Revealing meso-structure dynamics in additive manufacturing of energy storage via operando coherent X-ray scattering

3D printing is an emerging technology for the fabrication of energy storage devices, offering advan-tages over traditional manufacturing methods. However, optimization and design of such devices re-quires an understanding of the meso-structure formation during the 3D printing process. This study utilizes operando coherent X-ray scattering, X-ray Photon Correlation Spectroscopy (XPCS), to study the spatiotemporally-resolved far-from-equilibrium dynamics during direct ink writing 3D printing. Lithium Titanate (LTO) based ink is prepared and rheologically tested for its shear-thinning properties. Two-time intensity-intensity functions are calculated to be used in subsequent quantitative analysis, which allows for an overall characterization of the dynamics, description of an initial fast decorrelation and identi-fication of sudden rearrangements of subdomains of the sample. The results show the dynamics to be anisotropic, spatiotemporally heterogenous and marked by distinct rearrangement events, all of which impact the electrochemical performance of energy storage devices. The studied 3D printing ink is used to fabricate electrodes which are then electrochemically tested, showing good performance in cycling and retaining structural integrity. This work furthers the understanding of the far-from-equilibrium material dynamics during 3D printing, giving quantitative characterization of this process, and highlights aspects of structure formation relevant to the electrochemical performance of the resultant energy storage device. (c) 2021 Published by Elsevier Ltd.

Automated summary

The study utilizes X-ray scattering and X-ray photon correlation spectroscopy to investigate the dynamic changes in material structure during 3D printing, revealing anisotropic and spatiotemporally heterogeneous dynamics which impact the electrochemical performance of the resulting energy storage device.