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Folding Graphene Film Yields High Areal Energy Storage in Lithium-Ion Batteries

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Center for Multidimensional Carbon Materials (CMCM), Institute for Basic Science (IBS), Ulsan 44919, Republic of Korea
Department of Energy Engineering, School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
§ Department of Chemistry, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
School of Materials Science and Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
Cite this: ACS Nano 2018, 12, 2, 1739–1746
Publication Date (Web):January 19, 2018
Copyright © 2018 American Chemical Society

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    We show that a high energy density can be achieved in a practical manner with freestanding electrodes without using conductive carbon, binders, and current collectors. We made and used a folded graphene composite electrode designed for a high areal capacity anode. The traditional thick graphene composite electrode, such as made by filtering graphene oxide to create a thin film and reducing it such as through chemical or thermal methods, has sluggish reaction kinetics. Instead, we have made and tested a thin composite film electrode that was folded several times using a water-assisted method; it provides a continuous electron transport path in the fold regions and introduces more channels between the folded layers, which significantly enhances the electron/ion transport kinetics. A fold electrode consisting of SnO2/graphene with high areal loading of 5 mg cm–2 has a high areal capacity of 4.15 mAh cm–2, well above commercial graphite anodes (2.50–3.50 mAh cm–2), while the thickness is maintained as low as ∼20 μm. The fold electrode shows stable cycling over 500 cycles at 1.70 mA cm–2 and improved rate capability compared to thick electrodes with the same mass loading but without folds. A full cell of fold electrode coupled with LiCoO2 cathode was assembled and delivered an areal capacity of 2.84 mAh cm–2 after 300 cycles. This folding strategy can be extended to other electrode materials and rechargeable batteries.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsnano.7b08489.

    • Calculation of full cell energy density; measurement of the resistance before and after folding an rG-O/SnO2 film; XRD pattern of rG-O/SnO2 film; XPS measurement of G-O and rG-O films and rG-O/SnO2 film; TGA curve for the rG-O/SnO2 film; SEM images show the cross section of the rG-O/SnO2 film_1 mg cm–2; SEM images of a fold electrode; photos that show achieving two folds of an rG-O/SnO2 strip; galvanostatic discharge/charge curves of film electrodes and fold electrodes with different loading; cycle performance for film electrodes in terms of areal capacity; discharge curves for the Fold_5 electrode at different rates from 0.2C to 3C; ex situ TEM and XPS for the Fold_5 electrode after 100 cycles; electrode swelling measured by cross-sectional SEM images; photos of Film_5 and Fold_5 electrodes and counter Li foil after cycling; ex situ XPS spectra of C 1s and F 1s for the Fold_5 electrode after 100 cycles; data on the cathode and the precycle performance of the full cell (PDF)

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