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      Two-dimensional molybdenum carbide 2D-Mo 2C as a superior catalyst for CO 2 hydrogenation

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          Abstract

          Early transitional metal carbides are promising catalysts for hydrogenation of CO 2. Here, a two-dimensional (2D) multilayered 2D-Mo 2C material is prepared from Mo 2C T x of the MXene family. Surface termination groups T x (O, OH, and F) are reductively de-functionalized in Mo 2C T x (500 °C, pure H 2) avoiding the formation of a 3D carbide structure. CO 2 hydrogenation studies show that the activity and product selectivity (CO, CH 4, C 2–C 5 alkanes, methanol, and dimethyl ether) of Mo 2C T x and 2D-Mo 2C are controlled by the surface coverage of T x groups that are tunable by the H 2 pretreatment conditions. 2D-Mo 2C contains no T x groups and outperforms Mo 2C T x , β-Mo 2C, or the industrial Cu-ZnO-Al 2O 3 catalyst in CO 2 hydrogenation (evaluated by CO weight time yield at 430 °C and 1 bar). We show that the lack of surface termination groups drives the selectivity and activity of Mo-terminated carbidic surfaces in CO 2 hydrogenation.

          Abstract

          The development of robust and efficient catalysts for CO 2 hydrogenation to value-added chemicals is an urgent task. Here the authors report two-dimensional carbide catalyst based on earth-abundant molybdenum that hydrogenates CO 2 with high activity, stable performance and tunable selectivity.

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          Most cited references68

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          Two-dimensional nanocrystals produced by exfoliation of Ti3 AlC2.

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            ATHENA, ARTEMIS, HEPHAESTUS: data analysis for X-ray absorption spectroscopy using IFEFFIT.

            A software package for the analysis of X-ray absorption spectroscopy (XAS) data is presented. This package is based on the IFEFFIT library of numerical and XAS algorithms and is written in the Perl programming language using the Perl/Tk graphics toolkit. The programs described here are: (i) ATHENA, a program for XAS data processing, (ii) ARTEMIS, a program for EXAFS data analysis using theoretical standards from FEFF and (iii) HEPHAESTUS, a collection of beamline utilities based on tables of atomic absorption data. These programs enable high-quality data analysis that is accessible to novices while still powerful enough to meet the demands of an expert practitioner. The programs run on all major computer platforms and are freely available under the terms of a free software license.
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              Large-area high-quality 2D ultrathin Mo2C superconducting crystals.

              Transition metal carbides (TMCs) are a large family of materials with many intriguing properties and applications, and high-quality 2D TMCs are essential for investigating new physics and properties in the 2D limit. However, the 2D TMCs obtained so far are chemically functionalized, defective nanosheets having maximum lateral dimensions of ∼10 μm. Here we report the fabrication of large-area high-quality 2D ultrathin α-Mo2C crystals by chemical vapour deposition (CVD). The crystals are a few nanometres thick, over 100 μm in size, and very stable under ambient conditions. They show 2D characteristics of superconducting transitions that are consistent with Berezinskii-Kosterlitz-Thouless behaviour and show strong anisotropy with magnetic field orientation; moreover, the superconductivity is also strongly dependent on the crystal thickness. Our versatile CVD process allows the fabrication of other high-quality 2D TMC crystals, such as ultrathin WC and TaC crystals, which further expand the large family of 2D materials.
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                Author and article information

                Contributors
                fedoroal@ethz.ch
                muelchri@ethz.ch
                Journal
                Nat Commun
                Nat Commun
                Nature Communications
                Nature Publishing Group UK (London )
                2041-1723
                17 September 2021
                17 September 2021
                2021
                : 12
                : 5510
                Affiliations
                [1 ]Department of Mechanical and Process Engineering, ETH Zürich, CH 8092 Zürich, Switzerland
                [2 ]GRID grid.112485.b, ISNI 0000 0001 0217 6921, CNRS, CEMHTI UPR3079, Université d′Orléans, ; F-45071 Orléans, France
                [3 ]GRID grid.12527.33, ISNI 0000 0001 0662 3178, Present Address: Department of Energy and Power Engineering, , Tsinghua University, ; Beijing, 100084 China
                Author information
                http://orcid.org/0000-0003-1410-4794
                http://orcid.org/0000-0002-2672-4969
                http://orcid.org/0000-0002-2011-1707
                http://orcid.org/0000-0003-4306-0815
                http://orcid.org/0000-0001-9814-6726
                http://orcid.org/0000-0003-2234-6902
                Article
                25784
                10.1038/s41467-021-25784-0
                8448824
                34535647
                cb028c74-92cd-44d7-a7e0-75d13ec4aad8
                © The Author(s) 2021

                Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.

                History
                : 16 June 2021
                : 26 August 2021
                Funding
                Funded by: FundRef https://doi.org/10.13039/100010661, EC | Horizon 2020 Framework Programme (EU Framework Programme for Research and Innovation H2020);
                Award ID: 800419
                Award Recipient :
                Categories
                Article
                Custom metadata
                © The Author(s) 2021

                Uncategorized
                catalyst synthesis,heterogeneous catalysis,two-dimensional materials
                Uncategorized
                catalyst synthesis, heterogeneous catalysis, two-dimensional materials

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