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Developing functional textiles with a cooling effect is important for personal comfort in human life and activities. Although existing passive cooling fabrics exhibit promising cooling effects, they do not meet the thermal comfort requirements under many practical conditions. Here, we report a nanofiber membrane-based moisture-wicking passive cooling hierarchical metafabric that couples selective optical cooling and wick-evaporation cooling to achieve efficient temperature and moisture management. The hierarchical metafabric showed high sunlight reflectivity (99.16% in the 0.3-0.76 μm wavelength range and 88.60% in the 0.76-2.5 μm wavelength range), selective infrared emissivity (78.13% in the 8-13 μm wavelength range), and good moisture permeability owing to the optical properties of the material and hierarchical morphology design. Cooling performance experiments revealed that covering simulated skin with the hierarchical metafabric prevented overheating by 16.6 °C compared with traditional textiles, including a contribution from management of the humidity (∼8.2 °C). In addition to the personal thermal management ability, the hierarchical metafabric also showed good wearability.The manipulation of conductive nanowires (NWs) on semiconductor platforms provides important insights into the fabrication of nanoscale electronic devices. In this work, we directly observed the electric field-induced phase transitions in atomic Au-NWs self-assembled on Ge(001) surfaces using scanning tunneling microscopy (STM). The tunneling electrons and electric fields underneath a STM tip apex can effectively trigger a phase transition in Au-NWs on Ge(001) surfaces. Such phase transitions are associated with a remarkable atomic rearrangement in the Au-NWs, thereby modifying their band structures. Moreover, directly monitoring the dynamic reconstruction of Au-NWs on Ge(001) surfaces helps us to understand the NWs' intricate atomic configurations and their electronic properties. The spatially controlled phase transition at the nanometer scale using STM shows the possibility of modulating NWs' properties at an atomic scale.Zeolites with large cavities that are accessible via wide pore windows are desirable but very rare. They have been dominantly used as catalysts in industry. Here we report a novel porous germanosilicate SCM-25, the zeolite structure containing ordered meso-cavities (29.9 × 7.6 × 6.0 Å3) interconnected by 10- and 12-ring channels. SCM-25 was synthesized as nanosized crystals by using a simple organic structure-directing agent (OSDA). Three-dimensional (3D) electron diffraction shows that SCM-25 crystallizes in the orthorhombic space group Cmmm with a = 14.62 Å, b = 51.82 Å, c = 13.11 Å, which is one of the zeolites with the largest unit cell dimensions. We demonstrate that 3D electron diffraction is a powerful technique for determining the complex structure of SCM-25, including the disorders and distributions of framework atoms silicon and germanium. SCM-25 has a high surface area (510 m2/g) and high thermal stability (700 °C). Furthermore, we propose a potential postsynthetic strategy for the preparation of zeolites with ordered meso-cavities by applying the ADOR (assembly-disassembly-organization-reassembly) approach.Predictive models based on mobile measurements have been increasingly used to understand the spatiotemporal variations of intraurban air quality. However, the effects of meteorological factors, which significantly affect the dispersion of air pollution, on the urban-form-air-quality relationship have not been understood on a granular level. We attempt to fill this gap by developing predictive models of particulate matter (PM) in the Bronx (New York City) using meteorological and urban form parameters. The granular PM data was collected by mobile low-cost sensors as the ground truth. To evaluate the effects of meteorological factors, we compared the performance of models using the urban form within fixed and wind-sensitive buffers, respectively. We find better predictive power in the wind-sensitive group (R = 0.85) for NC10 (number concentration for particles with diameters of 1 μm-10 μm) than the control group (R = 0.01), and modest improvements for PM2.5 (R = 0.84 for the wind sensitive group, R = 0.77 for the control group), indicating that incorporating meteorological factors improved the predictive power of our models. We also found that urban form factors account for 62.95% of feature importance for NC10 and 14.90% for PM2.5 (9.99% and 4.91% for 3-D and 2-D urban form factors, respectively) in our Random Forest models. It suggests the importance of incorporating urban form factors, especially for the uncommonly used 3-D characteristics, in estimating intraurban PM. Our method can be applied in other cities to better capture the influence of urban context on PM levels.Particulate oxidative potential may comprise a key health-relevant parameter of particulate matter (PM) toxicity. To identify biological perturbations associated with particulate oxidative potential and examine the underlying molecular mechanisms, we recruited 54 participants from two dormitories near and far from a congested highway in Atlanta, GA. Fine particulate matter oxidative potential ("FPMOP") levels at the dormitories were measured using dithiothreitol assay. Plasma and saliva samples were collected from participants four times for longitudinal high-resolution metabolic profiling. We conducted metabolome-wide association studies to identify metabolic signals with FPMOP. Leukotriene metabolism and galactose metabolism were top pathways associated with ≥5 FPMOP-related indicators in plasma, while vitamin E metabolism and leukotriene metabolism were found associated with most FPMOP indicators in saliva. We observed different patterns