Research progress on the design of electrolyte additives and their functions for zinc-ion batteries

doi: 10.1088/2752-5724/acef41

1.
College of Chemistry and Materials Engineering, Beijing Technology and Business University, Beijing 100048, People’s Republic of China
2.
State Key Laboratory of Chemical Resource Engineering, Beijing Key Laboratory of Electrochemical Process and Technology of Materials, Beijing University of Chemical Technology, Beijing 10029, People’s Republic of China

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Corresponding author: E-mail: liulili@btbu.edu.cn; E-mail: chensm@buct.edu.cn

摘要

Abstract: In recent years, zinc-ion batteries (ZIBs) have been considered one of the most promising candidates for next-generation electrochemical energy storage systems due to their advantages of high safety, high specific capacity and high economic efficiency. As an indispensable component, the electrolyte has the function of connecting the cathode and the anode, and plays a key role in the performance of the battery. Different types of electrolytes have different effects on the performance of ZIBs, and the use of additives has further developed the research on modified electrolytes, thus effectively solving many serious problems faced by ZIBs. Therefore, to further explore the improvement of ZIBs by electrolyte engineering, it is necessary to summarize the current status of the design of various electrolyte additives, as well as their functions and mechanism in ZIBs. This paper analyzes the challenges faced by different electrolytes, reviews the different solutions of additives to solve battery problems in liquid electrolytes and solid electrolytes, and finally makes suggestions for the development of modified ZIB electrolytes. It is hoped that the review and strategies proposed in this paper will facilitate development of new electrolyte additives for ZIBs.
- zinc-ion batteries /
- additives /
- liquid electrolytes /
- solid electrolytes /
- interface
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Figure 1. Research advances in various kinds of electrolytes and additives in Zn-ion batteries. This includes liquid electrolytes (divided into aqueous systems, organic systems and water-organic hybrid systems), solid electrolytes (divided into hydrogel solid systems, polymeric gel systems and all-solid systems). Reprinted from [11], Copyright (2022), with permission from Elsevier. [13] John Wiley & Sons. [© 2022 WileyVCH GmbH]. [14] John Wiley & Sons. [© 2020 WILEYVCH Verlag GmbH & Co. KGaA, Weinheim]. [21] John Wiley & Sons. [© 2021 WileyVCH GmbH]. Reprinted from [22], Copyright (2022), with permission from Elsevier. Reprinted from [23], Copyright (2022), with permission from Elsevier. [24] John Wiley & Sons. [© 2021 WileyVCH GmbH].

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Figure 2. Existing challenges for cathodes and anodes in aqueous Zn-ion batteries, and the positive impact additives can play.

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Figure 3. (a) Growth process of Zn dendrites. (b) and (c) are the chemical mechanisms of the corrosion reaction and the hydrogen evolution reaction, respectively.

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Figure 4. (a) Scheme of Zn²⁺ solvation structure and Zn surface passivization in H₂O (left) and H₂O-DMSO (right) solvents. (b) SEM images of the Zn electrode in Zn/Zn symmetrical cells after 50 plating/stripping cycles at 0.5 mA cm^-2 and 0.5 mAh cm^-2 in ZnCl₂-H₂O-DMSO electrolytes. White lines indicate the etching depth in the cross-section view. Reprinted with permission from [34]. Copyright (2020) American Chemical Society. (c) Due to to PG’s hydrophobic nature (-CH₃ tail and hydrocarbon backbone), it can remove the hydrogen bubbles from the Zn surface that, in the PG-free electrolyte, induce porous and flaky Zn deposit formation. (d) In situ optical microscopy investigation of Zn deposition in a transparent Zn/Zn cell with PG-free and 10% PG electrolytes. (e) Cycling performance of AC/Zn cells in the three electrolytes; [35] John Wiley & Sons. [© 2022 WileyVCH GmbH]. (f), (g) Potential and current distribution of Zn deposition at a simulation time of 2 min in ZSO electrolyte (f) and ZSO/Ce electrolyte (g); gray lines with the arrows and the black lines at the bottom represent the current and the initial surface of the Zn anode. [36] John Wiley & Sons. [© 2022 WileyVCH GmbH]. (h) O 1s of Zn surface after charge-discharge process with 2 M LiCl as the additive. Reprinted with permission from [37]. Copyright (2021) American Chemical Society. (i) SEM images of Zn anodes plated in electrolyte with Hmim for 30 min at a current density of 1 mA cm^-2. Reprinted from [38], Copyright (2023), with permission from Elsevier.

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Figure 5. (a) Schematic illustration of Zn²⁺-solvation structure with or without DMA. Reprinted from [39], Copyright (2022), with permission from Elsevier. (b) Molecular structures of carbonate cosolvents (i.e. EC, PC, DMC and DEC). (c) Schematic illustration of Zn electrode interface chemistry in BE and BE + 7 m DEC. Reprinted with permission from [40]. Copyright (2022) American Chemical Society. (d) XRD patterns of Zn anodes immersed in Sel/ZnSO₄ and ZnSO₄ electrolytes. (e) In situ optical microscopy images of the cross-sectional Zn deposition morphology on the exposed area of ZnSe coated Cu foil in ZnSO₄ and Sel/ZnSO₄ electrolyte (current density: 5 mA cm^-2); [42] John Wiley & Sons. [© 2022 WileyVCH GmbH].

