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Screening promising hydrogen evolution reaction (HER) electrocatalysts for water splitting is crucial for the industrial scalability of sustainable energy storage. As HER catalysts, two‐dimensional (2D) MXenes are promising substitution materials for platinum. Tuning the surface termination and loading a single atom can help to improve the electrocatalytic performance of 2D MXenes. We utilized density functional theory (DFT) calculations to explore the catalyst activity, thermal stability, and dynamic stability of 2D single atom‐loaded MXenes with surface terminations. We demonstrate that 21 uninvestigated 2D single‐atom MXene catalysts, among 264 promising candidates, show an electrocatalytic activity surpassing that of platinum. Among the 21 most promising HER catalysts, 7 (Ti3C2I2Ir, Ti3C2Br2Cu, Ti3C2Br2Pt, Ti3C2Cl2Cu, Ti3C2Cl2Pt, Ti3C2Se2Au, and Ti3C2Te2Nb) are dynamically and thermally stable. Furthermore, machine learning tools predicted the catalyst activity and thermal stability using elemental properties that are easily available in chemical data repositories. [ABSTRACT FROM AUTHOR]

Electrocatalytic valorization of glycerol to formate is considered to be a promising sustainable approach; however, it holds great challenges to increase catalyst activity and deliver market‐demanded chemicals with high Faradaic efficiency (FE) and selectivity under industrial‐level current density. Herein, hierarchically structured phosphorus vacancy‐enriched nickel phosphide porous nanoarrays by copper doping, denoted as CuNiP/CuOx‐VP, are constructed via a facile glycol‐mediated solvothermal approach. The CuNiP/CuOx‐VP yields an industry‐level 1 A cm−2 at the ultralow potential of 1.75 V, while showing notable FE (96.94%) and selectivity (96.76%) to formate over a wide range of potentials. Impressively, a two‐electrode electrolyzer linked to H2 evolution possesses exceptional activity that merely requires a cell voltage of 1.45 V to deliver 40 mA cm−2, exhibiting a high FE (97.53%) for formate production and surpassing the vast majority of previously reported precious metal electrocatalysts. Microscopic and electrochemical characterizations manifest that the CuNiP/CuOx‐VP composed of porous NiP nanosheets attached to aggregated CuOx particles featuring superaerophobic‐hydrophilic morphology enables increased active sites, favorable electronic redistribution, and thus boosted electrocatalytic performance. This study demonstrates an effective nanoarrays electrode for catalyst discovery, going from facile catalyst synthesis to structure‐activity relationship and subsequently developing more highly active electrocatalysts for energy‐saving coproduction of valuable chemicals. [ABSTRACT FROM AUTHOR]