Room-temperature liquid metal engineered iron current collector enables stable and dendrite-free sodium metal batteries in carbonate electrolytes

doi:10.1016/j.jmst.2021.11.034

Abstract

Abstract:

Metallic sodium (Na) is believed to be a promising anode material for sodium-ion batteries (SIBs) due to its low electrochemical potential, high theoretical specific capacity, superior electrical conductivity, and so on. However, issues such as high chemical activity, the growth of Na dendrites, large volume change, and unstable interface impede its practical application. We design a cheap iron (Fe)-based substrate decorated by a thin liquid metal Ga layer for stable and dendrite-free Na metal anodes in low-cost carbonate electrolytes. The inherent mechanism of Ga-based liquid metal in inhibiting the growth of Na dendrites was revealed for the first time. Liquid metal Ga with sodiophilic property can act as nucleation seeds to decrease the nucleation barrier and induce homogeneous Na⁺ flux, resulting in uniform and dendrite-free Na deposition. Full cells with Na₃V₂(PO₄)₃ cathode were also assembled to verify the practical application ability of the modified Na metal anode. Under the regulation of the liquid metal layer, the Coulombic efficiency, cycling life, and capacity of batteries are obviously enhanced. The strategy proposed here cannot only reduce the cost of batteries but also improve their electrochemical and safety performance.

Key words: Stainless steel, Current collector, Sodium metal anode, Liquid metal, Carbonate electrolyte

Chuanliang Wei, Liwen Tan, Yuchan Zhang, Huiyu Jiang, Baojuan Xi, Shenglin Xiong, Jinkui Feng. Room-temperature liquid metal engineered iron current collector enables stable and dendrite-free sodium metal batteries in carbonate electrolytes[J]. J. Mater. Sci. Technol., 2022, 115: 156-165.

Figures/Tables 8

Fig. 1. (a) Schematic showing the fabrication process and inherent advantages of Ga-SSF. (b) A photograph of CF. (c) A photograph of SSF. (d) A photograph of SSF with a drop of liquid-state Ga. (e) A photograph of Ga-SSF. The diameter of these slices was 1.6 cm. (f-h) Top-view SEM images of CF, SSF, and Ga-SSF, respectively. (i) Cross-sectional SEM image of Ga-SSF.

Fig. 2. (a) XRD patterns of metallic Ga, SSF, and Ga-SSF. (b) XRD patterns of SSF after immersing in Li-ion, Na-ion, K-ion, Mg-ion electrolytes, and deionized water for 30 days. (c-f) SEM images of SSF after immersing in Li-ion, Na-ion, K-ion electrolytes, and deionized water for 30 days, respectively. (g) XPS full spectra of SSF and Ga-SSF. (h) High-resolution XPS spectra of Ga2p in Ga-SSF. (i) Contact angel of liquid electrolyte (1 M NaPF6 in EC/DEC with 5% FEC) on CF, SSF, and Ga-SSF.

Fig. 3. (a-c) The initial CV curves of Ga-SSF, CF, and SSF at 0.1 mV s-1 in -0.1 to 3 V, respectively. (d) XRD patterns after depositing 0.2 mAh cm-2 of Na on Ga-SSF at 0.1 mA cm-2. (e) Voltage-capacity curves of CF, SSF, and Ga-SSF. (f) The nucleation overpotential of Na on CF, SSF, and Ga-SSF. (g, h) Coulombic efficiency of CF, SSF, and Ga-SSF. (i) The 40th plating/stripping curves of Na on CF, SSF, and Ga-SSF in (h). (j) Voltage-time curves of symmetric cells for CF, SSF, and Ga-SSF at 0.5 mA cm-2. (k) An enlarged image at a certain time range in (j).

Fig. 4. Low-magnification SEM images. (a-c) Top-view SEM images after depositing 0.5, 1, and 2 mA h cm-2 of Na on CF at 0.2 mA cm-2, respectively. (d-f) Top-view SEM images after depositing 0.5, 1, and 2 mA h cm-2 of Na on SSF at 0.2 mA cm-2, respectively. (g-i) Top-view SEM images after depositing 0.5, 1, and 2 mA h cm-2 of Na on Ga-SSF at 0.2 mA cm-2, respectively.

Fig. 5. High-magnification SEM images. (a-c) Top-view SEM images after depositing 0.5, 1, and 2 mAh cm-2 of Na on CF at 0.2 mA cm-2, respectively. (d-f) Top-view SEM images after depositing 0.5, 1, and 2 mAh cm-2 of Na on SSF at 0.2 mA cm-2, respectively. (g-i) Top-view SEM images after depositing 0.5, 1, and 2 mAh cm-2 of Na on Ga-SSF at 0.2 mA cm-2, respectively.

Fig. 6. (a-c) Cross-sectional SEM images after depositing 2 mAh cm-2 of Na on CF, SSF, and Ga-SSF at 0.2 mA cm-2, respectively. (d-f) Enlarged SEM images in (a-c). (g-i) Nyquist plots after depositing 2 mAh cm-2 of Na on CF, SSF, and Ga-SSF at 0.2 mA cm-2, respectively.

Fig. 7. (a) Schematic showing the structure of Na metal full cells. (b) The rate capability of NVP-CFNa, NVP-SSFNa, and NVP-Ga-SSFNa full cells at different rates. (c-e) Charge-discharge curves of full cells at different rates. (f) Cycling performance of full cells at 2 C.

Fig. 8. (a-c) Schematics showing the deposition mechanism of Na metal anode on CF, SSF, and Ga-SSF, respectively.

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