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Research Papers

Freestanding Flexible Si Nanoparticles–Multiwalled Carbon Nanotubes Composite Anodes for Li-Ion Batteries and Their Prelithiation by Stabilized Li Metal Powder

[+] Author and Article Information
K. Yao

Materials Science and Engineering,
Florida State University,
Tallahassee, FL 32310;
Aero-Propulsion, Mechatronics and Energy
Center (AME),
Florida State University,
Tallahassee, FL 32310;
High-Performance Materials Institute (HPMI),
Florida State University,
Tallahassee, FL 32310

R. Liang

High-Performance Materials Institute (HPMI),
Florida State University,
Tallahassee, FL 32310;
Department of Industrial and Manufacturing
Engineering,
Florida A&M University—Florida State
University College of Engineering,
Tallahassee, FL 32310

J. P. Zheng

Aero-Propulsion, Mechatronics and Energy
Center (AME),
Florida State University,
Tallahassee, FL 32310;
Department of Electrical and Computer
Engineering,
Florida A&M University—Florida State University
College of Engineering,
Tallahassee, FL 32310
e-mail: zheng@eng.fsu.edu

Manuscript received December 23, 2015; final manuscript received March 20, 2016; published online xxxx x, xxxx. Assoc. Editor: Partha Mukherjee.

J. Electrochem. En. Conv. Stor. 13(1), 011004 (Apr 19, 2016) (6 pages) Paper No: JEECS-15-1026; doi: 10.1115/1.4033180 History: Received December 23, 2015; Revised March 20, 2016

Freestanding flexible Si nanoparticles–multiwalled carbon nanotubes (SiNPs–MWNTs) composite paper anodes for Li-ion batteries (LIBs) have been prepared using a combination of ultrasonication and pressure filtration. No conductive additive, binder, or metal current collector is used. The SiNPs–MWNTs composite electrode material achieves first cycle specific discharge and charge capacities of 2298 and 1492 mAh/g, respectively. To address the first cycle irreversibility, stabilized Li metal powder (SLMP) has been utilized to prelithiate the composite anodes. As a result, the first cycle irreversible capacity loss is reduced from 806 to 28 mAh/g and the first cycle coulombic efficiency is increased from 65% to 98%. The relationship between different SLMP loadings and cell performance has been established to understand the prelithiation process of SLMP and to optimize the construction of Si-based cells. A cell containing the prelithiated anode is able to deliver charge capacity over 800 mAh/g without undergoing the initial discharge process, which enables the exploration of novel cathode materials.

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Figures

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Fig. 1

(a) A freestanding SiNPs–MWCNTs composite paper demonstrating its flexibility, (b) half-inch composite paper electrode, and (c) the electrode in (b) with SLMP pressed onto the surface

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Fig. 2

(a) Cross-sectional and (b) top-view SEM images of SiNPs–MWCNTs composite paper

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Fig. 3

Voltage profiles from first and second cycles of SiNPs–MWCNTs anode

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Fig. 4

Representative first cycle voltage profile of SLMP-prelithiated composite paper anode

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Fig. 5

(a) Open circuit potential, (b) first cycle charge/discharge capacity ratio, and (c) first cycle discharge (triangles) and charge (circles) capacities of SLMP-prelithiated cells as a function of SLMP to anode mass ratio. Inset in (b) shows the relationship for SLMP/anode mass ratio in the range of 0–0.4.

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Fig. 6

First cycle specific charge capacity (without first discharge) of SLMP-prelithiated cells and SLMP utilization versus SLMP/anode mass ratio

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Fig. 7

Schematic of three possible outcomes of SLMP toward Si particles. Note that the sizes of SLMP and Si particles are not true to scale.

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Fig. 8

SEM image of SiNPs–MWCNTs composite anode after prelithiation by SLMP

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