Modulation of acid-induced pea protein gels by gellan gum and glucono-δ-lactone: Rheological and microstructural insights.

This study investigated the effect of gellan gum (GG) and glucono-δ-lactone (GDL) on the acid-induced gel properties of pea protein isolate (PPI) pretreated with media milling. The inclusion of GG substantially enhanced the gel hardness of PPI gel from 18.69 g to 792.47 g though slightly reduced its water holding capacity (WHC). Rheological analysis showed that GG increased storage modulus (G') and decreased damping factor of gels in the small amplitude oscillatory shear region and transformed its strain thinning behavior into weak strain overshoot behavior in the large amplitude oscillatory shear region. SEM revealed that GG transformed the microstructure of gel from a uniform particle aggregate structure to a chain-like architecture composed of filaments with small protein particles attached. Turbidity and zeta potential analysis showed that GG promoted the transformation of PPI from a soluble polymer system to an insoluble coagulant during acidification. When GG content was relatively high (0.2 %-0.3 %), high GDL content increased the electrostatic interaction between PPI and GG molecules, causing their rapid aggregation into a dense irregular aggregate structure, further enhancing gel strength and WHC. Overall, GG and GDL can offer the opportunity to modulate the microstructure and gel properties of acid-induced PPI gels, presenting potential for diversifying food gel design strategies through PPI-GG hybrid systems.

Chiral phosphoric acid-catalyzed asymmetric epoxidation of alkenyl aza-heteroarenes using hydrogen peroxide.

The synthesis of chiral α-azaheteroaryl oxiranes via enantioselective catalysis is a formidable challenge due to the required complex stereoselectivity and diverse N-heterocyclic structures. These compounds play a crucial role in developing bioactive molecules, where precise chirality significantly influences biological activity. Here we show that using chiral phosphoric acid as a catalyst, our method efficiently addresses these challenges. This technique not only achieves high enantio- and diastereoselectivity but also demonstrates superior chemo- and stereocontrol during the epoxidation of alkenyl aza-heteroarenes. Our approach leverages a synergistic blend of electrostatic and hydrogen-bonding interactions, enabling the effective activation of both substrates and hydrogen peroxide. The resulting chiral oxiranes exhibit enhanced diversity and functionality, aiding the construction of complex chiral azaaryl compounds with contiguous stereocenters. Kinetic and density functional theory studies elucidate the mechanism, highlighting chiral phosphoric acid's pivotal role in this intricate enantioselective process.

Precursor Induced Assembly of Si Nanoparticles Encapsulated in Graphene/Carbon Matrices and the Influence of Al2 O3 Coating on their Properties as Anode for Lithium-Ion Batteries.

The theoretical capacity of pristine silicon as anodes for lithium-ion batteries (LIBs) can reach up to 4200 mAh g-1 , however, the low electrical conductivity and the huge volume expansion limit their practical application. To address this challenge, a precursor strategy has been explored to induce the curling of graphene oxide (GO) flakes and the enclosing of Si nanoparticles by selecting protonated chitosan as both assembly inducer and carbon precursor. The Si nanoparticles are dispersed first in a slurry of GO by ball milling, then the resulting dispersion is dried by a spray drying process to achieve instantaneous solution evaporation and compact encapsulation of silicon particles with GO. An Al2 O3 layer is constructed on the surface of Si@rGO@C-SD composites by the atomic layer deposition method to modify the solid electrolyte interface. This strategy enhances obviously the electrochemical performance of the Si as anode for LIBs, including excellent long-cycle stability of 930 mAh g-1 after 1000 cycles at 1000 mA g-1 , satisfied initial Coulomb efficiency of 76.7%, and high rate ability of 806 mAh g-1 at 5000 mA g-1 . This work shows a potential solution to the shortcomings of Si-based anodes and provides meaningful insights for constructing high-energy anodes for LIBs.

Carbon Nanofibers Decorated by MoS2 Nanosheets with Tunable Quantity as Self-Supporting Anode for High-Performance Lithium Ion Batteries.

