Greershannon2971

These results demonstrate the effectiveness of our strategy, and this approach can be further extended to other inorganic materials in thin-film form.The effects of oxidation on the gastric digestion properties of soybean protein isolates (SPIs) in a model of lipoxygenase (LOX)-catalyzed linoleic acid (LA) oxidation system and the multiscale structural characterization of SPI hydrolysate were investigated. Results indicated that the feature of SPI hydrolysate is dependent upon the degree of oxidation. Pepsin hydrolysis caused a red shift in fluorescence intensity and a reduction in surface hydrophobicity and diminished the particle size of SPI hydrolysate during gastric digestion. Compared with the control, mild oxidation was beneficial to protein unfolding and gastric digestibility, as manifested by minimal molecular weight (MW) distribution >50 kDa (32.34%) and smaller peptide fragments under scanning electron microscopy. However, severe oxidation brought about 39.47% loss of free amino acids. It was interesting to find that glycinin was more vulnerable to pepsin hydrolysis after oxidation as compared to the native SPI. Overall, the moderately oxidized SPI appeared to be digested to a greater extent.Li-rich cathodes have been in considerable attention for their high reversible capacity. However, they have serious problems like poor cycling with intense capacity decay and voltage fading, which restrict their access to practical applications. In this work, a facile and efficient strategy is proposed to alleviate these intrinsic issues with a high-efficiency electrolyte system. This special electrolyte enables Li-rich cathodes to deliver superior integrated performance with a high initial discharge capacity of 301 mAh·g-1, outstanding cycling stability with a capacity retention of 88% at 0.5 C over 500 cycles, and a remarkable rate capability of 136 mAh·g-1 at 5 C, respectively. What is more, the voltage fading is largely suppressed. Physical and electrochemical characterizations demonstrate that the robust CEI film formed on the cathode surface contributes to the improved electrochemical performance. This work provides a new approach to surmount defects of Li-rich materials and will largely promote their practical applications on Li-ion batteries.Triple-conducting materials have been proved to improve the performance of popular protonic ceramic electrolysis cells. However, partially because of the complexity of the water-splitting reaction involving three charge carriers, that is, oxygen (O2-), proton (H+), and electron (e-), the triple-conducting reaction mechanism was not clear, and the reaction conducting pathways have seldom been addressed. In this study, the triple-conducting Ruddlesden-Popper phase Pr1.75Ba0.25NiO4+δ as an anode on the BaCe0.7Zr0.1Y0.1Yb0.1O3-δ electrolyte was fabricated and its electroresponses were characterized by electrochemical impedance spectroscopy with various atmospheres and temperatures. The impedance spectra are deconvoluted by means of the distribution of the relaxation time method. The surface exchange rate and chemical diffusivity of H+ and O2- are characterized by electrical conductivity relaxation. The physical locations of electrochemical processes are also identified by atomic layer deposition with a surface inhibitor. A microkinetics model is proposed toward conductivities, triple-conducting pathways, reactant dependency, surface exchange and bulk diffusion capabilities, and other relevant properties. Finally, the rate-limiting steps and suggestions for further improvement of electrode performance are presented.Understanding colloid transport in subsurface environments is challenging because of complex interactions among colloids, groundwater, and porous media over several length scales. Here, we report a versatile method to assemble bead-based microfluidic porous media analogues with chemical heterogeneities of different configurations. We further study the transport of colloidal particles through a family of porous media analogues that are randomly packed with oppositely charged beads with different mixing ratios. We recorded the dynamics of colloidal particle deposition at the level of single grains. From these, the maximum surface coverage (θmax = 0.051) was measured directly. The surface-blocking function and the deposition coefficient (kpore = 3.56 s-1) were obtained. Using these pore-scale parameters, the transport of colloidal particles was modeled using a one-dimensional advection-dispersion-deposition equation under the assumption of irreversible adsorption between oppositely charged beads and colloids, showing very good agreement with experimental breakthrough curves and retention profiles at the scale of the entire porous medium analogue. This work presents a new approach to fabricate chemically heterogeneous porous media in a microfluidic device that enables the direct measurement of pore-scale colloidal deposition. Compared with the conventional curve-fitting method for deposition constant, our approach allows quantitative prediction of colloidal breakthrough and retention via coupling of direct pore-scale measurements and an advection-dispersion-deposition model.Nanofluidic devices have become a powerful tool for extremely precise analyses at a single-molecule/nanoparticle level. However, a simple and sensitive molecular detection method is essential for nanofluidic devices because of ultrasmall volume (fL-aL). One such technology is photothermal spectroscopy (PTS), which utilizes light absorption and thermal relaxation by target molecules. Recently, we developed a photothermal optical diffraction (POD) detection method as PTS for nanofluidic devices. However, the detectable concentration