Digital Twin‐Driven All‐Solid‐State Battery: Unraveling the Physical and Electrochemical Behaviors

Abstract

The digital twin technique has been broadly utilized to efficiently and effectively predict the performance and problems associated with real objects via a virtual replica. However, the digitalization of twin electrochemical systems has not been achieved thus far, owing to the large amount of required calculations of numerous and complex differential equations in multiple dimensions. Nevertheless, with the help of continuous progress in hardware and software technologies, the fabrication of a digital twin‐driven electrochemical system and its effective utilization have become a possibility. Herein, a digital twin‐driven all‐solid‐state battery with a solid sulfide electrolyte is built based on a voxel‐based microstructure. Its validity is verified using experimental data, such as effective electronic/ionic conductivities and electrochemical performance, for LiNi0.70Co0.15Mn0.15O2 composite electrodes employing Li6PS5Cl. The fundamental performance of the all‐solid‐state battery is scrutinized by analyzing simulated physical and electrochemical behaviors in terms of mass transport and interfacial electrochemical reaction kinetics. The digital twin model herein reveals valuable but experimentally inaccessible time‐ and space‐resolved information including dead particles, specific contact area, and charge distribution in the 3D domain. Thus, this new computational model is bound to rapidly improve the all‐solid‐state battery technology by saving the research resources and providing valuable insights.

Rate Limitations in Composite Solid-State Battery Electrodes: Revealing Heterogeneity with Operando Microscopy

“…Recent studies have begun to probe these phenomena in solid-state composite cathodes. Minnmann et al and Park et al examined the effects of electrode microstructure on power density by probing the impacts of the relative electronic and ionic conductivities of the electrode. , Bielefeld et al and Shi et al combined modeling with electrochemical measurements to examine the effect of particle size on percolation pathways and accessible capacities. , A variety of ex situ , in situ , and operando techniques have also been used to visualize lithiation throughout the composite cathode, including Raman imaging, electron energy loss spectroscopy (EELS), , X-ray absorption spectroscopy (XAS), time-of-flight secondary ion mass spectrometry (ToF SIMS), and Kelvin probe force microscopy (KPFM) …”

Cycling Performance and Limitations of LiNiO2 in Solid-State Batteries

“…Apart from chemo-mechanical degradation and gassing, performance decay of SSB cells is usually attributed to SE degradation at the interface with the other cell components. , To gain insight into the chemical nature of the degradation products, ex situ X-ray photoelectron spectroscopy (XPS, Figure ) measurements were carried out. Figure a,b shows the S 2p and P 2p core-level spectra for the pristine Li 6 PS 5 Cl SE and for the uncycled and cycled composite cathodes.…”

High-Energy All-Solid-State Organic–Lithium Batteries Based on Ceramic Electrolytes

“…The uniform distribution of materials within a composite electrode may enhance electrochemical performance in multiple ways. The uniform distribution of solid electrolyte alone would form a better connected ionic transport network that could improve performance on all fronts. − Further homogenized distribution of the active material would enable faster charge transport within the active material and more efficient charge transfer between the active material and the electrolyte. , To probe the importance of each step, we measured the conductivity of both the electrodes made from hand-milled and cryomilled powders. EIS of Cu/PTO-Li 3 PS 4 /Cu cells was performed in the temperature range of 25–100 °C, and the conductivity values were extracted by fitting the Nyquist plot following a procedure reported for mixed electronic–ionic conductors (Figure S3).…”