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Tubular hollow fibre electrodes for CO2 reduction made from copper aluminum alloy with drastically increased intrinsic porosity
2020, Bell, Daniel, Rall, Deniz, Großeheide, Maren, Marx, Lennart, Hülsdünker, Laura, Wessling, Matthias
Electrochemical reduction of CO2 to higher-order hydrocarbon products offers a significant contribution to the challenge of a circular economy. In the pursuit of better copper metal catalyst, it was early on realized that increasing productivity of copper catalysts systems is reliant on high surface area per volume. Tubular gas diffusion electrodes offer such properties. In this work, we present a methodology to fabricate tubular hollow fibre copper electrodes with drastically increased intrinsic porosity. Our described method utilizes a standard dealloying process of copper aluminium particles to induce an intra-particle nanoporosity. The specific surface area increases from 0.126 m2 g−1 before dealloying to 6.194 m2 g−1 after dealloying. In comparison to conventional planar copper electrodes and literature data from conventional copper hollow fibres, the intra-particle porosity leads to a drastically increase in electrochemical activity. Electrochemical measurements reveal increased current densities at low over-potentials in comparison to conventional copper electrodes under identical experimental conditions emphasizing the significant impact of the porosity on the electrode performance. The presented method can be easily transferred to other alloy particles, highlighting its versatility for electrode fabrication. © 2019 The Author(s)
On charge percolation in slurry electrodes used in vanadium redox flow batteries
2019, Lohaus, Johannes, Rall, Deniz, Kruse, Maximilian, Steinberger, Viktoria, Wessling, Matthias
In vanadium redox flow battery systems porous carbon felts are commonly employed as electrodes inside the flow channel. Recently, slurry electrodes (or flow suspension electrodes) were introduced as a potentially viable electrode system. Such electrode systems are little understood so far. Mass, momentum and charge transfer phenomena co-occur, interactions with each other are nearly impossible to capture experimentally. We present a novel discrete model of the particulate phase combining theories from fluid dynamics, colloidal physics, and electrochemistry with a coupled CFD-DEM approach. The methodology allows to visualize local phenomena occurring during the charging of the battery and to compute the net current of the slurry electrode system. We demonstrate that an increasing particle volume fraction enables the formation of conducting networks in the flow electrode until a threshold is reached. Our study concludes, that the assumption of all particles participating in the charge transfer as assumed in pure CFD investigations is not necessarily valid.