Two-dimensional molybdenum disulfide (MoS2) is considered as a highly promising anode material for lithium-ion batteries (LIBs) due to its unique layer structure, large plane spacing, and high theoretical specific capacity; however, the overlap of MoS2 nanosheets and inherently low electrical conductivity lead to rapid capacity decay, resulting in poor cycling stability and low multiplicative performance. This severely limits its practical application in LIBs. To overcome the above problems, composite fibers with a core//sheath structure have been designed and fabricated. The sheath moiety of MoS2 nanosheets is uniformly anchored by the hydrothermal treatment of the axial of carbon nanofibers derived from an electrospinning method (CNFs//MoS2). The quantity of the MoS2 nanosheets on the CNFs substrates can be tuned by controlling the amount of utilized thiourea precursor. The influence of the MoS2 nanosheets on the electrochemical properties of the composite fibers has been investigated. The synergistic effect between MoS2 and carbon nanofibers can enhance their electrical conductivity and ionic reversibility as an anode for LIBs. The composite fibers deliver a high reversible capacity of 866.5 mA h g-1 after 200 cycles at a current density of 0.5 A g-1 and maintain a capacity of 703.3 mA h g-1 after a long cycle of 500 charge-discharge processes at 1 A g-1.

Skin-like cryogel electronics from suppressed-freezing tuned polymer amorphization.

The sole situation of semi-crystalline structure induced single performance remarkably limits the green cryogels in the application of soft devices due to uncontrolled freezing field. Here, a facile strategy for achieving multifunctionality of cryogels is proposed using total amorphization of polymer. Through precisely lowering the freezing point of precursor solutions with an antifreezing salt, the suppressed growth of ice is achieved, creating an unusually weak and homogenous aggregation of polymer chains upon freezing, thereby realizing the tunable amorphization of polymer and the coexistence of free and hydrogen bonding hydroxyl groups. Such multi-scale microstructures trigger the integrated properties of tissue-like ultrasoftness (Young's modulus <10 kPa) yet stretchability, high transparency (~92%), self-adhesion, and instantaneous self-healing (<0.3 s) for cryogels, along with superior ionic-conductivity, antifreezing (-58 °C) and water-retention abilities, pushing the development of skin-like cryogel electronics. These concepts open an attractive branch for cryogels that adopt regulated crystallization behavior for on-demand functionalities.

Electrochemical Activation of Nitromethane to Construct Isoxazoline Aldoximes.

Activation of nitromethane to endow new reactivity is an interesting and meaningful but also challenging topic. Herein, we report an electrochemical activation of nitromethane to serve as both the heterocyclic skeleton and oxime sources for the construction of isoxazoline aldoximes. The isoxazoline aldoximes that are prepared by four steps with the reported strategy are synthesized in a single step from low-cost and readily available nitromethane and olefins with moderate to excellent yields under our electrochemical conditions. The reaction also takes advantage of high atom-economy and E-selectivity. Moreover, the mechanism is studied by control experiments, a kinetic isotope effect (KIE) study, cyclic voltammogram (CV) experiments, and density functional theory (DFT) calculations. The mechanistic results reveal that nitromethane may be activated under electrochemical conditions to deliver a 1,2,5-oxadiazole 2-oxide intermediate, which undergoes [3+2] cycloaddition with olefins to yield isoxazoline aldoximes.

Pd-Enriched-Core/Pt-Enriched-Shell High-Entropy Alloy with Face-Centred Cubic Structure for C1 and C2 Alcohol Oxidation.

