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Abstract Data‐intensive discovery of water‐splitting catalysts can accelerate the development of sustainable energy technologies, such as the photocatalytic and/or electrocatalytic production of renewable hydrogen fuel. Through computational screening, 13 materials were recently predicted as potential water‐splitting photocatalysts: Cu₃NbS₄, CuYS₂, SrCu₂O₂, CuGaO₂, Na₃BiO_4,Sr₂PbO₄, LaCuOS, LaCuOSe, Na₂TeO₄, La₄O₄Se₃, Cu₂WS₄, BaCu₂O₂, and CuAlO₂. Herein, these materials are synthesized, their bandgaps and band alignments are experimentally determined, and their photoelectrocatalytic hydrogen evolution properties are assessed. Using cyclic voltammetry and chopped illumination experiments, 9 of the 13 materials are experimentally found to have bandgaps and band alignments that straddle the potentials required for the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER), as computationally predicted. During photocatalytic testing, 12 of the materials yield a measurable photocurrent. However, only three are found to be active for the HER, with Cu₃NbS₄, CuYS₂, and Cu₂WS₄producing H₂in amounts comparable to bare TiO₂; a benchmark photocatalyst. This study provides experimental validation of computational bandgap and band alignment predictions while also successfully identifying active photocatalysts. 

Abstract While lithium ion batteries with electrodes based on intercalation compounds have dominated the portable energy storage market for decades, the energy density of these materials is fundamentally limited. Today, rapidly growing demand for this type of energy storage is driving research into materials that utilize alternative reaction mechanisms to enable higher energy densities. Transition metal compounds are one such class of materials, with storage enabled by “conversion” reactions, where the material is converted to new compound upon lithiation. MoS₂is one example of this type of material that has generated a large amount of interest recently due to its high theoretical lithium storage capacity compared to graphite. Here, cryogenic scanning transmission electron microscopy techniques are used to reveal the atomic‐scale processes that occur during reaction of a model monolayer MoS₂system by enabling the unaltered atomic structure to be determined at various levels of lithiation. It is revealed that monolayer MoS₂can undergo a conversion reaction even with no substrate, and that the resulting particles are smaller than those that form in bulk MoS₂, likely due to the more limited 2D diffusion. Additionally, while bilayer MoS₂undergoes intercalation with a corresponding phase transition before conversion, monolayer MoS₂does not.