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The temporally and spatially resolved tracking of lithium intercalation and electrode degradation processes are crucial for detecting and understanding performance losses during the operation of lithium-batteries. Here, high-throughput X-ray computed tomography has enabled the identification of mechanical degradation processes in a commercial Li/MnO 2 primary battery and the indirect tracking of lithium diffusion; furthermore, complementary neutron computed tomography has identified the direct lithium diffusion process and the electrode wetting by the electrolyte. Virtual electrode unrolling techniques provide a deeper view inside the electrode layers and are used to detect minor fluctuations which are difficult to observe using conventional three dimensional rendering tools. Moreover, the ‘unrolling’ provides a platform for correlating multi-modal image data which is expected to find wider application in battery science and engineering to study diverse effects e.g. electrode degradation or lithium diffusion blocking during battery cycling. The combination of X-ray and neutron CT enables 4D studies, i.e. to explore the evolution of 3D structures with time. Here the authors apply this approach to a Li-ion primary cell, revealing elsewhere unseen trends in the spatial distribution of performance aided by a new ‘unrolling’ methodology.

Driving range and fast charge capability of electric vehicles are heavily dependent on the 3D microstructure of lithium-ion batteries (LiBs) and substantial fundamental research is required to optimise electrode design for specific operating conditions. Here we have developed a full microstructure-resolved 3D model using a novel X-ray nano-computed tomography (CT) dual-scan superimposition technique that captures features of the carbon-binder domain. This elucidates how LiB performance is markedly affected by microstructural heterogeneities, particularly under high rate conditions. The elongated shape and wide size distribution of the active particles not only affect the lithium-ion transport but also lead to a heterogeneous current distribution and non-uniform lithiation between particles and along the through-thickness direction. Building on these insights, we propose and compare potential graded-microstructure designs for next-generation battery electrodes. To guide manufacturing of electrode architectures, in-situ X-ray CT is shown to reliably reveal the porosity and tortuosity changes with incremental calendering steps. The 3D microstructure of the electrode predominantly determines the electrochemical performance of Li-ion batteries. Here, the authors show that the microstructural heterogeneities lead to non-uniform Li insertion and current distribution while graded-microstructures improve the performance.

Proton exchange membrane fuel cells, consuming hydrogen and oxygen to generate clean electricity and water, suffer acute liquid water challenges. Accurate liquid water modelling is inherently challenging due to the multi-phase, multi-component, reactive dynamics within multi-scale, multi-layered porous media. In addition, currently inadequate imaging and modelling capabilities are limiting simulations to small areas (<1 mm 2 ) or simplified architectures. Herein, an advancement in water modelling is achieved using X-ray micro-computed tomography, deep learned super-resolution, multi-label segmentation, and direct multi-phase simulation. The resulting image is the most resolved domain (16 mm 2 with 700 nm voxel resolution) and the largest direct multi-phase flow simulation of a fuel cell. This generalisable approach unveils multi-scale water clustering and transport mechanisms over large dry and flooded areas in the gas diffusion layer and flow fields, paving the way for next generation proton exchange membrane fuel cells with optimised structures and wettabilities. Accurate liquid water modelling is challenging. Here the authors use X-ray micro-computed tomography, deep learned super-resolution, multi-label segmentation, and direct multiphase simulation to simulate fuel cell and guide fuel cell design.