High-entropy alloy nanoparticles (HEA NPs) have aroused great interest globally with their unique electrochemical, catalytic, and mechanical properties, as well as diverse activity and multielement tunability for multi-step reactions. Herein, a facile low-temperature synthesis method at atmospheric pressure is employed to synthesize Pd-enriched-HEA-core and Pt-enriched-HEA-shell NPs with a single phase of face-centred cubic structure. Interestingly, the lattice of both Pd-enriched-HEA-core and Pt-enriched-HEA-shell enlarge during the formation process of HEA, with tensile strains included in the core and shell of HEA. The as-obtained PdAgSn/PtBi HEA NPs show excellent electrocatalytic activity and durability for methanol oxidation reaction (MOR) and ethanol oxidation reaction (EOR). The specific (mass) activity of PdAgSn/PtBi HEA NPs for MOR is 4.7 mA cm-2 (2874 mA mg(Pd+Pt) -1 ), about 1.7 (5.9) and 1.5 (4.8) times higher than that of commercial Pd/C and Pt/C catalysts, respectively. Additional to high-entropy effect, Pt sites and Pd sites on the interface of the HEA act synergistically to facilitate the multi-step process towards EOR. This study offers a promising way to find a feasible route for scalable HEA manufacturing with promising applications.

Proton-mediated reversible switching of metastable ferroelectric phases with low operation voltages.

The exploration of ferroelectric phase transitions enables an in-depth understanding of ferroelectric switching and promising applications in information storage. However, controllably tuning the dynamics of ferroelectric phase transitions remains challenging owing to inaccessible hidden phases. Here, using protonic gating technology, we create a series of metastable ferroelectric phases and demonstrate their reversible transitions in layered ferroelectric α-In2Se3 transistors. By varying the gate bias, protons can be incrementally injected or extracted, achieving controllable tuning of the ferroelectric α-In2Se3 protonic dynamics across the channel and obtaining numerous intermediate phases. We unexpectedly discover that the gate tuning of α-In2Se3 protonation is volatile and the created phases remain polar. Their origin, revealed by first-principles calculations, is related to the formation of metastable hydrogen-stabilized α-In2Se3 phases. Furthermore, our approach enables ultralow gate voltage switching of different phases (below 0.4 volts). This work provides a possible avenue for accessing hidden phases in ferroelectric switching.

Microspheres of Si@Carbon-CNTs composites with a stable 3D interpenetrating structure applied in high-performance lithium-ion battery.

The huge volumetric expansion (>300 %) of Si that occurs during the charge-discharge process makes it to have poor cycling ability and weak stable structure. These factors are considered as critical obstacles to the further development of Si as anode for lithium-ion batteries (LIBs). Herein, novel 3D interpenetrating microspheres, i.e., Si@C-CNTs, which consist of silicon nanoparticles interpenetrated with carbon nanotubes (CNTs) and stuck with amorphous carbon (C) have been designed and prepared via a spray-drying assisted approach. As anode of LIBs, Si@C-CNTs microspheres can achieve high silicon loadings of around 86 % and a high initial coulomb efficiency of 80.8 %. The electrodes maintain a reversible specific capacity of 1585.9mAh/g at 500 mA g-1 after 200 cycles, and deliver an excellent rate capability of 756.4 mAh/g at 5 A g-1. The outstanding performance of Si@C-CNTs can be due to their 3D interpenetrating structure and the synergy effect between the CNTs network and amorphous carbon therein. They synergistically act as conductive matrices which significantly improve the conductivity of the composite; they also act binders and reinforcing skeleton which help the composite spheres to have stable structure. Especially, the latter (reinforcing skeleton) alleviates the volumetric effect induced by the expansion and shrinkage of silicon particles during lithiation. The unique architecture provides an ideal model that can be used to design Si-based composite anode for advanced LIBs.

Effects of WeChat platform-based nursing intervention on disease severity and maternal and infant outcomes of patients with gestational diabetes mellitus.

