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      Weakly Polarized Organic Cation-Modified Hydrated Vanadium Oxides for High-Energy Efficiency Aqueous Zinc-Ion Batteries

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          Highlights

          • A vanadium oxide (TMPA-VOH) is synthesized with trimethylphenylammonium cations chemically pre-inserted into hydrated vanadium oxide.

          • The pre-intercalation of weakly polarized organic cations strategically utilizes both ionic and molecular pre-intercalation effects.

          • TMPA-VOH, with modified crystal structure and morphology, increased V 4+ content, and weakened electrostatic interactions between Zn 2+ and the V-O lattice, demonstrates enhanced voltage, storage capacity, structural stability, and reaction kinetics.

          Supplementary Information

          The online version contains supplementary material available at 10.1007/s40820-024-01339-y.

          Abstract

          Vanadium oxides, particularly hydrated forms like V 2O 5· nH 2O (VOH), stand out as promising cathode candidates for aqueous zinc ion batteries due to their adjustable layered structure, unique electronic characteristics, and high theoretical capacities. However, challenges such as vanadium dissolution, sluggish Zn 2+ diffusion kinetics, and low operating voltage still hinder their direct application. In this study, we present a novel vanadium oxide ([C 6H 6N(CH 3) 3] 1.08V 8O 20·0.06H 2O, TMPA-VOH), developed by pre-inserting trimethylphenylammonium (TMPA +) cations into VOH. The incorporation of weakly polarized organic cations capitalizes on both ionic pre-intercalation and molecular pre-intercalation effects, resulting in a phase and morphology transition, an expansion of the interlayer distance, extrusion of weakly bonded interlayer water, and a substantial increase in V 4+ content. These modifications synergistically reduce the electrostatic interactions between Zn 2+ and the V–O lattice, enhancing structural stability and reaction kinetics during cycling. As a result, TMPA-VOH achieves an elevated open circuit voltage and operation voltage, exhibits a large specific capacity (451 mAh g –1 at 0.1 A g –1) coupled with high energy efficiency (89%), the significantly-reduced battery polarization, and outstanding rate capability and cycling stability. The concept introduced in this study holds great promise for the development of high-performance oxide-based energy storage materials.

          Supplementary Information

          The online version contains supplementary material available at 10.1007/s40820-024-01339-y.

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          Most cited references72

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          Zn/MnO2 Battery Chemistry With H+ and Zn2+ Coinsertion.

          Rechargeable aqueous Zn/MnO2 battery chemistry in a neutral or mildly acidic electrolyte has attracted extensive attention recently because all the components (anode, cathode, and electrolyte) in a Zn/MnO2 battery are safe, abundant, and sustainable. However, the reaction mechanism of the MnO2 cathode remains a topic of discussion. Herein, we design a highly reversible aqueous Zn/MnO2 battery where the binder-free MnO2 cathode was fabricated by in situ electrodeposition of MnO2 on carbon fiber paper in mild acidic ZnSO4+MnSO4 electrolyte. Electrochemical and structural analysis identify that the MnO2 cathode experience a consequent H+ and Zn2+ insertion/extraction process with high reversibility and cycling stability. To our best knowledge, it is the first report on rechargeable aqueous batteries with a consequent ion-insertion reaction mechanism.
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            A reflection on lithium-ion battery cathode chemistry

            Lithium-ion batteries have aided the portable electronics revolution for nearly three decades. They are now enabling vehicle electrification and beginning to enter the utility industry. The emergence and dominance of lithium-ion batteries are due to their higher energy density compared to other rechargeable battery systems, enabled by the design and development of high-energy density electrode materials. Basic science research, involving solid-state chemistry and physics, has been at the center of this endeavor, particularly during the 1970s and 1980s. With the award of the 2019 Nobel Prize in Chemistry to the development of lithium-ion batteries, it is enlightening to look back at the evolution of the cathode chemistry that made the modern lithium-ion technology feasible. This review article provides a reflection on how fundamental studies have facilitated the discovery, optimization, and rational design of three major categories of oxide cathodes for lithium-ion batteries, and a personal perspective on the future of this important area.
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              Active Materials for Aqueous Zinc Ion Batteries: Synthesis, Crystal Structure, Morphology, and Electrochemistry

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                Author and article information

                Contributors
                gzcao@uw.edu
                Journal
                Nanomicro Lett
                Nanomicro Lett
                Nano-Micro Letters
                Springer Nature Singapore (Singapore )
                2311-6706
                2150-5551
                22 February 2024
                22 February 2024
                December 2024
                : 16
                : 129
                Affiliations
                [1 ]Department of Materials Science and Engineering, University of Washington, ( https://ror.org/00cvxb145) Seattle, WA 98195 USA
                [2 ]School of Materials Science and Engineering, Tongji University, ( https://ror.org/03rc6as71) Shanghai, 201804 People’s Republic of China
                Article
                1339
                10.1007/s40820-024-01339-y
                10884394
                38386163
                177dcac2-63fc-455e-bc45-579203749fa7
                © The Author(s) 2024

                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
                : 11 September 2023
                : 4 January 2024
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                © Shanghai Jiao Tong University 2024

                zinc-ion battery,vanadium oxide,v2o5·nh2o,pre-intercalation,interlayer engineering

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