The performance of lithium ion electrodes is hindered by unfavorable chemical heterogeneities that pre-exist or develop during operation. Time-resolved spatial descriptions are needed to understand the link between such heterogeneities and a cell’s performance. Here, operando high-resolution X-ray diffraction-computed tomography is used to spatially and temporally quantify crystallographic heterogeneities within and between particles throughout both fresh and degraded Li x Mn 2 O 4 electrodes. This imaging technique facilitates identification of stoichiometric differences between particles and stoichiometric gradients and phase heterogeneities within particles. Through radial quantification of phase fractions, the response of distinct particles to lithiation is found to vary; most particles contain localized regions that transition to rock salt LiMnO 2 within the first cycle. Other particles contain monoclinic Li 2 MnO 3 near the surface and almost pure spinel Li x Mn 2 O 4 near the core. Following 150 cycles, concentrations of LiMnO 2 and Li 2 MnO 3 significantly increase and widely vary between particles. Dynamic chemical and structural heterogeneities within electrodes are known to lead to battery degradation and failure. Here, the authors show that X-ray diffraction computed tomography can be used to spatially quantify the dynamic crystallographic states of electrodes as they operate and degrade.

The phase separation dynamics in graphitic anodes significantly affects lithium plating propensity, which is the major degradation mechanism that impairs the safety and fast charge capabilities of automotive lithium-ion batteries. In this study, we present comprehensive investigation employing operando high-resolution optical microscopy combined with non-equilibrium thermodynamics implemented in a multi-dimensional (1D+1D to 3D) phase-field modeling framework to reveal the rate-dependent spatial dynamics of phase separation and plating in graphite electrodes. Here we visualize and provide mechanistic understanding of the multistage phase separation, plating, inter/intra-particle lithium exchange and plated lithium back-intercalation phenomena. A strong dependence of intra-particle lithiation heterogeneity on the particle size, shape, orientation, surface condition and C-rate at the particle level is observed, which leads to early onset of plating spatially resolved by a 3D image-based phase-field model. Moreover, we highlight the distinct relaxation processes at different state-of-charges (SOCs), wherein thermodynamically unstable graphite particles undergo a drastic intra-particle lithium redistribution and inter-particle lithium exchange at intermediate SOCs, whereas the electrode equilibrates much slower at low and high SOCs. These physics-based insights into the distinct SOC-dependent relaxation efficiency provide new perspective towards developing advanced fast charge protocols to suppress plating and shorten the constant voltage regime. Improved understanding of the spatial dynamics in graphite electrodes is needed to improve fast-charging protocols for Li-ion batteries. Here, authors highlight that lithiation heterogeneity leads to early lithium plating onset and find distinct relaxation behaviors at various states of charge.

Prevention and mitigation of thermal runaway presents one of the greatest challenges for the safe operation of lithium-ion batteries. Here, we demonstrate for the first time the application of high-speed synchrotron X-ray computed tomography and radiography, in conjunction with thermal imaging, to track the evolution of internal structural damage and thermal behaviour during initiation and propagation of thermal runaway in lithium-ion batteries. This diagnostic approach is applied to commercial lithium-ion batteries (LG 18650 NMC cells), yielding insights into key degradation modes including gas-induced delamination, electrode layer collapse and propagation of structural degradation. It is envisaged that the use of these techniques will lead to major improvements in the design of Li-ion batteries and their safety features. It is important to understand the mechanisms of thermally induced battery degradation and any safety hazards. Here, the authors use high-speed synchrotron radiation X-ray computed tomography to shed light on the structural and thermal dynamics associated with thermal runaway and failure of commercial Li-ion batteries.

Supercapacitors have shown extraordinary promise for miniaturized electronics and electric vehicles, but are usually limited by electrodes with rather low volumetric performance, which is largely due to the inefficient utilization of pores in charge storage. Herein, we design a freestanding graphene laminate film electrode with highly efficient pore utilization for compact capacitive energy storage. The interlayer spacing of this film can be precisely adjusted, which enables a tunable porosity. By systematically tailoring the pore size for the electrolyte ions, pores are utilized optimally and thereby the volumetric capacitance is maximized. Consequently, the fabricated supercapacitor delivers a stack volumetric energy density of 88.1 Wh l −1 in an ionic liquid electrolyte, representing a critical breakthrough for optimizing the porosity towards compact energy storage. Moreover, the optimized film electrode is assembled into an ionogel-based, all-solid-state, flexible smart device with multiple optional outputs and superior stability, demonstrating enormous potential as a portable power supply in practical applications. The volumetric performance of supercapacitors needs to be improved, but the usual trade-off between porosity and density is a problem. Here the authors develop a graphene laminate film with tunable porosity that leads to a volumetric energy density of 88.1 Wh l −1 at the device level.

