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      Efficient industrial-current-density acetylene to polymer-grade ethylene via hydrogen-localization transfer over fluorine-modified copper

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          Abstract

          Electrocatalytic acetylene semi-hydrogenation to ethylene powered by renewable electricity represents a sustainable pathway, but the inadequate current density and single-pass yield greatly impedes the production efficiency and industrial application. Herein, we develop a F-modified Cu catalyst that shows an industrial partial current density up to 0.76 A cm −2 with an ethylene Faradic efficiency surpass 90%, and the maximum single-pass yield reaches a notable 78.5%. Furthermore, the Cu-F showcase the capability to directly convert acetylene into polymer-grade ethylene in a tandem flow cell, almost no acetylene residual in the production. Combined characterizations and calculations reveal that the Cu δ+ (near fluorine) enhances the water dissociation, and the generated active hydrogen are immediately transferred to Cu 0 (away from fluorine) and react with the locally adsorbed acetylene. Therefore, the hydrogen evolution reaction is surpassed and the overall acetylene semi-hydrogenation performance is boosted. Our findings provide new opportunity towards rational design of catalysts for large-scale electrosynthesis of ethylene and other important industrial raw.

          Abstract

          Efficient electroreduction of acetylene to ethylene is crucial for industrial applications. Here, the authors reported fluorine modified copper for direct conversion of acetylene to polymer-grade ethylene in one single-pass with industrial-current-density.

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          Most cited references34

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          Progress and Perspectives of Electrochemical CO2 Reduction on Copper in Aqueous Electrolyte

          To date, copper is the only heterogeneous catalyst that has shown a propensity to produce valuable hydrocarbons and alcohols, such as ethylene and ethanol, from electrochemical CO2 reduction (CO2R). There are variety of factors that impact CO2R activity and selectivity, including the catalyst surface structure, morphology, composition, the choice of electrolyte ions and pH, and the electrochemical cell design. Many of these factors are often intertwined, which can complicate catalyst discovery and design efforts. Here we take a broad and historical view of these different aspects and their complex interplay in CO2R catalysis on Cu, with the purpose of providing new insights, critical evaluations, and guidance to the field with regard to research directions and best practices. First, we describe the various experimental probes and complementary theoretical methods that have been used to discern the mechanisms by which products are formed, and next we present our current understanding of the complex reaction networks for CO2R on Cu. We then analyze two key methods that have been used in attempts to alter the activity and selectivity of Cu: nanostructuring and the formation of bimetallic electrodes. Finally, we offer some perspectives on the future outlook for electrochemical CO2R.
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            Electrocatalytic reduction of CO2 to ethylene and ethanol through hydrogen-assisted C–C coupling over fluorine-modified copper

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              Identification of non-precious metal alloy catalysts for selective hydrogenation of acetylene.

              The removal of trace acetylene from ethylene is performed industrially by palladium hydrogenation catalysts (often modified with silver) that avoid the hydrogenation of ethylene to ethane. In an effort to identify catalysts based on less expensive and more available metals, density functional calculations were performed that identified relations in heats of adsorption of hydrocarbon molecules and fragments on metal surfaces. This analysis not only verified the facility of known catalysts but identified nickel-zinc alloys as alternatives. Experimental studies demonstrated that these alloys dispersed on an oxide support were selective for acetylene hydrogenation at low pressures.
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                Author and article information

                Contributors
                lengky@nwu.edu.cn
                zhenglr@ihep.ac.cn
                yuntengqu@nwu.edu.cn
                Journal
                Nat Commun
                Nat Commun
                Nature Communications
                Nature Publishing Group UK (London )
                2041-1723
                16 December 2023
                16 December 2023
                2023
                : 14
                : 8384
                Affiliations
                [1 ]International Collaborative Center on Photoelectric Technology and Nano Functional Materials, Institute of Photonics and Photon-Technology, Northwest University, ( https://ror.org/00z3td547) 710069 Xi’an, Shaanxi China
                [2 ]GRID grid.494567.d, ISNI 0000 0004 4907 1766, Université Paris-Saclay, CentraleSupélec, ENS Paris-Saclay, CNRS, LMPS-Laboratoire de Mécanique Paris-Saclay, 8-10 rue Joliot-Curie, ; Gif-sur-Yvette, 91190 France
                [3 ]Institute of High Energy Physics, ( https://ror.org/03v8tnc06) 100039 Beijing, China
                [4 ]School of Chemistry and Materials Science, University of Science and Technology of China, ( https://ror.org/04c4dkn09) 230026 Hefei, China
                Author information
                http://orcid.org/0000-0003-4269-1455
                http://orcid.org/0000-0002-8182-0339
                http://orcid.org/0000-0002-0964-3358
                http://orcid.org/0000-0001-9524-2843
                Article
                44171
                10.1038/s41467-023-44171-5
                10725425
                38104169
                cfd26ba2-e7f2-4216-8c61-f7ed813809b1
                © The Author(s) 2023

                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 licence, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence 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 licence, visit http://creativecommons.org/licenses/by/4.0/.

                History
                : 24 July 2023
                : 4 December 2023
                Funding
                Funded by: FundRef https://doi.org/10.13039/501100001809, National Natural Science Foundation of China (National Science Foundation of China);
                Award ID: 22275147
                Award ID: 21902150
                Award ID: 52301289
                Award Recipient :
                Funded by: Natural Science Basic Research Program of Shaanxi 2022JM-018
                Funded by: Natural Science Basic Research Program of Shaanxi 2022JQ-082
                Categories
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                © Springer Nature Limited 2023

                Uncategorized
                electrocatalysis
                Uncategorized
                electrocatalysis

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