The principal inhibitor of fast charging lithium ion cells is the graphite negative electrode, where favorable conditions for lithium plating occur at high charge rates, causing accelerated degradation and safety...

The hot pressing process for fabricating membrane electrode assemblies (MEAs) has been widely adopted, yet little is known of its effects on the microstructural properties of the different components of the MEA. In particular, the interaction of the electrolyte, electrode and gas diffusion layer (GDL) due to lamination is difficult to probe as conventional imaging techniques cannot access the internal structure of the MEA. Here, a novel approach is used, which combines characterisation of hot-pressed membrane electrode assemblies using X-ray computed tomography, thermogravimetric analysis, differential scanning calorimetry and atomic force microscopy, with electrochemical performance measurements from polarisation curves and high-frequency impedance spectroscopy. Membrane electrode assemblies hot pressed at 100 o C, 130 o C and 170 o C reveal significant differences in microstructure, which has a consequence for the performance. When hot pressed at 100 o C, which is lower than the glass transition temperature of Nafion (123 o C), the catalyst only partially bonds with the Nafion membrane, leading to increased Ohmic resistance. At 170 o C, the Nafion membrane intrudes into the electrode, forming pinholes, degrading the catalyst layer and filling pores in the GDL. Finally, at 130 o C, the interfacial contact is optimum, with similar roughness factor between the catalyst and Nafion membrane surface, indicating effective lamination of layers.

Over the last century, X-ray imaging instruments and their accompanying tomographic reconstruction algorithms have developed considerably. With improved tomogram quality and resolution, voxel sizes down to tens of nanometres can now be achieved. Moreover, recent advancements in readily accessible lab-based X-ray computed tomography (X-ray CT) instruments have produced spatial resolutions comparable to specialist synchrotron facilities. Electrochemical energy conversion devices, such as fuel cells and batteries, have inherently complex electrode microstructures to achieve competitive power delivery for consideration as replacements for conventional sources. With resolution capabilities spanning tens of microns to tens of nanometres, X-ray CT has become widely employed in the three-dimensional (3D) characterisation of electrochemical materials. The ability to perform multiscale imaging has enabled characterisation from system-down to particle-level, with the ability to resolve critical features within device microstructures. X-ray characterisation presents a favourable alternative to other 3D methods such as focused ion beam scanning electron microscopy, due to its non-destructive nature, which allows four-dimensional (4D) studies, three spatial dimensions plus time, linking structural dynamics to device performance and lifetime. X-ray CT has accelerated research from fundamental understanding of the links between cell structure and performance, to the improvement in manufacturing and scale-up of full electrochemical cells. Furthermore, this has aided in the mitigation of degradation and celllevel failures such as thermal runaway. This review presents recent developments in the use of X-ray CT as a characterisation method and its role in the advancement of electrochemical materials engineering.

The increasing use of intermittent renewable energy sources calls for novel approaches to large-scale energy conversion and storage. Hydrogen can be readily stored and produced from renewable sources using polymer electrolyte membrane water electrolysers (PEMWEs). Mass transport of water and product gas in the liquid-gas diffusion layer (LGDL) is critical for PEMWE performance, particularly at high current densities. In this work, neutron radiography is deployed to measure the spatial distribution of water within three different LGDLs, while X-ray micro-computed tomography (XCT) is used to characterize the microstructure of the LGDL materials. The combination of these two techniques yields valuable insight into water transport within the LGDL. Significant local water heterogeneity is observed and a link between flow-field geometry/location and LGDL mass transport is identified. It is further shown that the pore volume in these LGDLs is significantly under-utilized, pointing the way towards design optimisation of LGDL materials and architectures.

Ceramic fuel cells offer a clean and efficient means of producing electricity through a variety of fuels. However, miniaturization of cell dimensions for portable device application remains a challenge, as volumetric power densities generated by readily-available planar/tubular ceramic cells are limited. Here, we demonstrate a concept of ‘micro-monolithic’ ceramic cell design. The mechanical robustness and structural integrity of this design is thoroughly investigated with real-time, synchrotron X-ray diffraction computed tomography, suggesting excellent thermal cycling stability. The successful miniaturization results in an exceptional power density of 1.27 W cm −2 at 800 °C, which is among the highest reported. This holistic design incorporates both mechanical integrity and electrochemical performance, leading to mechanical property enhancement and representing an important step toward commercial development of portable ceramic devices with high volumetric power (>10 W cm −3 ), fast thermal cycling and marked mechanical reliability.

X-ray nano-tomography was used to study the strain evolution of an NMC electrode under uniaxial compression to mimic calendering.

Polymer electrolyte membrane water electrolysers (PEMWE) are a key technology for producing clean ('green') hydrogen for decarbonisation of the transport sector and grid stabilization utilising increasing levels of renewable energy. Understanding the complex interplay of factors that affect device operation is key to improving the technology and advanced diagnostic techniques have a major role to play. In this work, acoustic emission analysis is used as a non-destructive, operando diagnostic tool to provide information about the relative number and size of gas bubbles generated locally within a PEMWE, providing effective characterization of the local flow regime. An optically transparent single-channel PEMWE is used to investigate the relationship between the acoustic signals obtained and the two-phase flow conditions inside the cell. Results show good correlation between the number of acoustic 'hits' and the number of bubbles passing through the flow channel. The size of bubbles is also shown to affect the average frequency of the hits. Consequently, the transition between flow regimes can be identified by acoustic emission analysis, paving the way for a simple, low-cost, nondestructive means of mapping flow inside commercial-scale PEMWEs.

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, 12.6 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.