pytrax: A simple and efficient random walk implementation for calculating the directional tortuosity of images

Given the huge advances in tomographic imaging capability in recent years, image analysis has become a powerful means of measuring transport and structural properties of porous materials. One of the most important material characteristics is the tortuosity, which is difficult to measure experimentally. We present pytrax: (tortuosity from random axial movements) a simple and efficient random walk method implemented in python to calculate the average tortuosity and orthogonal directional tortuosity components of an image. The code works for both two and three-dimensional images and completes a statistically significant number of walks in parallel for large images in a few minutes using a standard desktop computer. By comparison, a Lattice Boltzmann or finite element simulation on similar sized images can take several hours

Fluid Transport Properties from 3D Tomographic Images of Electrospun Carbon Electrodes for Flow Batteries

Three-dimensional x-ray computer tomography images were obtained of electrospun poly(acrylonitrile) electrodes for a flow battery. The materials were imaged before and after carbonization. Information about the internal morphology; local fiber size and porosity, was analyzed and provided key insights into both the electrospinning and carbonizing processes. It was found that traditional imaging techniques may not be suitable for materials generated through electrospinning as it is a highly dynamic process. The fiber size tended to vary throughout the process while the porosity was relatively constant. Viscous flow was modelled through the material using the Lattice Boltzmann Method and the 3D flow fields that resulted provided further information about the role of heterogenous features on the performance of an electrospun electrode in a flow battery. The local porosity of the material had the largest effect on the material’s flow dynamics

The effect of non-uniform compression on the performance of polymer electrolyte fuel cells

The mechanical compression used in the construction of PEFCs improves effective current collection and gas sealing, however it results in structural deformation of the MEA, affecting reactant transport with adverse consequences for the electrochemical performance of the cell. The present study uses X-ray CT to characterise MEA under compression and determine effective properties of the porous domain. The comprehensive modelling approach couples a structural model of the MEA under compression to a multi-phase, non-isothermal electrochemical performance model. Liquid water saturation in the cathode domain that promotes mass transport losses is validated with neutron radiography. Here, the structural model considers the fuel cell stacking process at three compressions and highlights the non-uniform distribution of porosity and effective properties under non-uniform cell compression, affecting localised current distribution and water transport. An increase in compression showed a negligible effect on the performance in the activation region, the performance was marginally improved in the ohmic region and significantly affected in mass transport region, promoting cell flooding. The non-uniform compression effects are found to be important considerations for robust modelling studies as it increases the nonuniformity in localised current, temperature and flooding that would further alter the durability of the fuel cell

Three-dimensional image based modelling of transport parameters in lithium-sulfur batteries

An elemental sulfur electrode was imaged with X-ray micro and nano computed tomography and segmented into its constituent phases. Morphological parameters including phase fractions and pore and particle size distributions were calculated directly from labelled image data, and flux based simulations were performed to determine the effective molecular diffusivity of the pore phase and electrical conductivity of the conductive carbon and binder phase, Deff and σeff, that can be used as an input for Li-S battery modelling. In addition to its crucial role in providing electrical conductivity within the sulfur electrode, the intrinsic porosity of the carbon binder domain was found to significantly influence Li-ion transport within the electrode. Neglecting this intrinsic porosity results in an overestimation of the electrical conductivity within the sulfur electrode, and an underestimation of the tortuosity of the Li-ion conducting phase by ca. 56%. The derivation of effective transport parameters directly from image data may aid in the development of more realistic models of Li-S battery systems by reducing the reliance on empirical correlations, and the uncertainties arising from assumptions made in these correlations

An Advanced Microstructural and Electrochemical Datasheet on 18650 Li-Ion Batteries with Nickel-Rich NMC811 Cathodes and Graphite-Silicon Anodes

Cylindrical lithium-ion batteries are used across a wide range of applications from spacesuits to automotive vehicles. Specifically, many manufacturers are producing cells in the 18650 geometry i.e. a steel cylinder of diameter and length ca. 18 and 65 mm, respectively. One example is the LG Chem INR18650 MJ1 (nominal values: 3.5 Ah, 3.6 V, 12.2 Wh). This article describes the electrochemical performance and microstructural assembly of such cells, where all the under-pinning data is made openly available for the benefit of the wider community. The charge-discharge capacity is reported for 400 operational cycles via the manufacturer's guidelines along with full-cell, individual electrode coating and particle 3D imaging. Within the electrochemical data, the distinction between protocol transition, beginning-of-life (BoL) capacity loss, and prolonged degradation is outlined and, subsequently, each aspect of the microstructural characterization is broken down into key metrics that may aid in understanding such degradation (e.g. electrode assembly layers, coating thickness, areal loading, particle size and shape). All key information is summarized in a quick-access advanced datasheet in order to provide an initial baseline of information to guide research paths, inform experiments and aid computational modellers

