Oxygen Vacancy-Enhanced Centrosymmetric Breaking of SrFeO3- x for Piezoelectric-Catalyzed Synthesis of H2O2.

Normally, only noncentrosymmetric structure of the materials can potentially be piezoelectric. Thus, it is limited in the field of piezoelectricity for the centrosymmetric structure of the material. In this work, the performance of piezoelectricity is successfully achieved from centrosymmetric SrFeO3- x by modulating oxygen vacancies, which have a surface piezoelectric potential up to 93 mV by using Kelvin-probe force microscopy (KPFM). Moreover, the piezoelectric effects of SrFeO3- x are also evaluated by piezoelectric catalytic effect and density functional theory calculations (DFT). The results show that the piezo-catalytic degradation of tetracycline reaches 96% after 75 min by ultrasonic mechanical vibration and the production of H2O2 by SrFeO3- x piezoelectric synthesis could reach 1821 µmol L-1. In addition, the DFT results indicate that the intrinsic effect of oxygen vacancies effectively promotes the adsorption and activation of O2 and H2O as well as intermediates and improves the piezoelectric catalytic activity. This work provides an effective basis for realizing the piezoelectricity of centrosymmetric materials and regulating the development of piezoelectric catalytic properties.

Regulating Hydrogen/Oxygen Species Adsorption via Built-in Electric Field -Driven Electron Transfer Behavior at the Heterointerface for Efficient Water Splitting.

Alkaline water electrolysis (AWE) plays a crucial role in the realization of a hydrogen economy. The design and development of efficient and stable bifunctional catalysts for both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) are pivotal to achieving high-efficiency AWE. Herein, WC1-x/Mo2C nanoparticle-embedded carbon nanofiber (WC1-x/Mo2C@CNF) with abundant interfaces is successfully designed and synthesized. Benefiting from the electron transfer behavior from Mo2C to WC1-x, the electrocatalysts of WC1-x/Mo2C@CNF exhibit superior HER and OER performance. Furthermore, when employed as anode and cathode in membrane electrode assembly devices, the WC1-x/Mo2C@CNF catalyst exhibits enhanced catalytic activity and remarkable stability for 100 hours at a high current density of 200 mA cm-2 towards overall water splitting. The experimental characterizations and theoretical simulation reveal that modulation of the d-band center for WC1-x/Mo2C@CNF, achieved through the asymmetric charge distribution resulting from the built-in electric field induced by work function, enables optimization of adsorption strength for hydrogen/oxygen intermediates, thereby promoting the catalytic kinetics for overall water splitting. This work provides promising strategies for designing highly active catalysts in energy conversion fields.

Electrospun Cellulose Nanocrystals Reinforced Flexible Sensing Paper for Triboelectric Energy Harvesting and Dynamic Self-Powered Tactile Perception.

The technical synergy between flexible sensing paper and triboelectric nanogenerator (TENG) in the next stage of artificial intelligence Internet of Things engineering makes the development of intelligent sensing paper with triboelectric function very attractive. Therefore, it is extremely urgent to explore functional papers that are more suitable for triboelectric sensing. Here, a cellulose nanocrystals (CNCs) reinforced PVDF hybrid paper (CPHP) is developed by electrospinning technology. Benefitting from the unique effects of CNCs, CPHP forms a solid cross-linked network among fibers and obtains a high-strength (25 MPa) paper-like state and high surface roughness. Meanwhile, CNCs also improve the triboelectrification effect of CPHP by assisting the PVDF matrix to form more electroactive phases (96% share) and a higher relative permittivity (17.9). The CPHP-based TENG with single electrode configuration demonstrates good output performance (open-circuit voltage of 116 V, short-circuit current of 2.2 µA and power density of 91 mW m-2 ) and ultrahigh pressure-sensitivity response (3.95 mV Pa-1 ), which endows CPHP with reliable power supply and sensing capability. More importantly, the CPHP-based flexible self-powered tactile sensor with TENG array exhibits multifunctional applications in imitation Morse code compilation, tactile track recognition, and game character control, showing great prospects in the intelligent inductive device and human-machine interaction.

Constructing CoO/Mo2 C Heterostructures with Interfacial Electron Redistribution Induced by Work Functions for Boosting Overall Water Splitting.