OBJECTIVE: To determine the effects of WeChat platform-based nursing intervention on the disease control and pregnancy outcomes of patients with gestational diabetes mellitus (GDM). METHODS: A total of 112 patients with GDM treated in our hospital from December 2018 to December 2020 were enrolled, and their clinical data were retrospectively analysed. Among them, 61 pregnant women were given routine nursing as the control group (Con group), and the other 51 were given WeChat platform-based interactive continuous nursing intervention as the observation group (Obs group). The blood glucose (BG) of the two groups before and after nursing was compared, and their self-management level and nursing satisfaction were evaluated. The maternal and infant outcomes of the two groups were also compared. RESULTS: Before nursing, BG and glycosylated hemoglobin (HbA1c) levels in the two groups were comparatively high, without notable difference between the two groups (P>0.05); after nursing, the levels of fasting blood glucose, 2 hour postprandial blood glucose (2h-PG), and HbA1c in the Obs group decreased significantly, and were significantly lower than those in the Con group (P<0.05). Additionally, the two groups were similar in self-management level scores before nursing (P>0.05), while after nursing, the scores of diet management, exercise management, BG monitoring management and foot care management in the Obs group increased and were significantly higher than those in the Con group (P<0.05). The Obs group expressed significantly higher nursing satisfaction than the Con group (χ2=6.078, P<0.05). The total incidence of adverse pregnancy outcome in Obs group was lower than that in Con group (χ2-5.566, P<0.05). According to the analysis of risk factors, older age, pre-pregnancy BMI ≥24 kg/m2, and history of diabetes mellitus were independent risk factors for adverse pregnancy outcomes of pregnant women, while WeChat platform-based interactive continuous nursing was a protective factor against adverse pregnancy outcome (P<0.05). CONCLUSION: WeChat platform-based interactive continuous nursing intervention can help patients master comprehensive self-management skills to achieve good control of GDM, improve their satisfaction toward nursing and lower the risk of adverse outcome.

Unveiling the Synergistic Effects of Monodisperse Sea Urchin-like PdPb Alloy Nanodendrites as Stable Electrocatalysts for Ethylene Glycol and Glycerol Oxidation Reactions.

In recent times, the fabrication of noble metal-based catalysts with controllable morphologies has become a research hotspot. Electrocatalytic devices with excellent catalytic performance and enhanced durability for the ethylene glycol oxidation reaction (EGOR) and the glycerol oxidation reaction (GOR) are significant for commercial direct fuel cells. Herein, a series of PdPb sea urchin-like nanodendrite (ND) structures with controllable molar ratios were synthesized as EGOR and GOR electrocatalysts of high efficiency. The optimized structurally regular Pd3Pb NDs exhibit the best electrocatalytic activity and outstanding stability compared to other samples and commercial Pt/C. In addition, the integrated Pb on Pd3Pb NDs can mitigate the bond energy the intermediates generate and further boost the electrooxidation of the intermediates by supplying enough active sites without considering its intrinsic structure, which is beneficial to the enhanced EGOR and GOR activity and stability. With the assistance of electrochemical measurement, the mechanism of the enhanced alloy was further investigated. This paper presents a promising strategy to fabricate catalysts with stable structures, which will elucidate a very promising approach for developing Pd-based catalysts for further applications in fuel cells.

Starfruit-like vanadium oxide with Co2+ pre-intercalation and amorphous carbon confinement as a superior cathode for supercapacitors.

The vanadium dioxide (VO2(D)), with ultra-high theoretical capacitance, has been considered as a boon for electrode materials of advanced supercapacitors (SCs). However, the VO2 has a series of shortcomings such as poor electrical conductivity, severe structural damage, and rapid capacity fading during cycles, resulting in unsatisfactory electrochemical performance. Herein, the Co2+ pre-intercalation and amorphous carbon confined vanadium dioxide (CoxVO2@C) with starfruit-like nanostructure is synthesized on a conductive Ni foam substrate via a versatile and cost-effective method. As a cathode for SCs, the obtained CoxVO2@C not only enables a small amount of Co2+ pre-intercalation layer to offer faster ion diffusion kinetics for VO2, but also utilizes a high-conductivity amorphous carbon to protect VO2 from dissolution in an alkaline electrolyte, thereby exhibiting the ultrahigh specific capacitance up to 4440.0 mF cm-2 at 5 mA cm-2 (525.2 F g-1 at 2 A g-1) and the prominent long-term stability performance of the electrode. Benefited from these excellent characteristics, a high-performance CoxVO2@C//V2O3 hybrid supercapacitor (HSC) device with an operating voltage of 1.7 V is further assembled. The HSC device delivers a superior energy density of 102.3 W h kg-1 at a power density of 6.1 kW kg-1, manifesting its practical feasibility.

