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Scalable synthesis of silicon-nanolayer-embedded graphite for high-energy lithium-ion batteries

Nature Energy volume 1, Article number: 16113 (2016) Cite this article

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An Author Correction to this article was published on 09 March 2020

Abstract

Existing anode technologies are approaching their limits, and silicon is recognized as a potential alternative due to its high specific capacity and abundance. However, to date the commercial use of silicon has not satisfied electrode calendering with limited binder content comparable to commercial graphite anodes for high energy density. Here we demonstrate the feasibility of a next-generation hybrid anode using silicon-nanolayer-embedded graphite/carbon. This architecture allows compatibility between silicon and natural graphite and addresses the issues of severe side reactions caused by structural failure of crumbled graphite dust and uncombined residue of silicon particles by conventional mechanical milling. This structure shows a high first-cycle Coulombic efficiency (92%) and a rapid increase of the Coulombic efficiency to 99.5% after only 6 cycles with a capacity retention of 96% after 100 cycles, with an industrial electrode density of >1.6 g cm−3, areal capacity loading of >3.3 mAh cm−2, and <4 wt% binding materials in a slurry. As a result, a full cell using LiCoO2 has demonstrated a higher energy density (1,043 Wh l−1) than with standard commercial graphite electrodes.

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Figure 1: Schematic of fabrication and characterization of the SGC hybrid.
Figure 2: Electrochemical characterization of various electrodes.
Figure 3: Series of SEM images for electrode changes before and after 50 cycles.
Figure 4: Electrochemical comparison of a full cell between graphite (G) and SGC hybrid.
Figure 5: In situ TEM characterization of the SGC hybrid during lithiation.

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Acknowledgements

This work was supported by the IT R&D programme of the Ministry of Trade, Industry & Energy/Korea Evaluation Institute of Industrial Technology (MOTIE/KEIT) (Development of Li-rich Cathode and Carbon-free Anode Materials for High Capacity/High Rate Lithium Secondary Batteries, 10046306) and the 2016 Research Fund (1.160033.01) of UNIST (Ulsan National Institute of Science and Technology). Also, Y.C. acknowledges support from the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies, Battery Materials Research Program of the US Department of Energy.

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Authors and Affiliations

  1. Department of Energy Engineering, School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea

    Minseong Ko, Sujong Chae, Jiyoung Ma, Namhyung Kim, Hyun-Wook Lee & Jaephil Cho

  2. Department of Materials Science and Engineering, Stanford University, Stanford, California 94305, USA

    Hyun-Wook Lee & Yi Cui

  3. Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA

    Yi Cui

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  1. Minseong Ko
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Contributions

M.K. conceived and designed the experiments, and performed data interpretation. M.K. prepared the samples and carried out the main experiments. S.C. assisted with the data interpretation and designed the experimental scheme; H.-W.L. conducted in situ TEM characterization and detailed discussion on analytic results. J.M. assisted with sample preparation and performed the energy-dispersive spectroscopy measurement. N.K. provided data analysis. M.K., S.C., H.-W.L., Y.C. and J.C. co-wrote the paper.

Corresponding authors

Correspondence to Hyun-Wook Lee, Yi Cui or Jaephil Cho.

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The authors declare no competing financial interests.

Supplementary information

Supplementary Information

Supplementary Figures 1–9, Supplementary Tables 1 and 2, Supplementary Notes, Supplementary References. (PDF 938 kb)

Supplementary Video 1

Lithiation of a Si nanolayer coated on the surface of empty volume space. The Si nanolayer can expand toward empty volume space upon lithiation, leading to no rupture and interference between Si and graphite. The movie is played at 10× speed. (MP4 16592 kb)

Supplementary Video 2

Lithiation of a Si nanolayer located in the gap between graphite layers. The Si nanolayer located in the gap between the graphite layers remains intact without any cracks and contact losses upon lithiation. The movie is played at 7× speed. (MP4 11800 kb)

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Ko, M., Chae, S., Ma, J. et al. Scalable synthesis of silicon-nanolayer-embedded graphite for high-energy lithium-ion batteries. Nat Energy 1, 16113 (2016). https://doi.org/10.1038/nenergy.2016.113

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