of perturbed pathways significantly associated with water-soluble and -insoluble FPMOPs, respectively. We confirmed five metabolites directly associated with FPMOP, including hypoxanthine, histidine, pyruvate, lactate/glyceraldehyde, and azelaic acid, which were implications of perturbations in acute inflammation, nucleic acid damage and repair, and energy perturbation. The unique metabolic signals were specific to FPMOP, but not PM mass, providing initial indication that FPMOP might constitute a more sensitive, health-relevant measure for elucidating etiologies related to PM2.5 exposures.The search for the signature of nonthermal (so-called "hot") electrons in illuminated plasmonic nanostructures requires detailed understanding of the nonequilibrium electron distribution under illumination, as well as a careful design of the experimental system employed to distinguish nonthermal electrons from thermal ones. Here, we provide a theory for using plasmonic molecular junctions to achieve this goal. We show how nonthermal electrons can be measured directly and separately from the unavoidable thermal response and discuss the relevance of our theory to recent experiments.Chiral sulfoximines have recently been considered as promising bioisosteres in medicinal chemistry. However, methods for preparing chiral sulfoximines in a stereoselective manner are underdeveloped. Herein, we demonstrate an asymmetric synthesis of chiral sulfoximines through a stereospecific S-alkylation of readily accessible chiral sulfinamides under practical conditions. A key to establishing the practical conditions was the identification of the intermediate structure in our previously reported S-alkylation by X-ray crystallographic analysis.Controlling the morphology of the metal-organic framework (MOF) for nanosheets is beneficial for understanding their crystal growth kinetics and useful for extending these MOF nanosheets to advanced applications, in particular for gas separation and device integration. However, synthesizing MOF nanosheets with uniform thickness or desirable size still remains challenging. Herein, we provide a crystal dissolution-growth strategy for fabricating dispersible porphyrin MOF nanosheets with lateral dimensions and nanometer thickness. A morphological transition (bulk crystals-nanosheets-bulk crystals) in Zn-TCPP was observed when controlling the crystal growth kinetics by adjusting the reaction parameters (temperature and acidity). These findings encouraged the synthesis of other types of nanosheets (Cu-TCPP, Zn-TCPP (Pd), and Cu-BDC nanosheets). Zn-TCPP (Pd) nanosheets were applied in field-effect transistors and exhibited photoresponse characteristics. This work demonstrates a new strategy for obtaining MOF nanosheets and casts a new light upon fabricating two-dimensional inorganic-organic hybrid materials with controlled thickness.Ferricyanide/ferrocyanide/guanidinium-based thermoelectrochemical cells have been investigated under different loading conditions in this work. Compared with ferricyanide/ferrocyanide-based devices, the device with guanidinium-added electrolytes shows higher power and energy densities. We observed that the enhanced performance is not due to the ionic Seebeck effect of guanidinium but because of the configuration entropy change resulting from the selective binding of Gdm+ to Fe(CN)64-. However, the device with guanidinium-added electrolyte does not show steady-state operation. The two possible reasons include (1) the difficult diffusion of Fe(CN)63- into the crystal layer of (Gdm+)n[Fe(CN)64-] at the hot electrode and (2) the difficult precipitation of (Gdm+)n[Fe(CN)64-] formed at the cold side upon the binding of the reduced Fe(CN)64- with Gdm+. Nevertheless, the performance recovers once the device is disconnected from the external loading. Due to the high thermopower after adding guanidinium, we successfully fabricate self-powered sensors by connecting four flexible cells in series. The sensors can transfer humidity, temperature, and air pressure data wirelessly using body heat. Therefore, ferricyanide/ferrocyanide/guanidinium is a promising electrolyte material for applications of low-grade energy harvesting.Aprotic lithium-oxygen batteries (LOBs) are promising energy storage systems characterized by ultrahigh theoretical energy density. Extensive research has been devoted to this battery technology, yet the detailed operational mechanisms involved, particularly unambiguous identification of various discharge products and their specific distributions, are still unknown or are subjects of controversy. This is partly because of the intrinsic complexity of the battery chemistry but also because of the lack of atomic-level insight into the oxygen electrodes acquired via reliable techniques. In the current study, it is demonstrated that electron beam irradiation could induce crystallization of amorphous discharge products. Cryogenic conditions and a low beam dosage have to be used for reliable transmission electron microscopy (TEM) characterization. High-resolution cryo-TEM and electron energy loss spectroscopy (EELS) analysis of toroidal discharge particles unambiguously identified the discharge products as a dominating amorphous LiO2 phase with only a small amount of nanocrystalline Li2O2 islands dispersed in it. In addition, uniform mixing of carbon-containing byproducts is identified in the discharge particles with cryo-EELS, which leads to a slightly higher charging potential. The discharge products can be reversibly cycled, with no visible residue after full recharge. We believe that the amorphous superoxide dominating discharge particles can lead researchers to reconsider the chemistry of LOBs and pay special attention to exclude beam-induced artifacts in traditional TEM characterizations.

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