Assembly of Alloyed PdCu Nanosheets and Their Electrocatalytic Oxidation of Ethanol.

Two-dimensional (2D) nanostructured catalysts have attracted great attention in many important fields, including energy applications and chemical industry. In this study, PdCu nanosheet assemblies (NSAs) have been synthesized and investigated as electrocatalysts for direct ethanol fuel cells in an alkaline medium. A great number of active sites on the nanosheets of PdCu NSAs for ethanol electro-oxidation are exposed, where the electron structures are optimized combined with the second element copper. Electrochemical measurements show that PdCu NSA1 exhibits excellent catalytic activity (2536 mA mg-1) and cyclic stability compared to PdCu NSA2 (1700 mA mg-1) and PdCu NSA3 (1436 mA mg-1), much higher than commercial Pd/C. Kinetics studies on the electrolysis of ethanol suggest that PdCu NSAs should be more favorable at higher catalytic temperatures, higher concentrations of ethanol, and low pH value environments. The unique composition and structures PdCu NSA1 would result in the lowest energy barrier in the rate-controlling step of the ethanol oxidation reaction (EOR), confirmed by density functional theory (DFT). The formation mechanism of PdCu NSAs and their excellent electrocatalytic activity toward EOR have been discussed and analyzed.

The Influence of Ionic Liquids Adsorption on the Electronic and Optical Properties of Phosphorene and Arsenene with Different Phases: A Computational Study.

Density functional theory (DFT) calculations have been performed to investigate the interfacial interactions of ionic liquids (ILs) on the α- and ß-phases of phosphorene (P) and arsenene (As). Nine representative ILs based on the combinations of 1-ethyl-3-methylimidazolium ([EMIM]+), N-methylpyridinium ([MPI]+), and trimethylamine ([TMA]+) cations paired to tetrafluoroborate ([BF4]-), trifluoromethanesulfonate ([TFO]-), and chloridion (Cl-) anions were used as adsorbates on the 2D P and As nanosheets with different phases to explore the effect of IL adsorption on the electronic and optical properties of 2D materials. The calculated structure, adsorption energy, and charge transfer suggest that the interaction between ILs and P and As nanosheets is dominated by noncovalent forces, and the most stable adsorption structures are characterized by the simultaneous interaction of the cation and anion with the surface, irrespective of the types of ILs and surfaces. Furthermore, the IL adsorption leads to the larger change in the electronic properties of ß-phase P and As than those of their α-phase counterparts, which demonstrates that the adsorption properties are not only related to the chemical elements, but also closely related to the phase structures. The present results provide insight into the further applications of ILs and phosphorene (arsenene) hybrid materials.

Alloyed Palladium-Lead Nanosheet Assemblies for Electrocatalytic Ethanol Oxidation.

Synthesizing alloyed bimetallic electrocatalysts with a three-dimensional (3D) structure assembly have arouse great interests in electrocatalysis. We synthesized a class of alloyed Pd3Pb/Pd nanosheet assemblies (NSAs) composed of a two-dimensional (2D) sheet structure with adjustable compositions via an oil bath approach at a low temperature. Both the scanning electron microscopy (SEM) and transmission electron microscopy (TEM) images reveal the successful formation of the nanosheet structure, where the morphology of Pd3Pb/Pd NSAs can be regulated by adjusting the atomic mole ratio of Pb and Pb metal precursors. The power X-ray diffraction (XRD) pattern shows that Pd3Pb/Pd NSA catalysts are homogeneously alloyed. Electrochemical analysis and the density functional theory (DFT) method demonstrate that the electrocatalytic activity of the alloyed Pd3Pb/Pd NSAs can be improved by the doping of the Pb element. As a result of the addition of element Pb and change of the electron structure, the electrocatalytic activity toward ethanol oxidation of alloyed Pd3Pb/Pd-15 NSA can reach up to 2886 mA mg-1, which is approximately 2.8 times that of the pure Pd NSA counterpart (1020 mA mg-1). The Pd3Pb/Pd NSAs are favorable in a high catalytic temperature, high KOH concentration, and high ethanol concentration.