The permeability of shales is important, because it controls where oil and gas resources can migrate to and where in the Earth hydrocarbons are ultimately stored. Shales have a well-known anisotropic directional permeability that is inherited from the depositional layering of sedimentary laminations, where the highest permeability is measured parallel to laminations and the lowest permeability is perpendicular to laminations. We combine state of the art laboratory permeability experiments with high-resolution X-ray computed tomography and for the first time can quantify the three-dimensional interconnected pathways through a rock that define the anisotropic behaviour of shales. Experiments record a physical anisotropy in permeability of one to two orders of magnitude. Two- and three-dimensional analyses of micro- and nano-scale X-ray computed tomography illuminate the interconnected pathways through the porous/permeable phases in shales. The tortuosity factor quantifies the apparent decrease in diffusive transport resulting from convolutions of the flow paths through porous media and predicts that the directional anisotropy is fundamentally controlled by the bulk rock mineral geometry. Understanding the mineral-scale control on permeability will allow for better estimations of the extent of recoverable reserves in shale gas plays globally.

Heat generation and therefore thermal transport plays a critical role in ensuring performance, ageing and safety for lithium-ion batteries (LIB). Increased battery temperature is the most important ageing accelerator. Understanding and managing temperature and ageing for batteries in operation is thus a multiscale challenge, ranging from the micro/nanoscale within the single material layers to large, integrated LIB packs. This paper includes an extended literature survey of experimental studies on commercial cells investigating the capacity and performance degradation of LIB. It compares the degradation behavior in terms of the influence of operating conditions for different chemistries and cell sizes. A simple thermal model for linking some of these parameters together is presented as well. While the temperature appears to have a large impact on ageing acceleration above room temperature during cycling for all studied cells, the effect of SOC and C rate appear to be rather cell dependent.Through the application of new simulations, it is shown that during cell testing, the actual cell temperature can deviate severely from the reported temperature depending on the thermal management during testing and C rate. It is shown, that the battery lifetime reduction at high C rates can be for large parts due to an increase in temperature especially for high energy cells and poor cooling during cycling studies. Measuring and reporting the actual battery (surface) temperature allow for a proper interpretation of results and transferring results from laboratory experiments to real applications.

Metal anodes hold considerable promise for high-energy-density batteries but are fundamentally limited by electrochemical irreversibility caused by uneven metal deposition and dendrite formation, which compromise battery lifespan and safety. The chaotic ion flow (or ion flux vortex) near the electrode surface, driving these instabilities, has remained elusive due to limitations in conventional techniques such as scanning electron and atomic force microscopies, which are invasive and incapable of probing internal structures of deposits. Here, we employ in-situ X-ray computed tomography (CT) to non-destructively visualize Zn deposition on LAPONITE-coated Zn anodes, thereby revealing the internal structural evolution and deposition orientation. Combined with computational fluid dynamics simulations, we demonstrate that the LAPONITE coating, with its separated positive and negative charge centers, suppresses ionic vortex formation, guiding uniform, dense, and vertically aligned Zn growth along (100) plane, thereby significantly mitigating dendrite growth. This translates into a 3.17-Ah Zn-MnO 2 pouch cell with stable performance over 100 cycles, offering a viable path toward scalable, high-performance metal-anode batteries. Uneven zinc growth limits the reversibility of zinc metal batteries. Here, authors use in situ X-ray computed tomography and fluid dynamics simulations to reveal how synthetic clay coating suppresses chaotic ion flow, enabling uniform zinc growth and stable cycling in a large-scale pouch cell.