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Interfacial-engineering-enabled practical low-temperature sodium metal battery

Nature Nanotechnology volume 17, pages 269–277 (2022)Cite this article

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Abstract

Solid-state sodium (Na) batteries have received extensive attention as a promising alternative to room-temperature liquid electrolyte Na-ion batteries and high-temperature liquid electrode Na–S batteries because of safety concerns. However, the major issues for solid-state Na batteries are a high interfacial resistance between solid electrolytes and electrodes, and Na dendrite growth. Here we report that a yttria-stabilized zirconia (YSZ)-enhanced beta-alumina solid electrolyte (YSZ@BASE) has an extremely low interface impedance of 3.6 Ω cm2 with the Na metal anode at 80 °C, and also exhibits an extremely high critical current density of ~7.0 mA cm–2 compared with those of other Li- and Na-ion solid electrolytes reported so far. With a trace amount of eutectic NaFSI–KFSI molten salt at the electrolyte/cathode interface, a quasi-solid-state Na/YSZ@BASE/NaNi0.45Cu0.05Mn0.4Ti0.1O2 full cell achieves a high capacity of 110 mAh g–1 with a Coulombic efficiency >99.99% and retains 73% of the cell capacity over 500 cycles at 4C and 80 °C. Extensive characterizations and theoretical calculations prove that the stable β-NaAlO2-rich solid–electrolyte interphase and strong YSZ support matrix play a critical role in suppressing the Na dendrite as they maintain robust interfacial contacts, lower electronic conduction and prevent the continual reduction of BASE through oxygen-ion compensation.

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Fig. 1: Characterization of YSZ@BASE.
Fig. 2: Characterization of the YSZ@BASE/Na interface at RT and 80 °C.
Fig. 3: Fundamentals of YSZ@BASE/Na metal interfacial reaction at 80 °C.
Fig. 4: Dendrite suppression capability and interface chemistry of YSZ@BASE at 80 °C.
Fig. 5: Stability mechanism of YSZ@BASE/Na interface at 80 °C.
Fig. 6: Demonstration of a high-voltage cell with a YSZ@BASE and Na anode.

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All relevant data that support the plots within this article and other findings of this study are available from the corresponding authors upon request.

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Acknowledgements

This work was supported by US Department of Energy (DOE) under award no. DEEE0008856 at the University of Maryland (UMD) and Office of Electricity (OE) at Pacific Northwest National Laboratory (PNNL). We appreciate useful discussions with I. Gyuk of the DOE-OE Grid Storage Program. T.D. is grateful for financial support from the Engie Chuck Edwards Memorial Fellowship at UMD. Additional support is from North Carolina A&T State University (NC A&T) through a faculty start-up fund. Some of the TEM and XPS analyses were conducted in the William R. Wiley Environmental Molecular Sciences Laboratory, a national scientific user facility sponsored by the DOE’s Office of Biological and Environmental Research and located at PNNL. PNNL is a multiprogram laboratory operated by Battelle Memorial Institute for the DOE under contract DE-AC05-76RL01830. We also thank J. F. Bonnett for the YSZ@BASE conversion, J. Song for cathode preparation, M. E. Bowden for the XRD analysis, and M. H. Engelhard for the XPS characterization. Part of the SEM analysis was done by K. Nowlin at the Joint School of Nanoscience and Nanoengineering, an academic collaboration between NC A&T and the University of North Carolina at Greensboro.

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  1. These authors contributed equally: Tao Deng, Xiao Ji.

Authors and Affiliations

  1. Department of Chemical and Biomolecular Engineering, University of Maryland, College Park, MD, USA

    Tao Deng, Xiao Ji, Longsheng Cao, Xiulin Fan & Chunsheng Wang

  2. Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland, WA, USA

    Tao Deng, Hee-Jung Chang, Hui Wang, Xiaolin Li, David Reed, Ji-Guang Zhang & Vincent L. Sprenkle

  3. Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, WA, USA

    Lianfeng Zou & Chongmin Wang

  4. Department of Applied Engineering Technology, North Carolina A&T State University, Greensboro, NC, USA

    Obinna Chiekezi, Toyosi R. Adebisi & Xiaochuan Lu

  5. Energy Storage & Advanced Transportation Department, Idaho National Laboratory, Idaho Falls, ID, USA

    Bin Li

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Contributions

T.D., Chunsheng Wang and X.L. proposed the research and designed the experiment. T.D., X.L., O.C., L.C., T.R.A. and H.-J.C. performed the experiments (material synthesis, characterization, battery fabrication and testing, and so on). X.J., T.D., Chungsheng Wang and X.L. conceived the simulation protocol, and X.J. carried out the simulations. L.Z., Chongmin Wang and X.F. performed the TEM, FIB, STEM–EDS analyses. T.D., Chungsheng Wang and X.L. analysed the data and wrote the manuscript with suggestions and comments from all the authors. All the authors contributed to the interpretation of the results.

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Correspondence to Chunsheng Wang or Xiaochuan Lu.

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Peer review information Nature Nanotechnology thanks Yoon Seok Jung, Guoxiu Wang and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Figs. 1–30, Discussion and Tables 1–4.

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Deng, T., Ji, X., Zou, L. et al. Interfacial-engineering-enabled practical low-temperature sodium metal battery. Nat. Nanotechnol. 17, 269–277 (2022). https://doi.org/10.1038/s41565-021-01036-6

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