Scalable Superior Chemical Sensing Performance of Stretchable Ionotronic Skin via a π-Hole Receptor Effect.

Skin-attachable gas sensors provide a next-generation wearable platform for real-time protection of human health by monitoring environmental and physiological chemicals. However, the creation of skin-like wearable gas sensors, possessing high sensitivity, selectivity, stability, and scalability (4S) simultaneously, has been a big challenge. Here, an ionotronic gas-sensing sticker (IGS) is demonstrated, implemented with free-standing polymer electrolyte (ionic thermoplastic polyurethane, i-TPU) as a sensing channel and inkjet-printed stretchable carbon nanotube electrodes, which enables the IGS to exhibit high sensitivity, selectivity, stability (against mechanical stress, humidity, and temperature), and scalable fabrication, simultaneously. The IGS demonstrates reliable sensing capability against nitrogen dioxide molecules under not only harsh mechanical stress (cyclic bending with the radius of curvature of 1 mm and cyclic straining at 50%), but also environmental conditions (thermal aging from -45 to 125 °C for 1000 cycles and humidity aging for 24 h at 85% relative humidity). Further, through systematic experiments and theoretical calculations, a π-hole receptor mechanism is proposed, which can effectively elucidate the origin of the high sensitivity (up to parts per billion level) and selectivity of the ionotronic sensing system. Consequently, this work provides a guideline for the design of ionotronic materials for the achievement of high-performance and skin-attachable gas-sensor platforms.

Ion adsorption-induced reversible polarization switching of a van der Waals layered ferroelectric.

Solid-liquid interface is a key concept of many research fields, enabling numerous physical phenomena and practical applications. For example, electrode-electrolyte interfaces with electric double layers have been widely used in energy storage and regulating physical properties of functional materials. Creating a specific interface allows emergent functionalities and effects. Here, we show the artificial control of ferroelectric-liquid interfacial structures to switch polarization states reversibly in a van der Waals layered ferroelectric CuInP2S6 (CIPS). We discover that upward and downward polarization states can be induced by spontaneous physical adsorption of dodecylbenzenesulphonate anions and N,N-diethyl-N-methyl-N-(2-methoxyethyl)-ammonium cations, respectively, at the ferroelectric-liquid interface. This distinctive approach circumvents the structural damage of CIPS caused by Cu-ion conductivity during electrical switching process. Moreover, the polarized state features super-long retention time (>1 year). The interplay between ferroelectric dipoles and adsorbed organic ions has been studied systematically by comparative experiments and first-principles calculations. Such ion adsorption-induced reversible polarization switching in a van der Waals ferroelectric enriches the functionalities of solid-liquid interfaces, offering opportunities for liquid-controlled two-dimensional ferroelectric-based devices.

Bidirectional heterostructures consisting of graphene and lateral MoS2/WS2 composites: a first-principles study.

First-principles calculations have been performed to explore the structural and electronic properties of bidirectional heterostructures composed of graphene and (MoS2) X /(WS2)4-X (X = 1, 2, 3) lateral composites and compare them with those of heterobilayers formed by graphene and pristine MS2 (M = Mo, W). The band gaps of the lateral heterostructures lie between those of pristine MoS2 and WS2. The weak coupling between the two layers can induce a tiny band-gap opening of graphene and formation of an n-type Schottky contact at the G-(MoS2) X /(WS2)4-X interface. Moreover, the combination ratio of MoS2/WS2 can control the electronic properties of G-(MoS2) X /(WS2)4-X . By applying external electric fields, the band gaps of (MoS2) X /(WS2)4-X (X = 0, 1, 2, 3, 4) monolayers undergo a direct-indirect transition, and semiconductor-metal transitions can be found in WS2. External electric fields can also be used effectively to tune the binding energies, charge transfers, and band structures (the types of Schottky and Ohmic contacts) of G-(MoS2) X /(WS2)4-X heterostructures. These findings suggest that G-(MoS2) X /(WS2)4-X heterostructures can serve as high-performance nano-electronic devices.