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      Sulfolane-containing aqueous electrolyte solutions for producing efficient ampere-hour-level zinc metal battery pouch cells

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          Abstract

          Aqueous zinc metal batteries are appealing candidates for grid energy storage. However, the inadequate electrochemical reversibility of the zinc metal negative electrode inhibits the battery performance at the large-scale cell level. Here, we develop practical ampere-hour-scale aqueous Zn metal battery pouch cells by engineering the electrolyte solution. After identifying the proton reduction as the primary source of H 2 evolution during Zn metal electrodeposition, we design an electrolyte solution containing reverse micelle structures where sulfolane molecules constrain water in nanodomains to hinder proton reduction. Furthermore, we develop and validate an electrochemical testing protocol to comprehensively evaluate the cell’s coulombic efficiency and zinc metal electrode cycle life. Finally, using the reverse micelle electrolyte, we assemble and test a practical ampere-hour Zn||Zn 0.25V 2O 5•nH 2O multi-layer pouch cell capable of delivering an initial energy density of 70 Wh L −1 (based on the volume of the cell components), capacity retention of about 80% after 390 cycles at 56 mA g −1 cathode and ~25 °C and prolonged cycling for 5 months at 56 mA g −1 cathode and ~25 °C.

          Abstract

          The negative electrode reversibility limits the lifespan of Zn metal batteries. Here, authors report an aqueous electrolyte with a reverse micelle structure that improves the reversibility of the Zn metal anode enabling the production of an ampere-hour-level pouch cell with five months lifetime.

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          Most cited references62

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          Efficient iterative schemes forab initiototal-energy calculations using a plane-wave basis set

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            Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set

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              A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu.

              The method of dispersion correction as an add-on to standard Kohn-Sham density functional theory (DFT-D) has been refined regarding higher accuracy, broader range of applicability, and less empiricism. The main new ingredients are atom-pairwise specific dispersion coefficients and cutoff radii that are both computed from first principles. The coefficients for new eighth-order dispersion terms are computed using established recursion relations. System (geometry) dependent information is used for the first time in a DFT-D type approach by employing the new concept of fractional coordination numbers (CN). They are used to interpolate between dispersion coefficients of atoms in different chemical environments. The method only requires adjustment of two global parameters for each density functional, is asymptotically exact for a gas of weakly interacting neutral atoms, and easily allows the computation of atomic forces. Three-body nonadditivity terms are considered. The method has been assessed on standard benchmark sets for inter- and intramolecular noncovalent interactions with a particular emphasis on a consistent description of light and heavy element systems. The mean absolute deviations for the S22 benchmark set of noncovalent interactions for 11 standard density functionals decrease by 15%-40% compared to the previous (already accurate) DFT-D version. Spectacular improvements are found for a tripeptide-folding model and all tested metallic systems. The rectification of the long-range behavior and the use of more accurate C(6) coefficients also lead to a much better description of large (infinite) systems as shown for graphene sheets and the adsorption of benzene on an Ag(111) surface. For graphene it is found that the inclusion of three-body terms substantially (by about 10%) weakens the interlayer binding. We propose the revised DFT-D method as a general tool for the computation of the dispersion energy in molecules and solids of any kind with DFT and related (low-cost) electronic structure methods for large systems.
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                Author and article information

                Contributors
                junfan@cityu.edu.hk
                cy.zhi@cityu.edu.hk
                Journal
                Nat Commun
                Nat Commun
                Nature Communications
                Nature Publishing Group UK (London )
                2041-1723
                1 April 2023
                1 April 2023
                2023
                : 14
                : 1828
                Affiliations
                [1 ]Hong Kong Center for Cerebro-Cardiovascular Health Engineering (COCHE), Hong Kong SAR, Shatin, N. T 999077 China
                [2 ]GRID grid.35030.35, ISNI 0000 0004 1792 6846, Department of Materials Science and Engineering, , City University of Hong Kong, ; Hong Kong SAR, Kowloon 999077 China
                [3 ]GRID grid.35030.35, ISNI 0000 0004 1792 6846, Hong Kong Institute for Advanced Study, , City University of Hong Kong, ; Hong Kong, Kowloon 999077 China
                [4 ]GRID grid.35030.35, ISNI 0000 0004 1792 6846, Hong Kong Institute for Clean Energy, , City University of Hong Kong, ; Hong Kong, Kowloon 999077 China
                Author information
                http://orcid.org/0000-0002-4497-0688
                http://orcid.org/0000-0001-8227-9671
                http://orcid.org/0000-0001-6766-5953
                Article
                37524
                10.1038/s41467-023-37524-7
                10067964
                37005392
                175b7cf1-053c-4136-b775-43667d58da60
                © 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 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
                : 8 August 2022
                : 20 March 2023
                Funding
                Funded by: Collaborative Research Fund
                Categories
                Article
                Custom metadata
                © The Author(s) 2023

                Uncategorized
                batteries,materials for energy and catalysis,energy storage,energy,electrochemistry
                Uncategorized
                batteries, materials for energy and catalysis, energy storage, energy, electrochemistry

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