range was in the order of μM (102 to 104 molecules), and further improvement in detection performance is strongly required. Here, we demonstrate solvent-enhanced POD with optimized experimental conditions and show its capability of concentration determination of nonfluorescent molecules in nanochannels at a countable molecular level. A relationship between the POD signal and thermal/optical properties of solvents is elucidated. We estimate the diffraction factor and photothermal factor of the solvent enhancement effect by thermal simulations and theoretical calculations. Experimental results show good agreement with the prediction, and the detection performance of the POD is successfully improved. At the optimized condition, we demonstrate the concentration determination with the limit of detection of 75 nM, which corresponds to an average of 10 molecules in a detection volume of 0.23 fL. Our sensitive nonfluorescent molecule detection method will be applied to a wide range of chemical/biological analyses utilizing nanofluidics.Versatile host materials with good chemical stability and carrier-transporting ability are quite responsible for achieving stable solution-processed thermally activated delayed fluorescence (TADF) organic light-emitting diodes (OLEDs). Herein, we reported three bipolar dendritic hosts with or without the electron-withdrawing pyridine moiety via 6-site-linkages, namely, 3,3'-bis(3,3″,6,6″-tetra-tert-butyl-9'H-[9,3'6',9″-tercarbazol]-9'-yl)-1,1'-biphenyl (mCDtCBP), 3,3″,6,6″-tetra-tert-butyl-9'-(6-(3-(3,3″,6,6″-tetra-tert-butyl-9'H-[9,3'6',9″-tercarbazol]-9'-yl)phenyl)pyridine-2-yl)-9'H-9,3'6',9″-tercarbazole (mCDtCBPy), and 6,6'-bis(3,3″,6,6″-tetra-tert-butyl-9'H-[9,3'6',9″-tercarbazol]-9'-yl)-2,2'-bipyridine (mCDtCBDPy), exhibiting outstanding solubility, thermal stability as well as electrochemical stability. According to the calculation of bond dissociation energy (BDE), photodegradation results, and carrier dynamics evaluation, a significant relationship between device stability and the pyridine-based dendritic hosts was uncovered. Using mCDtCDPy with the highest electron mobility as the host, the solution-processed bluish-green TADF-OLED showed the shortest operational lifetime due to the unbalanced charge fluxes despite its highest anionic BDE for good chemical stability. However, the device based on mCDtCBPy exhibited twice longer lifetime than that based on mCDtCBP in spite of their similar balanced charge transportation, highlighting the importance of higher anionic BDE of the C-N bond in the device degradation process. Our findings unveiled a potential approach to achieve a subtle regulation of chemical stability and carrier transportation for realizing stable solution-processed TADF-OLEDs.Diphylleia grayi-inspired hydrochromic nano/microstructured films have received much attention for its promising smart hydrochromic applications owing to their simple and low-cost but energy-effective strategy. A new type of water-switchable glazing film patterned with various nano/micro air-hole inverse opal arrays is introduced by selectively removing nano/microsphere polystyrene arrays embedded in the surface of polydimethylsiloxane (PDMS) films. Using the significant contrast ratio of the bleaching and the scattering states, we have optimized the switching properties of Mie scattered patterns. As a result, we obtained a single inverse opal layer-embedded PDMS adhesive film with hexagonally close-packed 1 μm air-hole arrays as an optimum scattered film. The differences of diffusive transmittance and optical haze values between the dry and the wet states of the best scattered film reached 44.93% (ΔTD.T = 59.11-14.18%) and 54.88% (ΔH = 69.42-14.54%), respectively. In addition, using the best-optimized inverse opal layer-embedded PDMS film, we fabricated a perfectly imitated Diphylleia grayi structure for camouflage application and an intelligent hydrochromic window device. The dynamic water modulation of the scattered opaque and nonscattered transparent state of the inverse opal-patterned PDMS adhesive film can provide an advanced platform structure in the area of hydrochromic technology for smart windows, camouflage, and clear umbrellas for rainy days.Although high-entropy alloys (HEAs) have shown tremendous potential for elevated temperature, anticorrosion, and catalysis applications, little is known on how HEA materials behave under complex service environments. Herein, we studied the high-temperature oxidation behavior of Fe0.28Co0.21Ni0.20Cu0.08Pt0.23HEA nanoparticles (NPs) in an atmospheric pressure dry air environment by in situ gas-cell transmission electron microscopy. It is found that the oxidation of HEA NPs is governed by Kirkendall effects with logarithmic oxidation rates rather than parabolic as predicted by Wagner's theory. Further, the HEA NPs are found to oxidize at a significantly slower rate compared to monometallic NPs. The outward diffusion of transition metals and formation of disordered oxide layer are observed in real time and confirmed through analytical energy dispersive spectroscopy, and electron energy loss spectroscopy characterizations. Localized ordered lattices are identified in the oxide, suggesting the formation of Fe2O3, CoO, NiO, and CuO crystallites in an overall disordered matrix. Hybrid Monte Carlo and molecular dynamics simulations based on first-principles energies and forces support these findings and show that the oxidation drives surface segregation of Fe, Co, Ni, and Cu, while Pt stays in the core region. The present work offers key insights into how HEA NPs behave under high-temperature oxidizing environment and sheds light on future design of highly stable alloys under complex service conditions.