This work uses VPP printing combined with a precursor approach to circumvent these problems. However, it presents two critical challenges: (1) the increase in viscosity of the composite resin and (2) the detrimental light scattering caused by the presence of solid particles in the resin, increasing the difficulty of printing. Since battery materials often consist of oxide compounds, their direct addition to the resin followed by 3D printing of battery electrodes is thus conceivable. This technique has been employed to 3D print composite resins highly loaded with ceramic particles of Al 2O 3 13, ZrO 2 14, and SiO 2 15, 16, 17. During the VPP process, a photopolymerizable resin is selectively polymerized to a crosslinked layer upon UV light exposure, and the procedure is repeated to create a macrostructure layer after layer with features down to 100 nm 12. Recent research in this area has made significant advances by utilizing 3D printing, owing to its ability to build intricate and tailored shapes with high resolution 8, 9, 10, 11. Unfortunately, the intercalation of independent 3D electrodes has often resulted in short circuits caused by the numerous surface irregularities. Based on these promising aspects, the development of nanorods and post arrays as a 3D independent electrode has been achieved by electrochemical growth onto a substrate, followed by electrophoretic deposition of the battery electroactive material 5, 6, 7. Consequently, the 3D batteries have shown a superior specific capacity, areal energy, and power density than traditional 2D batteries. Compared to conventional parallel-plate (2D) battery configuration, three-dimensional (3D) battery architectures can exhibit enhanced electrochemical performances due to their greater electroactive surface area, and an improved lithium ion diffusion 3, 4. In addition, it discusses the gaps that limit the multi-material 3D printing of batteries via the VPP process.ĭriven by the growing demand for portable consumer electronics and electric vehicles, in-depth research efforts have been devoted in the past years to improving energy and power density of lithium-ion batteries 1, 2. 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. 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. The absence of solid particles within the initial resin allows the production of smaller printed features that are crucial for 3D battery design. 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. In this work, for the first time, three-dimensional complex electrode structures of high-energy density LiNi 1/3Mn 1/3Co 1/3O 2 (NMC 111) material are developed by means of a vat photopolymerization (VPP) process combined with an innovative precursor approach. 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.
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