Surface Confinement Etching and Polarization Matter: A New Approach To Prepare Ultrathin PtAgCo Nanosheets for Hydrogen-Evolution Reactions

One of the important objectives in fuel-cell technology is to improve the activity and reduce the loading of Pt for hydrogen-evolution electrocatalysis. Here, an oxidative etching strategy of stacking faults is developed to prepare Pt­AgCo nanosheets by element-specific anisotropic growth. Sophisticated use of defects in crystal growth allows tailoring the morphology and interfacial polarization to improve catalytic performance of nanosheets for the hydrogen-evolution reaction. Systematic studies reveal that the presence of the stacking faults may be the knob for the formation of nanosheets. In particular, the chemical composition of nanosheets is potentially the key for altering the hydrogen-evolution reaction. As a result, the Pt­AgCo-II ultrathin nanosheets possess useful HER properties, achieving a current density up to 705 mA cm^–2 at a potential of −400 mV

Microfluidic Chip-Based Modeling of Three-Dimensional Intestine–Vessel–Liver Interactions in Fluorotelomer Alcohol Biotransformation

Plyfluoroalkyl substance (PFAS), featured with incredible persistence and chronic toxicity, poses an emerging ecological and environmental crisis. Although significant progress has been made in PFAS metabolism in vivo, the underlying mechanism of metabolically active organ interactions in PFAS bioaccumulation remains largely unknown. We developed a microfluidic-based assay to recreate the intestine–vessel–liver interface in three dimensions, allowing for high-resolution, real-time images and precise quantification of intestine–vessel–liver interactions in PFAS biotransformation. In contrast to the scattered arrangement of vascular endothelium on the traditional d-polylysine-modified two-dimensional (2D) plate, the microtubules in our three-dimensional (3D) platform formed a dense honeycomb network through the ECM, with longer tubular structures. Additionally, the slope culture of epithelial cells in our platform exhibited a closely arranged and thicker cell layer than the planar culture. To dynamically monitor the metabolic crosstalk in the intestinal–vascular endothelium–liver interaction under exposure to fluorotelomer alcohols (FTOHs), we combined the chip with a solid-phase extraction-mass spectrometry (SPE-MS) system. Our findings revealed that endothelial cells were involved in the metabolic process of FTOHs. The transformation of intestinal epithelial and hepatic epithelial cells produces toxic metabolite fluorotelomer carboxylic acids (FTCAs), which circulate to endothelial cells and affect angiogenesis. This system shows promise as an enhanced surrogate model and platform for studying pollutant exposure as well as for biomedical and pharmaceutical research

Synthesis of High-Quality Brookite TiO₂ Single-Crystalline Nanosheets with Specific Facets Exposed: Tuning Catalysts from Inert to Highly Reactive

The brookite phase of TiO₂ is hardly prepared and rarely studied in comparison with the common anatase and rutile phases. In addition, there exist immense controversies over the cognition of the light-induced liveliness of this material. Here, a novel, low-basicity solution chemistry method was first used to prepare homogeneous high-quality brookite TiO₂ single-crystalline nanosheets surrounded with four {210}, two {101}, and two {201} facets. These nanosheets exhibited outstanding activity toward the catalytic degradation of organic contaminants superior even to that of Degussa P25, due to the exposure of high-energy facets and the effective suppression of recombination rates of photogenerated electrons and holes by these facets as the oxidative and reductive sites. In contrast, irregularly faceted phase-pure brookite nanoflowers and nanospindles were inactive in catalytic reactions. These results demonstrate that the photocatalytic activity of brookite TiO₂ is highly dependent upon its exposed facets, which offers a strategy for tuning the catalysts from inert to highly active through tailoring of the morphology and surface structure

Competitive Coordination Strategy to Finely Tune Pore Environment of Zirconium-Based Metal–Organic Frameworks

Metal–organic frameworks (MOFs) are a class of crystalline porous materials with reticular architectures. Precisely tuning pore environment of MOFs has drawn tremendous attention but remains a great challenge. In this work, we demonstrate a competitive coordination approach to synthesize a series of zirconium–metalloporphyrinic MOFs through introducing H₂O and monocarboxylic acid as modulating reagents, in which well-ordered mesoporous channels could be observed clearly under conventional transmission electron microscopy. Owing to plenty of unsaturated Lewis acid catalytic sites exposed in the visualized mesoporous channels, these structures exhibit outstanding catalytic activity and excellent stability in the chemical fixation of carbon dioxide to cyclic carbonates. The zirconium-based MOFs with ordered channel structures are expected to pave the way to expand the potential applications of MOFs