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Cited by 434Advancements in Battery MaterialsBattery Modeling and ManagementAdvanced Battery Materials and Technologies

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Fast-charging high-energy lithium-ion batteries via implantation of amorphous silicon nanolayer in edge-plane activated graphite anodes

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Kim, Namhyung, Chae, Sujong, Ma, Jiyoung, Ko, Minseong, Cho, Jaephil·2017·Nature Communications
DOI 10.1038/s41467-017-00973-yPMC PMC5634447
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Abstract

As fast-charging lithium-ion batteries turn into increasingly important components in forthcoming applications, various strategies have been devoted to the development of high-rate anodes. However, despite vigorous efforts, the low initial Coulombic efficiency and poor volumetric energy density with insufficient electrode conditions remain critical challenges that have to be addressed. Herein, we demonstrate a hybrid anode via incorporation of a uniformly implanted amorphous silicon nanolayer and edge-site-activated graphite. This architecture succeeds in improving lithium ion transport and minimizing initial capacity losses even with increase in energy density. As a result, the hybrid anode exhibits an exceptional initial Coulombic efficiency (93.8%) and predominant fast-charging behavior with industrial electrode conditions. As a result, a full-cell demonstrates a higher energy density (≥1060 Wh l −1 ) without any trace of lithium plating at a harsh charging current density (10.2 mA cm −2 ) and 1.5 times faster charging than that of conventional graphite.

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Crossref · 10.1038/s41467-017-00973-y

