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Self-smoothing anode for achieving high-energy lithium metal batteries under realistic conditions



Despite considerable efforts to stabilize lithium metal anode structures and prevent dendrite formation, achieving long cycling life in high-energy batteries under realistic conditions remains extremely difficult due to a combination of complex failure modes that involve accelerated anode degradation and the depletion of electrolyte and lithium metal. Here we report a self-smoothing lithium–carbon anode structure based on mesoporous carbon nanofibres, which, coupled with a lithium nickel–manganese–cobalt oxide cathode with a high nickel content, can lead to a cell-level energy density of 350–380 Wh kg−1 (counting all the active and inactive components) and a stable cycling life up to 200 cycles. These performances are achieved under the realistic conditions required for practical high-energy rechargeable lithium metal batteries: cathode loading ≥4.0 mAh cm−2, negative to positive electrode capacity ratio ≤2 and electrolyte weight to cathode capacity ratio ≤3 g Ah−1. The high stability of our anode is due to the amine functionalization and the mesoporous carbon structures that favour smooth lithium deposition.

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Journal peer review information: Nature Nanotechnology thanks James Tour, Karim Zaghib and the other anonymous reviewer(s) for their contribution to the peer review of this work.

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This work was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the US Department of Energy (DOE) through the Advanced Battery Materials Research (BMR) program (Battery500 Consortium) under contract no. DE-AC02-05CH11231. The transmission electron microscopy, STEM, SEM, energy-dispersive X-ray diffraction, X-ray diffraction, X-ray photoemission spectroscopy, Raman, Fourier transform infrared spectroscopy and computational calculations were conducted in the William R. Wiley Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility sponsored by the DOE’s Office of Biological and Environmental Research and located at PNNL. PNNL is operated by Battelle for the DOE under contract DE-AC05-76RL01830. We thank D. Zhao of Fudan University for discussion during the exploration to solve Li wetting. We thank H. Lee of PNNL for optimizing the figures.

Author information

J.L. and C.N. conceived the research and designed the experiments. C.N. performed the material synthesis, characterization, electrochemical measurements and analysed the data. J.M., X.W., Z.L. and L.M. performed some experiments in the exploration to solve Li wetting. L.L. and C.W. carried out the in situ STEM experiment. D.M. performed the molecular dynamics simulation. H.P., W.X., J.X. and J.-G.Z. revised the manuscript. C.N. and J.L. wrote the paper with input from all the authors.

Competing interests

The authors declare no competing interests.

Correspondence to Jun Liu.

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    Supplementary Figures 1–10; Supplementary Tables 1 and 2.

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    • Rodrigo V. Salvatierra
    •  & James M. Tour

    Nature Nanotechnology (2019)

Fig. 1: Illustration of self-smoothing behaviour in the Li–C anode.
Fig. 2: Characterizations of Li infiltration into carbon film.
Fig. 3: Self-smoothing behaviour in a Li–C anode during electrochemical cycling.
Fig. 4: Traditional test of Li-C||NMC622 cell with a low-loading cathode, excess Li and flooded electrolyte.
Fig. 5: Electrochemical performance of Li–C||NMC622 and Li–C||NMC811 cells under the realistic constrained conditions required for high energy densities.