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      High‐Capacity Zinc Anode with 96 % Utilization Rate Enabled by Solvation Structure Design

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          Abstract

          Aqueous zinc‐ion batteries (AZBs) show promises for large‐scale energy storage. However, the zinc utilization rate (ZUR) is generally low due to side reactions in the aqueous electrolyte caused by the active water molecules. Here, we design a novel solvation structure in the electrolyte by introduction of sulfolane (SL). Theoretical calculations, molecular dynamics simulations and experimental tests show that SL remodels the primary solvation shell of Zn 2+, which significantly reduces the side reactions of Zn anode and achieves high ZUR under large capacities. Specifically, the symmetric and asymmetric cells could achieve a maximum of ∼96 % ZUR at an areal capacity of 24 mAh cm −2. In a ZUR of ∼67 %, the developed Zn−V 2O 5 full cell can be stably cycled for 500 cycles with an energy density of 180 Wh kg −1 and Zn‐AC capacitor is stable for 5000 cycles. This electrolyte structural engineering strategy provides new insight into achieving high ZUR of Zn anodes for high performance AZBs.

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          Most cited references52

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          Highly reversible zinc metal anode for aqueous batteries

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            Roadmap for advanced aqueous batteries: From design of materials to applications

            Aqueous batteries are a reliable alternative for next-generation safe, low-cost, and scalable energy storage.
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              Manipulating the ion-transfer kinetics and interface stability for high-performance zinc metal anodes

              We report a new class of Zn anodes modified by a three-dimensional nanoporous ZnO architecture (Zn@ZnO-3D), which can accelerate the kinetics of Zn 2+ transfer and deposition, inhibit dendrite growth, and reduce the side-reactions. The zinc metal is recognized as one of the most promising anodes for Zn-based batteries in an energy-storage system. However, the deposition and transfer of bivalent Zn 2+ into the host structure suffer from sluggish kinetics accompanying the side-reactions at the interface. Herein, we report a new class of Zn anodes modified by a three-dimensional (3D) nanoporous ZnO architecture coating on a Zn plate (designated as Zn@ZnO-3D) prepared by in situ Zn(OH) 4 2− deposition onto the surface. This novel structure has been proven to accelerate the kinetics of Zn 2+ transfer and deposition via the electrostatic attraction toward Zn 2+ rather than the hydrated one in the electrical double layer. As a consequence, it achieves an average 99.55% Zn utilization and long-time stability for 1000 cycles. Meanwhile, the Zn@ZnO-3D/MnO 2 cell shows no capacity fading after 500 cycles at 0.5 A g −1 with a specific capacity of 212.9 mA h g −1 . We believe that the mechanistic insight into the kinetics and thermodynamic properties of the Zn metal and the understanding of structure–interface–function relationships are very useful for other metal anodes in aqueous systems.
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                Author and article information

                Contributors
                Journal
                Angewandte Chemie International Edition
                Angew Chem Int Ed
                Wiley
                1433-7851
                1521-3773
                January 16 2023
                December 08 2022
                January 16 2023
                : 62
                : 3
                Affiliations
                [1 ] Department of Applied Chemistry School of Chemistry and Materials Science Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of China 230026 Hefei Anhui China
                [2 ] Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of China 230026 Hefei Anhui China
                Article
                10.1002/anie.202214966
                22f70f46-c562-4e3f-83e8-e22d2397ac18
                © 2023

                http://onlinelibrary.wiley.com/termsAndConditions#vor

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