as source of carbon for the synthesis of fuels or other C(1) molecules such as formic acid and methanol is also described and the conditions for its implementation are outlined. A comparison of chemical and biotechnological conversion routes of CO(2) is made and the barriers to their exploitation are highlighted.
            Bookmark
            • Record: found
            • Abstract: found
            • Article: not found

            Reversible hydrogen storage using CO2 and a proton-switchable iridium catalyst in aqueous media under mild temperatures and pressures.

            Green plants convert CO(2) to sugar for energy storage via photosynthesis. We report a novel catalyst that uses CO(2) and hydrogen to store energy in formic acid. Using a homogeneous iridium catalyst with a proton-responsive ligand, we show the first reversible and recyclable hydrogen storage system that operates under mild conditions using CO(2), formate and formic acid. This system is energy-efficient and green because it operates near ambient conditions, uses water as a solvent, produces high-pressure CO-free hydrogen, and uses pH to control hydrogen production or consumption. The extraordinary and switchable catalytic activity is attributed to the multifunctional ligand, which acts as a proton-relay and strong π-donor, and is rationalized by theoretical and experimental studies.
              Bookmark
              • Record: found
              • Abstract: found
              • Article: not found

              Catalytic hydrogenation of carbon dioxide using Ir(III)-pincer complexes.

              Catalytic hydrogenation of carbon dioxide in aqueous potassium hydroxide was performed using a newly synthesized isopropyl-substituted PNP-pincer iridium trihydride complex as a catalyst. Potassium formate was obtained with turnover numbers up to 3,500,000 and a turnover frequency of 150,000 h(-1), both of which are the highest values reported to date.
                Bookmark

                Author and article information

                Journal
                Nat Commun
                Nat Commun
                Nature Communications
                Nature Pub. Group
                2041-1723
                02 June 2014
                : 5
                : 4017
                Affiliations
                [1 ]Institut des Sciences et Ingénierie Chimiques, Ecole Polytechnique Fédérale de Lausanne (EPFL) , CH-1015 Lausanne, Switzerland
                Author notes
                Article
                ncomms5017
                10.1038/ncomms5017
                4059918
                24886955
                d683eeba-8825-48d1-9666-ce863458366f
                Copyright © 2014, Nature Publishing Group, a division of Macmillan Publishers Limited. All Rights Reserved.

                This work is licensed under a Creative Commons Attribution-NonCommercial-ShareAlike 3.0 Unported License. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by-nc-sa/3.0/

                History
                : 05 February 2014
                : 30 April 2014
                Categories
                Article

                Uncategorized
                Uncategorized

                Comments

                Comment on this article