A Molecular-Sieving Interphase Towards Low-Concentrated Aqueous Sodium-Ion Batteries

doi:10.1007/s40820-024-01340-5

Abstract

Abstract:

Aqueous sodium-ion batteries are known for poor rechargeability because of the competitive water decomposition reactions and the high electrode solubility. Improvements have been reported by salt-concentrated and organic-hybridized electrolyte designs, however, at the expense of cost and safety. Here, we report the prolonged cycling of ASIBs in routine dilute electrolytes by employing artificial electrode coatings consisting of NaX zeolite and NaOH-neutralized perfluorinated sulfonic polymer. The as-formed composite interphase exhibits a molecular-sieving effect jointly played by zeolite channels and size-shrunken ionic domains in the polymer matrix, which enables high rejection of hydrated Na⁺ ions while allowing fast dehydrated Na⁺ permeance. Applying this coating to electrode surfaces expands the electrochemical window of a practically feasible 2 mol kg^-1 sodium trifluoromethanesulfonate aqueous electrolyte to 2.70 V and affords Na₂MnFe(CN)₆//NaTi₂(PO₄)₃ full cells with an unprecedented cycling stability of 94.9% capacity retention after 200 cycles at 1 C. Combined with emerging electrolyte modifications, this molecular-sieving interphase brings amplified benefits in long-term operation of ASIBs.

Key words: Molecular sieving effect, Electrode coatings, Aqueous sodium ion batteries, Dilute aqueous electrolytes

Tingting Liu, Han Wu, Hao Wang, Yiran Jiao, Xiaofan Du, Jinzhi Wang, Guangying Fu, Yaojian Zhang, Jingwen Zhao, Guanglei Cui. A Molecular-Sieving Interphase Towards Low-Concentrated Aqueous Sodium-Ion Batteries[J]. Nano-Micro Letters, 2024, 16(1): 144-.

Tingting Liu, Han Wu, Hao Wang, Yiran Jiao, Xiaofan Du, Jinzhi Wang, Guangying Fu, Yaojian Zhang, Jingwen Zhao, Guanglei Cui. [J]. Nano-Micro Letters, 2024, 16(1): 144-.

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URL: https://www.qk.sjtu.edu.cn/nml/EN/10.1007/s40820-024-01340-5

https://www.qk.sjtu.edu.cn/nml/EN/Y2024/V16/I1/144

Figures/Tables 5

Fig. 1 a ATR-FTIR spectra of Nafion-Na and Nafion-Na/NaX. b, c TEM spectra and d SAXS patterns of Nafion-Na and Nafion-Na/NaX. e Arrhenius plots of ionic conductivity for Nafion-Na, Nafion-Na/NaX and PVDF/NaX membranes (infiltrated with 2 m NaOTF)

Fig. 2 a The digital photograph of NaOTF permeability test device and b the corresponding Na⁺/OTF⁻ molar ratios of the water side. c Schematic of the test device for water permeability. d The water flux of CM, CM@Nafion-Na, and CM@Nafion-Na/NaX. e ATR-FTIR spectra of 2 m NaOTF, 2 m NaOTF saturated Nafion-Na and Nafion-Na/NaX membranes. f Schematic of Nafion-Na/NaX for molecular sieving

Fig. 3 ESWs of 9 m NaOTF on the unprotected working electrode and 2 m NaOTF, on unprotected, Nafion-Na protected, and Nafion-Na/NaX protected working electrodes at a scan rate of 1.0 mV s⁻¹

Fig. 4 a CV curves of NMF//NTP full cells equipped with unprotected, Nafion-Na protected and Nafion-Na/NaX protected electrodes using 2 m NaOTF (performed at 1 mV s⁻¹). Voltage profiles and H₂ signals of NMF//NTP cells in the 2 m NaOTF electrolyte with b unprotected, c Nafion-Na protected and d Nafion-Na/NaX protected electrodes at 140 mA g⁻¹

Fig. 5 a Cycle performance of the NMF//NTP full cells in 2 m NaOTF with unprotected, Nafion-Na protected, and Nafion-Na/NaX protected electrodes at 140 mA g⁻¹ (based on the mass of NMF). b ICP-OES results of Mn and Fe contents in electrolytes of full cells after 200 cycles. SEM images of unprotected, Nafion-Na protected, and Nafion-Na/NaX protected cathodes c-e before and f-h after 200 cycles

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