Additive manufacturing of LiNi1/3Mn1/3Co1/3O2 battery electrode material via vat photopolymerization precursor approach

Ana C Martinez; Alexis Maurel; Ana P Aranzola; Sylvie Grugeon; Stéphane Panier; Loic Dupont; Jose A Hernandez-Viezcas; Bhargavi Mummareddy; Beth L Armstrong; Pedro Cortes; Sreeprasad T Sreenivasan; Eric MacDonald

doi:10.1038/s41598-022-22444-1

Additive manufacturing of LiNi_1/3Mn_1/3Co_1/3O₂ battery electrode material via vat photopolymerization precursor approach

Sci Rep. 2022 Nov 8;12(1):19010. doi: 10.1038/s41598-022-22444-1.

Authors

Ana C Martinez^#¹, Alexis Maurel^#², Ana P Aranzola³, Sylvie Grugeon^{4

5}, Stéphane Panier^{4

6}, Loic Dupont^{4

5}, Jose A Hernandez-Viezcas⁷, Bhargavi Mummareddy⁸, Beth L Armstrong⁹, Pedro Cortes⁸, Sreeprasad T Sreenivasan¹⁰, Eric MacDonald^{11

12}

Affiliations

¹ Department of Aerospace and Mechanical Engineering, The University of Texas at El Paso, El Paso, TX, 79968, USA. acmartinezm@utep.edu.
² Department of Aerospace and Mechanical Engineering, The University of Texas at El Paso, El Paso, TX, 79968, USA. amaurel@utep.edu.
³ Department of Aerospace and Mechanical Engineering, The University of Texas at El Paso, El Paso, TX, 79968, USA.
⁴ Laboratoire de Réactivité et de Chimie des Solides, UMR CNRS 7314, Hub de l'Énergie, Université de Picardie Jules Verne, 80039, Amiens Cedex, France.
⁵ RS2E, Réseau Français sur le Stockage Électrochimique de l'Energie, FR CNRS 3459, 80039, Amiens, France.
⁶ Laboratoire des Technologies Innovantes, LTI-EA 3899, Université de Picardie Jules Verne, 80025, Amiens, France.
⁷ Department of Chemistry and Biochemistry, The University of Texas at El Paso, El Paso, TX, 79968, USA.
⁸ Department of Civil, Environmental, and Chemical Engineering, Youngstown State University, Youngstown, OH, 44555, USA.
⁹ Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, TN, 37831, USA.
¹⁰ Department of Chemistry and Biochemistry, The University of Texas at El Paso, El Paso, TX, 79968, USA. sreenivasan@utep.edu.
¹¹ Department of Aerospace and Mechanical Engineering, The University of Texas at El Paso, El Paso, TX, 79968, USA. emac@utep.edu.
¹² Manufacturing Science Division, Oak Ridge National Laboratory, Oak Ridge, TN, 37830, USA. emac@utep.edu.

^# Contributed equally.

Abstract

Additive manufacturing, also called 3D printing, has the potential to enable the development of flexible, wearable and customizable batteries of any shape, maximizing energy storage while also reducing dead-weight and volume. In this work, for the first time, three-dimensional complex electrode structures of high-energy density LiNi_1/3Mn_1/3Co_1/3O₂ (NMC 111) material are developed by means of a vat photopolymerization (VPP) process combined with an innovative precursor approach. This innovative approach involves the solubilization of metal precursor salts into a UV-photopolymerizable resin, so that detrimental light scattering and increased viscosity are minimized, followed by the in-situ synthesis of NMC 111 during thermal post-processing of the printed item. The absence of solid particles within the initial resin allows the production of smaller printed features that are crucial for 3D battery design. The formulation of the UV-photopolymerizable composite resin and 3D printing of complex structures, followed by an optimization of the thermal post-processing yielding NMC 111 is thoroughly described in this study. Based on these results, this work addresses one of the key aspects for 3D printed batteries via a precursor approach: the need for a compromise between electrochemical and mechanical performance in order to obtain fully functional 3D printed electrodes. In addition, it discusses the gaps that limit the multi-material 3D printing of batteries via the VPP process.