Abstract
Complex solid‐solution electrocatalysts (also referred to as high‐entropy alloy) are gaining increasing interest owing to their promising properties which were only recently discovered. With the capability of forming complex single‐phase solid solutions from five or more constituents, they offer unique capabilities of fine‐tuning adsorption energies. However, the elemental complexity within the crystal structure and its effect on electrocatalytic properties is poorly understood. We discuss how addition or replacement of elements affect the adsorption energy distribution pattern and how this impacts the shape and activity of catalytic response curves. We highlight the implications of these conceptual findings on improved screening of new catalyst configurations and illustrate this strategy based on the discovery and experimental evaluation of several highly active complex solid solution nanoparticle catalysts for the oxygen reduction reaction in alkaline media.
Highlights
Despite remarkable achievements in designing novel electrocatalysts,[1] state-of-the-art catalysts are still often based on noble metals
We highlight the implications of these conceptual findings on improved screening of new catalyst configurations and illustrate this strategy based on the discovery and experimental evaluation of several highly active complex solid solution nanoparticle catalysts for the oxygen reduction reaction in alkaline media
This is especially important for complex multi electron–proton transfer reactions, such as the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER), in which scaling relations play an important role and novel approaches are required for a breakthrough.[2]
Summary
Adjusting of the activity of ORR catalysts was shown experimentally by tailoring the CSS composition,[8] a strategy which could be rationalized by a theoretical study of the adsorption energy distribution pattern (AEDP)[4] and its implication on the specific electrochemical behavior.[3] it was not yet shown which effect different AEDPs have on activity curves and which effects are expected for addition or replacement of elements within the CSS phase We elucidate these fundamental concepts and discuss which information about the AEDP can be gained by analyzing the experimental activity curves. We reveal intrinsically active CSS catalysts, which can be further optimized for their implementation in catalyst films
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