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Discovery of Manganese-Based Solar Fuel Photoanodes via Integration of Electronic Structure Calculations, Pourbaix Stability Modeling, and High-Throughput Experiments

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The solar photoelectrochemical generation of hydrogen and carbon-containing fuels comprises a critical energy technology for establishing sustainable energy resources. The photoanode, which is responsible for solar-driven oxygen evolution, has persistently limited technology advancement due to the lack of materials that exhibit both the requisite electronic properties and operational stability. Efforts to extend the lifetime of solar fuel devices increasingly focus on mitigating corrosion in the highly oxidizing oxygen evolution environment, motivating our development of a photoanode discovery pipeline that combines electronic structure calculations, Pourbaix stability screening, and high-throughput experiments. By applying the pipeline to ternary metal oxides containing manganese, we identify a promising class of corrosion-resistant materials and discover five oxygen evolution photoanodes, including the first demonstration of photoelectrocatalysis with Mn-based ternary oxides and the introduction of alkaline earth manganates as promising photoanodes for establishing a durable solar fuels technology.

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