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Figures

Fig. 1 Schematic of the procedures for fabrication and characterization of SEAG. a Fabrication of SEAG: the adsorbed Ni penetrated graphite via catalytic hydrogenation at 1000 °C, which led to edge-plane activation on the surface of graphite. b Cross-sectional illustration showing the detailed structural characteristics of SEAG. c HR-TEM image of a Ni nanoparticle embedded in EAG. d Relationship between the square root of the scan rate and the peak current: the slope indicates the relative electrochemically active surface area. SEM images of pristine graphite e, graphite with adsorbed Ni on its surface f, and the SEAG composite g. Scale bars, 5 nm c, 5 μm e, f, g
Fig. 1 Schematic of the procedures for fabrication and characterization of SEAG. a Fabrication of SEAG: the adsorbed Ni penetrated graphite via catalytic hydrogenation at 1000 °C, which led to edge-plane activation on the surface of graphite. b Cross-sectional illustration showing the detailed structural characteristics of SEAG. c HR-TEM image of a Ni nanoparticle embedded in EAG. d Relationship between the square root of the scan rate and the peak current: the slope indicates the relative electrochemically active surface area. SEM images of pristine graphite e, graphite with adsorbed Ni on its surface f, and the SEAG composite g. Scale bars, 5 nm c, 5 μm e, f, gCC BY · PubMed Central
Fig. 2 Physical properties of SEAG. a XRD pattern of SEAG. b Statistical analysis of the particle-size distribution of pristine graphite (gray) and SEAG (red). c Tap density and d specific surface area of pristine graphite (gray), EAG (orange), SEAG (red), and conventional NG (blue)
Fig. 2 Physical properties of SEAG. a XRD pattern of SEAG. b Statistical analysis of the particle-size distribution of pristine graphite (gray) and SEAG (red). c Tap density and d specific surface area of pristine graphite (gray), EAG (orange), SEAG (red), and conventional NG (blue)CC BY · PubMed Central
Fig. 3 Detailed investigation of cross-sectional SEAG. a SEM image of SEAG in cross-sectional view: SEAG maintained a rigid inner graphite framework despite going through catalytic hydrogenation. HAADF-STEM images with EDS mapping analysis of b the activated holes and silicon nanolayer on the graphite surface and d the nickel nanoparticle piercing the core of graphite. e Magnified HAADF-STEM image of d. HR-TEM images at the interfacial region of c SEAG and f a nickel nanoparticle; fast Fourier-transform images are shown in the insets. The nickel nanoparticle was clearly separated from silicon by the graphitic carbon shell, which prevented the unfavorable formation of Ni silicide. Scale bars, a 5 μm, b 1 μm, c, f 10 nm, d 200 nm, e 30 nm
Fig. 3 Detailed investigation of cross-sectional SEAG. a SEM image of SEAG in cross-sectional view: SEAG maintained a rigid inner graphite framework despite going through catalytic hydrogenation. HAADF-STEM images with EDS mapping analysis of b the activated holes and silicon nanolayer on the graphite surface and d the nickel nanoparticle piercing the core of graphite. e Magnified HAADF-STEM image of d. HR-TEM images at the interfacial region of c SEAG and f a nickel nanoparticle; fast Fourier-transform images are shown in the insets. The nickel nanoparticle was clearly separated from silicon by the graphitic carbon shell, which prevented the unfavorable formation of Ni silicide. Scale bars, a 5 μm, b 1 μm, c, f 10 nm, d 200 nm, e 30 nmCC BY · PubMed Central
Fig. 4 Electrochemical characterization of various anodes in half-cell configurations. a Voltage profiles of SEAG, SEAG with Ni silicide, and graphite in the 1st cycle. b Plots of reversible capacity and cycling CE vs. cycle number for SEAG, SEAG with Ni silicide, and graphite over 50 cycles. The a 1st cycle and b cycling test were carried out at current densities of 0.35 and 1.75 mA cm−2, respectively (1C = 3.5 mA cm−2). c Galvanostatic charge capacities of SEAG under various lithiation current densities from 0.35 to 10.5 mA cm−2, compared to SEAG with Ni silicide and graphite. d Voltage profiles during charging process of SEAG and graphite, measured at increasing current densities from 3.5 to 10.5 mA cm−2; the inset shows a plot of SOC divided into galvanostatic/potentiostatic stages at each current density
Fig. 4 Electrochemical characterization of various anodes in half-cell configurations. a Voltage profiles of SEAG, SEAG with Ni silicide, and graphite in the 1st cycle. b Plots of reversible capacity and cycling CE vs. cycle number for SEAG, SEAG with Ni silicide, and graphite over 50 cycles. The a 1st cycle and b cycling test were carried out at current densities of 0.35 and 1.75 mA cm−2, respectively (1C = 3.5 mA cm−2). c Galvanostatic charge capacities of SEAG under various lithiation current densities from 0.35 to 10.5 mA cm−2, compared to SEAG with Ni silicide and graphite. d Voltage profiles during charging process of SEAG and graphite, measured at increasing current densities from 3.5 to 10.5 mA cm−2; the inset shows a plot of SOC divided into galvanostatic/potentiostatic stages at each current densityCC BY · PubMed Central
Fig. 5 Fast-charging performance of full-cells with anodes of graphite and the SEAG composite. Voltage profiles at charging current density of a 5.1 mA cm−2, b 7.7 mA cm−2, and c 10.2 mA cm−2. Fast-charging cycling performance in the potential range from 4.35 to 2.7 V for 50 cycles under increasing charging current densities of d 5.1 mA cm−2, e 7.7 mA cm−2, and f 10.2 mA cm−2. The discharging current density was fixed at 1.7 mA cm−2 in all cycling tests. g Time required to charge to 80% of SOC at each current density. h Plot of volumetric energy density vs. applied charging current density for graphite and SEAG. The volumetric energy densities were calculated from the total thickness of both the cathode and anode, considering the electrode volume expansion at the lithiated state during the first cycle. In the electrode composed of SEAG, a volumetric energy density of 1060 Wh l−1 was delivered under an applied charging current density of 10.2 mA cm−2
Fig. 5 Fast-charging performance of full-cells with anodes of graphite and the SEAG composite. Voltage profiles at charging current density of a 5.1 mA cm−2, b 7.7 mA cm−2, and c 10.2 mA cm−2. Fast-charging cycling performance in the potential range from 4.35 to 2.7 V for 50 cycles under increasing charging current densities of d 5.1 mA cm−2, e 7.7 mA cm−2, and f 10.2 mA cm−2. The discharging current density was fixed at 1.7 mA cm−2 in all cycling tests. g Time required to charge to 80% of SOC at each current density. h Plot of volumetric energy density vs. applied charging current density for graphite and SEAG. The volumetric energy densities were calculated from the total thickness of both the cathode and anode, considering the electrode volume expansion at the lithiated state during the first cycle. In the electrode composed of SEAG, a volumetric energy density of 1060 Wh l−1 was delivered under an applied charging current density of 10.2 mA cm−2CC BY · PubMed Central
Fig. 6 Dimensional and morphological changes of the electrodes after fast-charging cycles. a Irreversible increase in thickness of the electrode at the delithiated state under 7.7 mA cm−2 for 10 cycles. Photographs of b SEAG electrode and e graphite electrode after 50 cycles at 7.7 mA cm−2. Top view and cross-sectional SEM images of c, d SEAG electrode and f, g graphite electrode. Yellow dash line indicates the deposited Li, which reacted with the electrolyte. Scale bars, c 100 μm, d, g 50 μm, f 400 μm
Fig. 6 Dimensional and morphological changes of the electrodes after fast-charging cycles. a Irreversible increase in thickness of the electrode at the delithiated state under 7.7 mA cm−2 for 10 cycles. Photographs of b SEAG electrode and e graphite electrode after 50 cycles at 7.7 mA cm−2. Top view and cross-sectional SEM images of c, d SEAG electrode and f, g graphite electrode. Yellow dash line indicates the deposited Li, which reacted with the electrolyte. Scale bars, c 100 μm, d, g 50 μm, f 400 μmCC BY · PubMed Central

