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Simulation of Micro/Nanopowder Mixing Characteristics for Dry Spray Additive Manufacturing of Li-Ion Battery Electrodes

[+] Author and Article Information
Brandon Ludwig

Mechanical and Aerospace Engineering,
Missouri University of Science and Technology,
400 West 13th Street,
Rolla, MO 65409

Jin Liu, Yangtao Liu, Zhangfeng Zheng, Yan Wang

Mechanical Engineering,
Worchester Polytechnic Institute,
100 Institute Road,
Worchester, MA 01609

Heng Pan

Mechanical and Aerospace Engineering,
Missouri University of Science and Technology,
400 West 13th Street,
Rolla, MO 65409
e-mail: hp5c7@mst.edu

1Corresponding author.

Contributed by the Manufacturing Engineering Division of ASME for publication in the JOURNAL OF MICRO- AND NANO-MANUFACTURING. Manuscript received June 15, 2017; final manuscript received August 21, 2017; published online September 27, 2017. Assoc. Editor: Yayue Pan.

J. Micro Nano-Manuf 5(4), 040902 (Sep 27, 2017) (8 pages) Paper No: JMNM-17-1033; doi: 10.1115/1.4037769 History: Received June 15, 2017; Revised August 21, 2017

A new dry spraying additive manufacturing method for Li-ion batteries has been developed to replace the conventional slurry-casting technique for manufacturing Li-ion battery electrodes. A dry spray manufacturing process can allow for the elimination of the time- and energy-intensive slurry drying process needed due to the use solvents to make the electrodes. Previous studies into the new manufacturing method have shown successful fabrication of electrodes which have strong electrochemical and mechanical performance. Li-ion battery electrodes typically consist of three basic materials: active material (AM), binder particle additives (BPA), and conductive particle additives (CPA). In this paper, a discrete element method (DEM) simulation was developed and used to study the mixing characteristics of dry electrode powder materials. Due to the size of the particles being in the submicron to micron size range, the mixing characteristics are heavily dependent on van der Waals adhesive forces between the particles. Therefore, the effect the Li-ion battery electrode material surface energy has on the mixing characteristics was studied. Contour plots based on the DEM simulation results where the surface energy components of selected material types are changed were used to predict the mixing characteristics of different particle systems. For the cases studied, it is found that experimental mixing results are representative of the results of the DEM simulations.

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Figures

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Fig. 1

Solvent-free manufacturing process: (a) schematic of dry electrostatic spraying system, (b) representation of poorly mixed Li-ion battery electrode powders with agglomerations of additive particles, and (c) representation of well mixed Li-ion battery electrode powders with uniform distribution of additive particles

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Fig. 2

Contact mechanics of colliding particles: (a) contact interface and radius representation due to the collision of i and j particles and (b) representation of the i − j particle overlap due to collision

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Fig. 3

AM-BPA mixing. DEM simulation snapshots of AM-BPA mixing showing (a) premixing, (b) aggregation, and (c) intermixing. Analytical (d) and DEM (e) contour plots showing similar mixing behavior. (f) Comparison of mixing time found in DEM cases where intermixing and aggregation occurs.

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Fig. 4

AM-CPA mixing. DEM simulation snapshots of AM-CPA mixing showing (a) premixing, (b) intermixing, and (c) aggregation. (d) DEM contour plot showing the number of CPA in contact with the AM surface when the AM polar component is 2 mN m−1. (e) DEM contour plot showing the number of CPA in contact with the AM surface when the AM polar component is 100 mN m−1. (f) CPAs showing increased contact with higher polar surface energy AM as compared to low polar surface energy. (g) Comparison of mixing time found in DEM cases where intermixing and aggregation occurs.

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Fig. 5

BPA-CPA mixing: confirmation of analytical modeling results where a predicted intermixed case is confirmed by a DEM simulation (a) and where a predicted aggregation case is confirmed by another DEM simulation (b)

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Fig. 6

AM-BPA-CPA mixing: (a) DEM simulation showing mixing behavior of all three materials when the AM polar surface energy is 2 mN m−1 and (b) DEM simulation showing the mixing behavior of all three materials when the AM polar surface energy is increased to 100 mN m−1

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Fig. 7

Experimental mixing comparison: (a) SEM micrograph showing PVDF (representing BPA) particles attached to the surface of LCO (representing AM), (b) DEM confirmation of the experimental mixing result of AM-BPA with BPA particles attached to the AM surface, (c) SEM micrograph showing PVDF particles embedded within Super C65 carbon (representing CPA), and (d) DEM confirmation of the experimental mixing result of CPA-BPA with BPA particles embedded within the CPA

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