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A single-ion conducting covalent organic framework for aqueous rechargeable Zn-ion batteries.

ABSTRACT: Despite their potential as promising alternatives to current state-of-the-art lithium-ion batteries, aqueous rechargeable Zn-ion batteries are still far away from practical applications. Here, we present a new class of single-ion conducting electrolytes based on a zinc sulfonated covalent organic framework (TpPa-SO₃Zn_0.5) to address this challenging issue. TpPa-SO₃Zn_0.5 is synthesised to exhibit single Zn²⁺ conduction behaviour via its delocalised sulfonates that are covalently tethered to directional pores and achieve structural robustness by its β-ketoenamine linkages. Driven by these structural and physicochemical features, TpPa-SO₃Zn_0.5 improves the redox reliability of the Zn metal anode and acts as an ionomeric buffer layer for stabilising the MnO₂ cathode. Such improvements in the TpPa-SO₃Zn_0.5-electrode interfaces, along with the ion transport phenomena, enable aqueous Zn-MnO₂ batteries to exhibit long-term cyclability, demonstrating the viability of COF-mediated electrolytes for Zn-ion batteries.

SUBMITTER: Park S

PROVIDER: S-EPMC8162792 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Redox-active zinc thiolates for low-cost aqueous rechargeable Zn-ion batteries.

Project description:Aqueous zinc-ion batteries (AZIBs) are promising candidates for large-scale electrical energy storage due to the inexpensive, safe, and non-toxic nature of zinc. One key area that requires further development is electrode materials that store Zn2+ ions with high reversibility and fast kinetics. To determine the viability of low-cost organosulfur compounds as OEMs for AZIBs, we investigate how structural modification affects electrochemical performance in Zn-thiolate complexes 1 and 2. Remarkably, modification of one thiolate in 1 to sulfide in 2 reduces the voltage hysteresis from 1.04 V to 0.15 V. While 1 exhibits negligible specific capacity due to the formation of insulating DMcT polymers, 2 delivers a capacity of 107 mA h g-1 with a primary discharge plateau at 1.1 V vs. Zn2+/Zn. Spectroscopic studies of 2 suggest a Zn2+ and H+ co-insertion mechanism with Zn2+ as the predominant charge carrier. Capacity fading in Zn-2 cells likely results from the formation of (i) soluble H+ insertion products and (ii) non-redox-active side products. Increasing electrolyte concentration and using a Nafion membrane significantly enhances the stability of 2 by suppressing H+ insertion. Our findings provide insight into the molecular design strategies to reduce the polarization potential and improve the cycling stability of the thiolate/disulfide redox couple in aqueous battery systems.

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| S-EPMC8595410 | biostudies-literature

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Project description:Owing to its low cost and high safety, metallic zinc has received considerable attention as an anode material for zinc aqueous batteries (ZIBs). However, the Zn metal instability as a result ultrafast of obstinate dendrite formation, free-water-induced parasite reactions, and corrosive electrolytes has detrimental effects on the implementation of ZIBs. We present an alternative stable electrolyte for ZIBs based on a zinc chloride/ethylene glycol deep eutectic solvent (DES). This electrolyte consists of abundant low-cost materials and a utilizable Zn2+ concentration of approximately 1 M. It combines the advantages of the aqueous and DES media to provide safe and reversible Zn plating/stripping with a two-fold increase in the cycling life compared to that of conventional aqueous electrolytes. With these advantages, the Zn symmetric cell operates at 0.2 mA cm-2 for 300 h. Due to its high efficiency and compositional versatility, this electrolyte enables the investigation of a non-aqueous electrolyte family for ZIBs that fulfill grid-scale electrical energy storage requirements.

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Project description:Manganese oxide (MnO2) is one of the most promising intercalation cathode materials for zinc ion batteries (ZIBs). Specifically, a layered type delta manganese dioxide (?-MnO2) allows reversible insertion/extraction of Zn2+ ions and exhibits high storage capacity of Zn2+ ions. However, a poor conductivity of ?-MnO2, as well as other crystallographic forms, limits its potential applications. This study focuses on ?-MnO2 with nanoflower structure supported on graphite flake, namely MNG, for use as an intercalation host material of rechargeable aqueous ZIBs. Pristine ?-MnO2 nanoflowers and MNG were synthesized and examined using X-ray diffraction, electron spectroscopy, and electrochemical techniques. Also, performances of the batteries with the pristine ?-MnO2 nanoflowers and MNG cathodes were studied in CR2032 coin cells. MNG exhibits a fast insertion/extraction of Zn2+ ions with diffusion scheme and pseudocapacitive behavior. The battery using MNG cathode exhibited a high initial discharge capacity of 235 mAh/g at 200?mA/g specific current density compared to 130 mAh/g which is displayed by the pristine ?-MnO2 cathode at the same specific current density. MNG demonstrated superior electrical conductivity compared to the pristine ?-MnO2. The results obtained pave the way for improving the electrical conductivity of MnO2 by using graphite flake support. The graphite flake support significantly improved performances of ZIBs and made them attractive for use in a wide variety of energy applications.

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