Publication date: 10th April 2024
Ordered mesoporous oxides are characterized by a regular pore structure surrounded by single interconnected nanocrystallites. This unique architecture makes this class of material of high interest for a variety of electrochemical applications, e.g., for gas sensing, energy storage or catalysis. The open pore-solid framework provides good accessibility of the internal surfaces to the surrounding medium, as gases or liquids can completely penetrate into the mesopores, resulting in superior device performance compared to nanoparticles or disordered mesoporous counterparts. In addition, the electrochemical properties of ordered mesoporous oxides can be tailored, at least to some extent, by adjusting the pore size or by surface functionalization. However, a detailed knowledge about the impact of the mesoporous architecture on the electrical properties is necessary for further device optimization making a reliable electrochemical characterization of the materials indispensable. Electrochemical impedance spectroscopy is the method of choice to determine the electrical properties. However, the interconnected pore network hinders a simple estimation of the material-specific conductivity from the measured impedance.
Here, we use a 3D impedance network [1] to elucidate the impact of porosity on the impedance response of mesoporous thin films. The results demonstrate that the regular pore structure gives rise to a geometric current constriction effect, which dominates the impedance spectra in the whole frequency range. As a consequence, the effective conductivity values estimated from the total resistance and the electrode geometry underestimate the material-specific conductivity of the material by more than one order of magnitude. However, by a detailed analysis of computed impedance spectra for varying pore size, we were able to derive an empirical expression, which allows the estimation of the material-specific conductivity from the measured impedance with an error of less than 8% [2].
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