Space charge transfer of heterostructures driven by the work-function-induced built-in field can regulate the electronic structure of catalysts and boost the catalytic activity. Herein, an epitaxial heterojunction catalyst of CoO/Mo2 C with interfacial electron redistribution induced by work functions (WFs) is constructed for overall water splitting via a novel top-down strategy. Theoretical simulations and experimental results unveil that the WFs-induced built-in field facilitates the electron transfer from CoO to Mo2 C through the formed "Co─C─Mo" bond at the interface of CoO/Mo2 C, achieving interfacial electron redistribution, further optimizing the Gibbs free energy of primitive reaction step and then accelerating kinetics of hydrogen evolution reaction (HER). As expected, the CoO/Mo2 C with interfacial effects exhibits excellent HER catalytic activity with only needing the overpotential of 107 mV to achieve 10 mA cm-2 and stability for a 60-h continuous catalyzing. Besides, the assembled CoO/Mo2 C behaves the outstanding performance toward overall water splitting (1.58 V for 10 mA cm-2 ). This work provides a novel possibility of designing materials based on interfacial effects arising from the built-in field for application in other fields.

Enhanced Visible-Photocatalytic Activities in Strong Acids and Strong Alkalis of Flexible Iron-SrTiO3 Nanofibrous Membranes.

Traditional SrTiO3 (STO) materials have high brittleness and poor deformation resistance. In this work, macroscopically flexible iron-doped SrTiO3 (SFTO) nanofibrous membranes were prepared by electrospinning and calcination, which can be easily isolated and can maintain integrity to recycle as photocatalysts. Moreover, the SFTO nanofibrous membranes showed enhanced photocatalytic performance under strong acids (pH = 2) and strong alkalis (pH = 12). The SFTO nanofibrous membranes increased the catalytic rate of Congo red (CR) dye by about 10 times in visible light. The mechanism of photocatalytic activity enhancement was discussed by the combined effects of hydroxyl radicals and superoxide radicals. The successful preparation of SFTO nanofibrous membranes has offered a simple and economical approach to photocatalysis as well as environmental remediation.

Extra storage capacity in transition metal oxide lithium-ion batteries revealed by in situ magnetometry.

In lithium-ion batteries (LIBs), many promising electrodes that are based on transition metal oxides exhibit anomalously high storage capacities beyond their theoretical values. Although this phenomenon has been widely reported, the underlying physicochemical mechanism in such materials remains elusive and is still a matter of debate. In this work, we use in situ magnetometry to demonstrate the existence of strong surface capacitance on metal nanoparticles, and to show that a large number of spin-polarized electrons can be stored in the already-reduced metallic nanoparticles (that are formed during discharge at low potentials in transition metal oxide LIBs), which is consistent with a space charge mechanism. Through quantification of the surface capacitance by the variation in magnetism, we further show that this charge capacity of the surface is the dominant source of the extra capacity in the Fe3O4/Li model system, and that it also exists in CoO, NiO, FeF2 and Fe2N systems. The space charge mechanism revealed by in situ magnetometry can therefore be generalized to a broad range of transition metal compounds for which a large electron density of states is accessible, and provides pivotal guidance for creating advanced energy storage systems.

Reacquainting the Electrochemical Conversion Mechanism of FeS2 Sodium-Ion Batteries by Operando Magnetometry.

In spite of the excellent electrochemical performance in lithium-ion batteries (LIBs), transition-metal compounds usually show inferior capacity and cyclability in sodium-ion batteries (SIBs), implying different reaction schemes between these two types of systems. Herein, coupling operando magnetometry with electrochemical measurement, we peformed a comprehensive investigation on the intrinsic relationship between the ion-embedding mechanisms and the electrochemical properties of the typical FeS2/Na (Li) cells. Operando magnetometry together with ex-situ transmission electron microscopy (TEM) measurement reveal that only part of FeS2 is involved in the conversion reaction process, while the unreactive parts form "inactive cores" that lead to the low capacity. Through quantification with Langevin fitting, we further show that the size of the iron grains produced by the conversion reaction are much smaller in SIBs than that in LIBs, which may lead to more serious pulverization, thereby resulting in worse cycle performance. The underlying reason for the above two above phenomena in SIBs is the sluggish kinetics caused by the larger Na-ion radius. Our work paves a new way for the investigation of novel SIB materials with high capacity and long durability.

Artificial blood vessel biofuel cell for self-powered blood glucose monitoring.