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Figure 6. (a) Schematic diagram of Zn deposition behavior in Zn(OTf)₂ aqueous electrolyte containing TMU additives. (b) Schematic diagram of Zn deposition behavior in Zn(OTf)₂ aqueous electrolyte without TMU additives; [53] John Wiley & Sons. [© 2022 WileyVCH GmbH]. (c) Molecular dynamics simulation models of electrolytes with PFOA additives. H₂O molecular distribution of the Zn²⁺ first hydration layer in the electrolyte with PFOA additives. (d) Working window of different electrolytes. Reproduced from [54]. CC BY 4.0.

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Figure 7. (a) Schematic illustration of the effects of the electrolytes on V₂O₅ electrode during the electrochemical reactions. [65] John Wiley & Sons. [© 2021 WileyVCH GmbH]. (b) Photos of V₂O₅·1.6H₂O/MXene electrodes after 10 d of immersing time in Zn(OTf)₂-TEP/H₂O-80% and Zn(OTf)₂-H₂O electrolytes for 10 d, and photos of the glass fiber separators in the cells with Zn(OTf)₂-TEP/H₂O-80% electrolyte after 1000 cycles and Zn(OTf)₂-H₂O electrolyte after battery failure. Reprinted from [66], Copyright (2023), with permission from Elsevier. (c) Calculated HOMO and LUMO energy levels of H₂O, NMP and Zn²⁺-NMP complex. Reprinted from [68], Copyright (2023), with permission from Elsevier.

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Figure 8. (a) Schematic diagram of the battery storage mechanism of raw electrolyte and PEA-modified electrolyte. [69] John Wiley & Sons. [© 2023 WileyVCH GmbH]. FESEM images of the VN_xO_y/C electrode after 100 cycles at the current density of 0.5 A g^-1 operated in the electrolyte of (b) pure H₂O and (c) the H₂O-50% PEG system. Reprinted from [70], Copyright (2023), with permission from Elsevier. Schematic illustration of the hybrid aqueous battery storage mechanism with (d) pristine electrolyte and (e) SDS-modified electrolyte. Reprinted from [71], Copyright (2022), with permission from Elsevier. (f) XRD patterns of the fully discharged KVO cathode after 100 cycles in three different electrolytes. Reproduced from [72], with permission from Springer Nature.

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Figure 9. (a) Illustration of TU inhibiting the formation of the byproduct SO₄^2- during charging. Reprinted from [73], Copyright (2023), with permission from Elsevier. (b) XRD patterns of Zn anodes after specific cycles at 2 mA cm^-2 in 2.5 + 0.2 electrolytes. (c) At 10 A g^-1, the cycling performances of the Zn | 2.5 + 0 | NVO and Zn | 2.5 + 0.2 | NVO coin cells; [74] John Wiley & Sons. [© 2022 WileyVCH GmbH]. (d) Schematic illustration of DETA serving as a multifunctional electrolyte additive. (e) XRD pattern of the cathode in different states. Reprinted with permission from [75]. Copyright (2023) American Chemical Society.

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Figure 10. (a) SEM images of Zn deposits at the electrode surface cycled in TMPNMF electrolyte after 800 cycles of Zn deposition/stripping. Reprinted from [85], Copyright (2023), with permission from Elsevier. (b) Design strategy of an EMC-based electrolyte with a microheterogeneous anion solvation network for high-voltage Zn/graphite cells. [87] John Wiley & Sons. [© 2020 WileyVCH GmbH]. (c) Comparison of the cycling performance (capacity retention versus cycle number) of Zn-MnO₂ batteries using the three electrolytes. Illustration is the optical image of two CR2032-type coin cells that are assembled using aqueous and hydrous organic electrolytes and stored for different storage times. Reprinted from [90], Copyright (2023), with permission from Elsevier. (d) Charge/discharge profiles of Zn/Zn symmetric cells in various electrolytes: DMF (black), AN (red), TMP (blue), H₂O (pink), TEP (green). Reprinted from [89], Copyright (2022), with permission from Elsevier.

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Figure 11. (a) Schematic illustration of the anode SEI formation in EIWE. [95] John Wiley & Sons. [© 2020 WileyVCH GmbH]. (b) Schemes illustrating different reaction processes of Zn²⁺ solvation structure and interfacial interaction between the Zn anode surface and electrolyte in AWCS electrolytes. Reprinted from [11], Copyright (2022), with permission from Elsevier. (c) Cycling stability at 20 C with a current density of 5 A g^-1. (d) Cycling stability of EG 40 at -20 C with a current density of 0.2 A g^-1. Reproduced from [97] with permission from the Royal Society of Chemistry. Snapshot of the MD simulation cell and corresponding RDF plots for (e) 1 M Zn(OTf)₂ in water, (f) 50% PC-sat. Insets in panels are the corresponding representative solvation structure within a 0.3 nm scale. (g) Anode-free Cu-ZnMn₂O₄ batteries in different electrolytes with a current density of 0.5 mA cm^-2 (350 mA g^-1). Reprinted with permission from [98]. Copyright (2022) American Chemical Society.

