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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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Project description:Rechargeable aqueous zinc-ion batteries (RZIBs) provide a promising complementarity to the existing lithium-ion batteries due to their low cost, non-toxicity and intrinsic safety. However, Zn anodes suffer from zinc dendrite growth and electrolyte corrosion, resulting in poor reversibility. Here, we develop an ultrathin, fluorinated two-dimensional porous covalent organic framework (FCOF) film as a protective layer on the Zn surface. The strong interaction between fluorine (F) in FCOF and Zn reduces the surface energy of the Zn (002) crystal plane, enabling the preferred growth of (002) planes during the electrodeposition process. As a result, Zn deposits show horizontally arranged platelet morphology with (002) orientations preferred. Furthermore, F-containing nanochannels facilitate ion transport and prevent electrolyte penetration for improving corrosion resistance. The FCOF@Zn symmetric cells achieve stability for over 750 h at an ultrahigh current density of 40 mA cm-2. The high-areal-capacity full cells demonstrate hundreds of cycles under high Zn utilization conditions.

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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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