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Molecular Analysis of the Unusual Stability of an IrNbOx Catalyst for the Electrochemical Water Oxidation to Molecular Oxygen (OER)

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Falling,  Lorenz
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Kühl,  Stefanie
Interface Science, Fritz Haber Institute, Max Planck Society;

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Jones,  Travis
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Citation

Spöri, C., Falling, L., Kroschel, M., Brand, C., Bonakdarpour, A., Kühl, S., et al. (2021). Molecular Analysis of the Unusual Stability of an IrNbOx Catalyst for the Electrochemical Water Oxidation to Molecular Oxygen (OER). ACS Applied Materials and Interfaces, 13(3), 3748-3761. doi:10.1021/acsami.0c12609.


Cite as: http://hdl.handle.net/21.11116/0000-0007-F824-9
Abstract
Adoption of proton exchange membrane (PEM) water electrolysis technology on a global level will demand a significant reduction of today’s iridium loadings in the anode catalyst layers of PEM electrolyzers. However, new catalyst and electrode designs with reduced Ir content have been suffering from limited stability caused by (electro)chemical degradation. This has remained a serious impediment to a wider commercialization of larger-scale PEM electrolysis technology. In this combined DFT computational and experimental study, we investigate a novel family of iridium–niobium mixed metal oxide thin-film catalysts for the oxygen evolution reaction (OER), some of which exhibit greatly enhanced stability, such as minimized voltage degradation and reduced Ir dissolution with respect to the industry benchmark IrOx catalyst. More specifically, we report an unusually durable IrNbOx electrocatalyst with improved catalytic performance compared to an IrOx benchmark catalyst prepared in-house and a commercial benchmark catalyst (Umicore Elyst Ir75 0480) at significantly reduced Ir catalyst cost. Catalyst stability was assessed by conventional and newly developed accelerated degradation tests, and the mechanistic origins were analyzed and are discussed. To achieve this, the IrNbOx mixed metal oxide catalyst and its water splitting kinetics were investigated by a host of techniques such as synchrotron-based NEXAFS analysis and XPS, electrochemistry, and ab initio DFT calculations as well as STEM-EDX cross-sectional analysis. These analyses highlight a number of important structural differences to other recently reported bimetallic OER catalysts in the literature. On the methodological side, we introduce, validate, and utilize a new, nondestructive XRF-based catalyst stability monitoring technique that will benefit future catalyst development. Furthermore, the present study identifies new specific catalysts and experimental strategies for stepwise reducing the Ir demand of PEM water electrolyzers on their long way toward adoption at a larger scale.