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      CO 2 Hydrogenation at Atmospheric Pressure and Low Temperature Using Plasma-Enhanced Catalysis over Supported Cobalt Oxide Catalysts

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          Abstract

          CO 2 is a promising renewable, cheap, and abundant C1 feedstock for producing valuable chemicals, such as CO and methanol. In conventional reactors, because of thermodynamic constraints, converting CO 2 to methanol requires high temperature and pressure, typically 250 °C and 20 bar. Nonthermal plasma is a better option, as it can convert CO 2 at near-ambient temperature and pressure. Adding a catalyst to such plasma setups can enhance conversion and selectivity. However, we know little about the effects of catalysts in such systems. Here, we study CO 2 hydrogenation in a dielectric barrier discharge plasma-catalysis setup under ambient conditions using MgO, γ-Al 2O 3, and a series of Co x O y /MgO catalysts. While all three catalyst types enhanced CO 2 conversion, Co x O y /MgO gave the best results, converting up to 35% of CO 2 and reaching the highest methanol yield (10%). Control experiments showed that the basic MgO support is more active than the acidic γ-Al 2O 3, and that MgO-supported cobalt oxide catalysts improve the selectivity toward methanol. The methanol yield can be tuned by changing the metal loading. Overall, our study shows the utility of plasma catalysis for CO 2 conversion under mild conditions, with the potential to reduce the energy footprint of CO 2-recycling processes.

          Abstract

          CO 2 hydrogenation to CO and methanol was achieved near room temperature and atmospheric pressure using plasma-enhanced catalysis. The catalyst metal loading and cobalt oxide dispersion influence the product distribution.

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              The active site of methanol synthesis over Cu/ZnO/Al2O3 industrial catalysts.

              One of the main stumbling blocks in developing rational design strategies for heterogeneous catalysis is that the complexity of the catalysts impairs efforts to characterize their active sites. We show how to identify the crucial atomic structure motif for the industrial Cu/ZnO/Al(2)O(3) methanol synthesis catalyst by using a combination of experimental evidence from bulk, surface-sensitive, and imaging methods collected on real high-performance catalytic systems in combination with density functional theory calculations. The active site consists of Cu steps decorated with Zn atoms, all stabilized by a series of well-defined bulk defects and surface species that need to be present jointly for the system to work.
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                Author and article information

                Journal
                ACS Sustain Chem Eng
                ACS Sustain Chem Eng
                sc
                ascecg
                ACS Sustainable Chemistry & Engineering
                American Chemical Society
                2168-0485
                17 November 2020
                30 November 2020
                : 8
                : 47
                : 17397-17407
                Affiliations
                []Van‘t Hoff Institute for Molecular Sciences, University of Amsterdam , Science Park 904, 1090GD Amsterdam, The Netherlands
                []Department of Electrical Engineering and Electronics, University of Liverpool , L69 3GJ Liverpool, U.K.
                [§ ]Department of Chemical and Environmental Engineering, University of Oviedo , C/Julián Clavería, s/n., E-33071 Oviedo, Spain
                Author notes
                Article
                10.1021/acssuschemeng.0c05565
                7709469
                33282570
                3b42a9d4-4796-4263-8441-0593802c4e91
                © 2020 American Chemical Society

                This is an open access article published under a Creative Commons Non-Commercial No Derivative Works (CC-BY-NC-ND) Attribution License, which permits copying and redistribution of the article, and creation of adaptations, all for non-commercial purposes.

                History
                : 30 July 2020
                : 08 October 2020
                Categories
                Research Article
                Custom metadata
                sc0c05565
                sc0c05565

                green chemistry,plasma catalysis,methanol synthesis,cobalt oxide,co2 conversion

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