The compression of carbon felt electrodes for redox flow batteries leads to changes in the electrochemical performance and has a large effect on the pressure drop of electrolyte flow through the system. In this investigation, the authors have characterised the electrochemical performance of all-vanadium redox flow batteries by studying the effect of compression on the contact resistance, polarisation behaviour and efficiency. Contact resistance was seen to reduce from ca. 2.0 Ω cm 2 to 1.2 Ω cm 2 and an energy efficiency of 85% was obtained from a felt compressed to 75%. Moreover, X-ray computed tomography (CT) has been employed to study the microstructure of felt electrodes at compressions up to 70%, showing a linear decrease in porosity and a constant fibre surface areato-volume ratio. The pressure drop was modelled using computational fluid dynamics and employing the 3D structure of the felts obtained from CT, revealing that a 60% increase in compression related to a 44.5% increase in pressure drop.

SummaryLithium‐ion battery performance is intrinsically linked to electrode microstructure. Quantitative measurement of key structural parameters of lithium‐ion battery electrode microstructures will enable optimization as well as motivate systematic numerical studies for the improvement of battery performance. With the rapid development of 3‐D imaging techniques, quantitative assessment of 3‐D microstructures from 2‐D image sections by stereological methods appears outmoded; however, in spite of the proliferation of tomographic imaging techniques, it remains significantly easier to obtain two‐dimensional (2‐D) data sets. In this study, stereological prediction and three‐dimensional (3‐D) analysis techniques for quantitative assessment of key geometric parameters for characterizing battery electrode microstructures are examined and compared. Lithium‐ion battery electrodes were imaged using synchrotron‐based X‐ray tomographic microscopy. For each electrode sample investigated, stereological analysis was performed on reconstructed 2‐D image sections generated from tomographic imaging, whereas direct 3‐D analysis was performed on reconstructed image volumes. The analysis showed that geometric parameter estimation using 2‐D image sections is bound to be associated with ambiguity and that volume‐based 3‐D characterization of nonconvex, irregular and interconnected particles can be used to more accurately quantify spatially‐dependent parameters, such as tortuosity and pore‐phase connectivity.

a b s t r a c tRedox flow batteries offer a potential solution to an increase in renewable energy generation on the grid by offering long-term, large-scale storage and regulation of power. However, they are currently underutilised due to cost and performance issues, many of which are linked to the microstructure of the porous carbon electrodes used. Here, for the first time, we offer a detailed study of the in situ effects of compression on a commercially available carbon felt electrode. Visualisation of electrode structure using X-ray computed tomography shows the non-linear way that these materials compress and various metrics are used to elucidate the changes in porosity, pore size distribution and tortuosity factor under compressions from 0%-90%.

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