Lithium-Ion Battery 3D Printing: From Thermoplastic Material Extrusion to Vat Photopolymerization Process

Abstract

Transitioning from conventional 2D to complex 3D lithium-ion battery (LIB) architectures will increase electrochemically active surface area and lithium-ion diffusion paths, leading to improved specific capacity and power performance [1]. Our recent in-depth modeling studies and preliminary experiments [2] involving the simulation of a classical Ragone plot that exhibits the energy-power relationship illustrated that a gyroid 3D battery architecture has +158% performance at a high current density of 6C, in comparison to planar geometry. The fabrication of complex electrodes has been widely investigated through an electrochemically-assisted templated growth of current collector arrays, followed by electrophoretic deposition of the electroactive material [3]. However, such an approach is limited in geometries, and the interpenetration of both electrode networks often results in short circuits due to surface defects. The latter can be addressed with the geometric freedom of additive manufacturing, colloquially known as 3D printing, which paves the way toward fabricating complex shape-conformable battery components [4]. Here, a summary of our recent works on lithium-ion battery 3D printing via thermoplastic material extrusion will be presented [5-9]. In particular, the development of printable composite filaments (Graphite-, LiFePO4-, Li2TP-, PEO/LiTFSI-, SiO2-, Ag/Cu-based) corresponding to each part of a classical LIB (electrodes, electrolyte, separator, current collectors), as well as the importance of introducing an adequate plasticizer (such as poly(ethylene glycol) dimethyl ether average Mn 500 for polylactic acid) as an additive to enhance both printability and further electrochemical performances, will be addressed. Printing of the complete LIB in a single step using multi-material printing options, and the implementation of a solvent-free protocol [7] will also be discussed. Finally, the capability of vat photopolymerization processes, including stereolithography, digital light processing and two-photon polymerization (offering a greater resolution down to 0.1µm), to print high resolution LIB components will be presented.[1] J.W. Long, B. Dunn, D.R. Rolison, H.S. White, Three-dimensional battery architectures, Chemical Reviews 104(10) (2004) 4463-4492.[2] A. Maurel, M. Haukka, E. MacDonald, L. Kivijärvi, E. Lahtinen, H. Kim, M. Armand, A. Cayla, A. Jamali, S. Grugeon, L. Dupont, S. Panier, Considering lithium-ion battery 3D-printing via thermoplastic material extrusion and polymer powder bed fusion, Additive Manufacturing (2020) 101651.[3] L. Taberna, S. Mitra, P. Poizot, P. Simon, J.M. Tarascon, High rate capabilities Fe3O4-based Cu nano-architectured electrodes for lithium-ion battery applications, Nature Materials 5(7) (2006) 567-573.[4] H. Ragones, S. Menkin, Y. Kamir, A. Gladkikh, T. Mukra, G. Kosa, D. Golodnitsky, Towards smart free form-factor 3D printable batteries, Sustainable Energy & Fuels 2(7) (2018) 1542-1549.[5] A. Maurel, M. Courty, B. Fleutot, H. Tortajada, K. Prashantha, M. Armand, S. Grugeon, S. Panier, L. Dupont, Highly Loaded Graphite-Polylactic Acid Composite-Based Filaments for Lithium-Ion Battery Three-Dimensional Printing, Chemistry of Materials 30(21) (2018) 7484-7493.[6] A. Maurel, S. Grugeon, B. Fleutot, M. Courty, K. Prashantha, H. Tortajada, M. Armand, S. Panier, L. Dupont, Three-Dimensional Printing of a LiFePO4/Graphite Battery Cell via Fused Deposition Modeling, Scientific Reports 9(1) (2019) 18031.[7] A. Maurel, R. Russo, S. Grugeon, S. Panier, L. Dupont, Environmentally Friendly Lithium-Terephthalate/Polylactic Acid Composite Filament Formulation for Lithium-Ion Battery 3D-Printing via Fused Deposition Modeling, ECS Journal of Solid State Science and Technology 10(3) (2021) 037004.[8] A. Maurel, M. Armand, S. Grugeon, B. Fleutot, C. Davoisne, H. Tortajada, M. Courty, S. Panier, L. Dupont, Poly(Ethylene Oxide)-LiTFSI Solid Polymer Electrolyte Filaments for Fused Deposition Modeling Three-Dimensional Printing, Journal of the Electrochemical Society 167(7) (2020).[9] A. Maurel, H. Kim, R. Russo, S. Grugeon, M. Armand, S. Panier, L. Dupont, Ag-Coated Cu/Polylactic Acid Composite Filament for Lithium and Sodium-Ion Battery Current Collector Three-Dimensional Printing via Thermoplastic Material Extrusion, Frontiers in Energy Research 9(70) (2021).