Microstructural Evolution of Battery Electrodes During Calendering

Calendering is a crucial manufacturing process in the optimization of battery performance and lifetime due to its significant effect on the 3D electrode microstructure. By conducting an in situ calendering experiment on lithium-ion battery cathodes using X-ray nano-computed tomography, here we show that the electrodes composed of large particles with a broad size distribution experience heterogeneous microstructural self-arrangement. At high C-rates, the performance is predominantly restricted by sluggish solid-state diffusion, which is exacerbated by calendering due to the increased microstructural and lithiation heterogeneity, leading to active material underutilization. In contrast, electrodes consisting of small particles are structurally stable with more homogeneous deformation and a lower tortuosity, showing a much higher rated capacity that is less sensitive to calendering densification. Finally, the dependence of performance on the dual variation of both porosity and electrode thickness is investigated to provide new insights into the microstructural optimization for different applications in electrode manufacturing

Virtual unrolling of spirally-wound lithium-ion cells for correlative degradation studies and predictive fault detection

A spirally-wound LG 18650 MJ1 lithium-ion battery was imaged in 3D before and after 1061 cycles using X-ray computed tomography. The battery's capacity had faded to 79% of its initial value and some of that fade was attributed to delamination in the innermost region of the ‘jelly-roll’ structure. A method for virtually unrolling the jelly-roll and analysing it in different coordinates is presented. The method allows efficient comparison of the position and shape of the electrodes at different times and highlights imperfections present in the jelly-roll before cycling which were shown to nucleate the delamination of the electrode

Correlative acoustic time-of-flight spectroscopy and X-ray imaging to investigate gas-induced delamination in lithium-ion pouch cells during thermal runaway

It remains difficult to detect internal mechanical deformation and gas-induced degradation in lithium-ion batteries, especially outside specialized diagnostics laboratories. In this work, we demonstrate that electrochemical acoustic time-of-flight (EA-ToF) spectroscopy can be used as an insightful and field-deployable diagnostic/prognostic technique to sense the onset of failure. A 210 mAh commercial lithium-ion cell undergoing thermal abuse testing is probed with in situ and operando EA-ToF spectroscopy, together with simultaneous fractional thermal runaway calorimetry (FTRC) and synchrotron X-ray imaging. The combination of X-ray imaging and EA-ToF analysis provides new understanding into the through-plane mechanical deformation in lithium-ion batteries through direct visualisation and the acoustic ToF response. Internal structural changes, such as gas-induced delamination, are identified using EA-ToF spectroscopy due to variations in the attenuation and signal peak shifts. This is corroborated using X-ray imaging, demonstrating EA-ToF spectroscopy as a promising technique for detecting onset of battery failure

Lignin-derived electrospun freestanding carbons as alternative electrodes for redox flow batteries

Based on information provided the embargo period/end date is 12 monthsBased on information provided the embargo period/end date is 12 month

Identifying Defects in Li-Ion Cells Using Ultrasound Acoustic Measurements

Identification of the state-of-health (SoH) of Li-ion cells is a vital tool to protect operating battery packs against accelerated degradation and failure. This is becoming increasingly important as the energy and power densities demanded by batteries and the economic costs of packs increase. Here, ultrasonic time-of-flight analysis is performed to demonstrate the technique as a tool for the identification of a range of defects and SoH in Li-ion cells. Analysis of large, purpose-built defects across multiple length scales is performed in pouch cells. The technique is then demonstrated to detect a microscale defect in a commercial cell, which is validated by examining the acoustic transmission signal through the cell. The location and scale of the defects are confirmed using X-ray computed tomography, which also provides information pertaining to the layered structure of the cells. The demonstration of this technique as a methodology for obtaining direct, non-destructive, depth-resolved measurements of the condition of electrode layers highlights the potential application of acoustic methods in real-time diagnostics for SoH monitoring and manufacturing processes