The determination of the electrochemically active surface area and its effects on the electrocatalytic properties of structured nickel electrodes produced by additive manufacturing

Abstract

Additively manufactured (AM) nickel electrodes offer a great potential as an efficient solution for oxygen evolution catalysts in alkaline electrolyzers, since advanced fabrication methods allow the design of high surface area electrodes. The accurate determination of the electrochemical active surface area (ECSA) is a key step in the evaluation of the intrinsic catalytic activity of complex electrodes. In this work, we fabricated Ni electrodes with different macroscopic lattice structures using laser powder bed fusion of metals (PBF-LB/M). The selected designs allow exploring the effects of the electrode geometry on the electrochemical performance. X-ray photon spectroscopy (XPS) and a non-contact optical profilometer (NCOP) were used to investigate the composition and surface morphology of the electrodes. The ECSA was determined by three different approaches. 1. Linear and non-linear allometric fitting of the double layer capacitance from voltammetric experiments. 2. Integration of the Ni2+/Ni3+ transition, also from voltammetry. 3. Assessing double layer capacitance determined from electrochemical impedance spectroscopy (EIS) at open circuit potential (OCP) and the adsorption capacitance for the oxygen evolution reaction (OER) intermediates. Comparing these methods, large deviations in the resulting ECSAs were found, motivating a comprehensive discussion. In addition, four different reactions were investigated, ferri-ferrocyanide redox system, hydrogen evolution, ethanol electrooxidation, and oxygen evolution reaction. The obtained results demonstrate the potential of AM to tailor electrode performance by altering electrode geometry. The findings underline the importance of the ECSA determination for the comparison of the electrocatalytic activity in different electrodes.