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Citations

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Research works printed but not linked: 1

  1. Wu, H. & Cui, Y. Designing nanostructured Si anodes for high energy lithium ion batteries. Nano Today 7, 414–429 (2012). · DOI

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Metadata

Authors
Kim, N., Chae, S., Ma, J., Ko, M., & Cho, J.
Affiliations
Ulsan National Institute of Science and Technology (KR)
Corresponding author
  • Ko, Minseong
  • Cho, Jaephil
ORCID
Venue
Nature Communications
Publisher
Springer Science and Business Media LLC
Published
2017-10-09
Volume
8
Issue
1
Pages
812-812
ISSN
2041-1723 (ISSN-L)
DOI
10.1038/s41467-017-00973-y
PMC
PMC5634447
OpenAlex
W2764301473
Cited by
434
References
54
Citations by year
2026: 34 · 2025: 66 · 2024: 67 · 2023: 51 · 2022: 57 · 2021: 47 · 2020: 44 · 2019: 46 · 2018: 22
FWCI
12.73
Type
journal article
Language
en
Open access
Licence
Locations
  • Nature Communications (publishedVersion, cc-by)
  • Europe PMC (PubMed Central) (publishedVersion, cc-by)
  • PubMed Central (publishedVersion, cc-by)
  • PubMed (publishedVersion)
  • RePEc: Research Papers in Economics (submittedVersion)
  • DOAJ (DOAJ: Directory of Open Access Journals) (submittedVersion)
  • DOAJ (DOAJ: Directory of Open Access Journals) (submittedVersion, cc-by-sa)
  • Scholarworks@UNIST (Ulsan National Institute of Science and Technology) (submittedVersion)
Funders
Samsung
Topics
  • Physical Sciences › Engineering › Electrical and Electronic Engineering › Advancements in Battery Materials
  • Physical Sciences › Engineering › Automotive Engineering › Battery Modeling and Management
  • Physical Sciences › Engineering › Electrical and Electronic Engineering › Advanced Battery Materials and Technologies
Keywords
lithium-ion batteries, fast charging, graphite anode, hybrid anode, Coulombic efficiency, lithium plating, energy density, lithium ion transport

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