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Figure 12. Influence of various electrolyte additives on the solid electrolyte of the battery and related mechanisms. (a) Structure of the battery studied in nanomaterial-enhanced all-solid flexible Zn-carbon batteries. Reprinted with permission from [118]. Copyright (2010) American Chemical Society. (b) Schematic illustration of the preparation and structural characterization of the anti-freezing conductive organohydrogels. [117] John Wiley & Sons. [© 2017 WileyVCH Verlag GmbH & Co. KGaA, Weinheim]. (c) Schematic illustration of the strong hydrogen bonds between EG-waPUA, water and PAM in the AF-gel. Reproduced from [115] with permission from the Royal Society of Chemistry. (d) Schematic diagram of the synthesis of PAMPS/PAAM dual-network hydrogel. Reprinted from [116], Copyright (2022), with permission from Elsevier.

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Figure 13. Challenges facing the current hydrogel polymer electrolyte of ZIBs: (a) elastic stability of polyacrylamide (PAM)-hydrogel electrolytes after a day’s storage at various temperatures. Reproduced from [125]. CC BY 4.0. (b) Performance deterioration due to freezing of aqueous electrolyte at low temperatures. Reprinted with permission from [126]. Copyright (2022) American Chemical Society. (c) Low ion conductivity of electrolyte in low-temperature hydrogel solid electrolytes. (d) Photograph of PAMPS/PAAM hydrogel in a completely unloaded state and 50-cycle distortion. Reprinted from [116], Copyright (2022), with permission from Elsevier.

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Figure 14. (a) Formation energy from DFT calculations (PAM is viewed as one unit and the long chains are replaced by -CH₃). (b) Photos of the hydrogels at different temperatures. Reprinted from [139], Copyright (2022), with permission from Elsevier. (c) Schematic illustration of the fabrication of GG/SA and GG/SA/EG hydrogel electrolytes. Reprinted from [12], Copyright (2021), with permission from Elsevier. (d) Schematic diagram of the synthesis process of the PDZ-H electrolyte. (e) Digital photos of PDZ-H electrolyte at different temperatures from 20 to -40 C; [142] John Wiley & Sons. [© 2022 WileyVCH GmbH]. (f) Schematic illustration of the synthesis process at different states. Reprinted from [143], Copyright (2022), with permission from Elsevier.

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Figure 15. (a) Digital photos: the PAM hydrogel electrolytes were placed at 25 C and 50% humidity for 30 d. Reproduced from [125]. CC BY 4.0. (b) DFT optimized structures of PAM-H₂O-Gly, PAM-H₂O-EG, PVA-H₂O-Gly, and PAA-H₂O-Gly. (c) Configuration and bonding mechanism of the anti-freezing and anti-drying gel electrolyte. (d) Optical images of PAM-H₂O-Gly with different Gly content after 30 d in ambient environment. Reproduced from [147], with permission from Springer Nature. (e) Design principle of elastomer-coated alginate/PAM (polyacrylamide) organohydrogel electrolyte. Reproduced from [125]. CC BY 4.0.

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Figure 16. (a) Schematic view of GO phosphonation reaction and PAM-PGO structure showing hydrogen bonds. Reprinted from [156], Copyright (2022), with permission from Elsevier. (b) Schematic illustration of the synthesis route of the MMT-PAM hydrogel through a controllable accelerated polymerization mechanism. (c) Schematic illustration of the synthesis route of the MMT-PAM hydrogel through a traditional route; (b), (c) Reprinted from [157], Copyright (2023), with permission from Elsevier. (d) Illustration of the spatial structure of PVA-based hydrogel electrolyte in flexible solid-state Zn-polymer batteries with practical functions. Reprinted from [136], Copyright (2021), with permission from Elsevier.

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Figure 17. (a) Schematic illustration of the swelling method for the preparation of OHE, and structure merits of OHE. Reprinted from [163], Copyright (2022), with permission from Elsevier. (b) Schematic illustration of the construction of an ion migration channel under the applied electric field. Reproduced from [158]. CC BY 4.0.

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Figure 18. (a) Macroscopic morphologies of the SPE-Zn membrane, ILPE-Zn-4 membrane and ILPE-Zn-5 membrane. Reproduced from [175]. CC BY 4.0. (b) Representation of an effectual Zn-ionic conducting pathway through the space-charge layers of the neighboring SiO₂ grains. [172] John Wiley & Sons. [© 2019 Wiley Periodicals, Inc.].

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Figure 19. (a) Schematic illustration of the overall preparation process of the SPEs (PVHF/MXene-g-PMA). (b) Zn/MnHCF full cell discharge capacity at different temperatures; (a), (b) Reproduced from [100] with permission from the Royal Society of Chemistry. (c) Electrochemical performance at different temperatures. [14] John Wiley & Sons. [© 2020 WILEYVCH Verlag GmbH & Co. KGaA, Weinheim].

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