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Despite tremendous advances in AI, it remains a significant challenge to develop interactive task guidance systems that can offer situated, personalized guidance and assist humans in various tasks. These systems need to have a sophisticated understanding of the user as well as the environment, and make timely accurate decisions on when and what to say. To address this issue, we created a new multimodal benchmark dataset, Watch, Talk and Guide (WTaG) based on natural interaction between a human user and a human instructor. We further proposed two tasks: User and Environment Understanding, and Instructor Decision Making. We leveraged several foundation models to study to what extent these models can be quickly adapted to perceptually enabled task guidance. Our quantitative, qualitative, and human evaluation results show that these models can demonstrate fair performances in some cases with no task-specific training, but a fast and reliable adaptation remains a significant challenge. Our benchmark and baselines will provide a stepping stone for future work on situated task guidance. 

Abstract Aqueous photoelectrochemical (PEC) cells have long been considered a promising technology to convert solar energy into hydrogen. However, the solar‐to‐H 2 (STH) efficiency and cost‐effectiveness of PEC water splitting are significantly limited by sluggish oxygen evolution reaction (OER) kinetics and the low economic value of the produced O 2 , hindering the practical commercialization of PEC cells. Recently, organic upgrading PEC reactions, especially for alternative OERs, have received tremendous attention, which improves not only the STH efficiency but also the economic effectiveness of the overall reaction. In this review, PEC reaction fundamentals and reactant‐product cost analysis of organic upgrading reactions are briefly reviewed, recent advances made in organic upgrading reactions, which are categorized by their reactant substrates, such as methanol, ethanol, glycol, glycerol, and complex hydrocarbons, are then summarized and discussed. Finally, the current status, further outlooks, and challenges toward industrial applications are discussed. 

Developing stable and efficient electrocatalysts is vital for boosting oxygen evolution reaction (OER) rates in sustainable hydrogen production. High-entropy oxides (HEOs) consist of five or more metal cations, providing opportunities to tune their catalytic properties toward high OER efficiency. This work combines theoretical and experimental studies to scrutinize the OER activity and stability for spinel-type HEOs. Density functional theory confirms that randomly mixed metal sites show thermodynamic stability, with intermediate adsorption energies displaying wider distributions due to mixing-induced equatorial strain in active metal-oxygen bonds. The rapid sol-flame method is employed to synthesize HEO, comprising five 3d-transition metal cations, which exhibits superior OER activity and durability under alkaline conditions, outperforming lower-entropy oxides, even with partial surface oxidations. The study highlights that the enhanced activity of HEO is primarily attributed to the mixing of multiple elements, leading to strain effects near the active site, as well as surface composition and coverage.

 

Electrochemical two-electron water oxidation reaction (2e-WOR) has drawn significant attention as a promising process to achieve the continuous on-site production of hydrogen peroxide (H₂O₂). However, compared to the cathodic H₂O₂generation, the anodic 2e-WOR is more challenging to establish catalysts due to the severe oxidizing environment. In this study, we combine density functional theory (DFT) calculations with experiments to discover a stable and efficient perovskite catalyst for the anodic 2e-WOR. Our theoretical screening efforts identify LaAlO₃perovskite as a stable, active, and selective candidate for catalyzing 2e-WOR. Our experimental results verify that LaAlO₃achieves an overpotential of 510 mV at 10 mA cm⁻²in 4 M K₂CO₃/KHCO₃, lower than those of many reported metal oxide catalysts. In addition, LaAlO₃maintains a stable H₂O₂Faradaic efficiency with only a 3% decrease after 3 h at 2.7 V vs. RHE. This computation-experiment synergistic approach introduces another effective direction to discover promising catalysts for the harsh anodic 2e-WOR towards H₂O₂.

 

Electrochemical oxidation of water and electrolyte ions is a sustainable method for producing energy carriers and valuable chemicals. Among known materials for catalyzing oxidation reactions, titanium dioxide (TiO 2 ) offers excellent electrochemical stability but is less active than many other metal oxides. Herein, we used density functional theory calculations to predict an increase in catalytic activity by doping anatase TiO 2 with manganese atoms (Mn). We synthesized Mn-doped TiO 2 and then utilized X-ray absorption spectroscopy to study the chemical environment around the Mn site in the TiO 2 crystal structure. Our electrochemical experiments confirmed that TiO 2 , with the optimal amount of Mn, reduces the onset potential by 260 mV in a 2 M KHCO 3 (pH = ∼8) electrolyte and 370 mV in a 0.5 M H 2 SO 4 (pH = ∼0.5) electrolyte. Moreover, in 0.5 M H 2 SO 4 , we observed that the amount of Mn doping greatly impacts the selectivity towards oxygen production versus peroxysulfate formation. In 2 M KHCO 3 , the Mn doping of TiO 2 slightly decreases the selectivity towards oxygen production and increases the hydrogen peroxide formation. The Mn-doped TiO 2 shows good electrochemical stability for over 24 hours in both electrolytes.