Biofuel cell (BFC) is a kind of bio-cell based on biological enzymes. The enzyme as a catalyst can interconvert renewable and sustainable energy into each other more rapidly, such as the biochemical energy in glucose and ethanol into electrical energy. In this work, artificial blood vessel and fuel cell are based on polyaniline/thermoplastic polyurethane (PANI/TPU) fiber membrane with an average fiber diameter of 1300 nm, a film thickness of 167µm, and a permeability of 18.4 mm s-1. The PANI/TPU fiber membrane was prepared by electrospinning and followedin situpolymerization. The membrane has good flexibility and mechanical properties, and can be stretched up to 200%. The advantages of good hydrophilicity, biocompatibility and high porosity make it possible to efficiently load glucose oxidase and laccase. The prepared BFC can stably output a voltage of 50 mV in simulated blood, and the output electrical signal changes significantly with the change of glucose concentration, which may be used in implantable devices or blood glucose monitoring.

Study of the exciton dynamics in perylene bisimide (PBI) aggregates with symmetrical quasiclassical dynamics based on the Meyer-Miller mapping Hamiltonian.

The exciton dynamics in one-dimensional stacked PBI (Perylene Bisimide) aggregates was studied with SQC-MM dynamics (Symmetrical Quasiclassical Dynamics based on the Meyer-Miller mapping Hamiltonian). Based on linear vibronic coupling models, one-dimensional PBI aggregates with different lengths were investigated. Based on an investigation of short PBI aggregates (10 sites and 80-140 modes) using both the SQC-MM and ML-MCTDH (multilayer multiconfigurational time-dependent Hartree) methods, we showed that SQC-MM dynamics give a reasonable description of the exciton dynamics for organic PBI aggregates composed of 101 sites and 808 modes. This allows us to employ SQC-MM dynamics in the explicit study of exciton diffusion for long one-dimensional PBI aggregates based on models with different site-site coupling strengths with/without static disorder by including all the involved electronic and vibrational degrees of freedom.

Self-powered portable melt electrospinning for in situ wound dressing.

BACKGROUND: Electrospun (e-spun) nanofibers for wound dressing have attracted wide attention due to its large specific surface area, large porosity and breathability. Compared with solution electrospinning (e-spinning), melt e-spinning is more bio-friendly without toxic solvent participation, which provides the possibility of in situ e-spinning on wounds directly. However, previously reported melt e-spinning devices were usually bulky and cumbersome due to their necessary heating unit, and different components were separated to avoid electrostatic interference. RESULTS: In this article, we report on a self-powered hand-held melt e-spinning gun which can work without any external power supply (outdoors). The problem of electrostatic interference for this integrated device was solved by using a special high heat transfer insulation unit. The apparatus is easy and safe to operate by a single hand due to its small volume (24 × 6 × 13 cm3) and light weight (about 450 g). Some biodegradable polymers, for example, polycaprolactone (PCL) fibers were successful e-spun onto wounds directly by using this dressing gun. CONCLUSIONS: PCL fibrous membrane has good biocompatibility and can be in situ electrospun to wound surface as a wound dressing by the portable melt e-spinning gun. Besides wound dressing, this hand-held melt e-spinning gun may be used in 3D printing and experimental teaching demonstration aids.

Chemical Modification of the sp-Hybridized Carbon Atoms of Graphdiyne by Using Organic Sulfur.

Here, a new approach to further improve graphdiyne (GDY) based materials by using benzyl disulfide (BDS) as the sulfur source is demonstrated. The S radicals, generated from the homolysis of BDS, can react with the acetylenic bonds and be well confined in the triangle-like pores of GDY, forming S-GDY. The as-prepared S-GDY, which possesses numerous heteroatom defects and active sites, is suitable for applications in many electronic devices, such as lithium ion batteries (LIBs). As expected, the assembled LIBs based on S-GDY displayed improved electrochemical properties, including larger capacity and superior rate capability.

Initial sampling in symmetrical quasiclassical dynamics based on Li-Miller mapping Hamiltonian.

A symmetrical quasiclassical (SQC) dynamics approach based on the Li-Miller (LM) mapping Hamiltonian (SQC-LM) was employed to describe nonadiabatic dynamics. In principle, the different initial sampling procedures may be applied in the SQC-LM dynamics, and the results may be dependent on different initial sampling. We provided various initial sampling approaches and checked their influence. We selected two groups of models including site-exciton models for exciton dynamics and linear vibronic coupling models for conical intersections to test the performance of SQC-LM dynamics with the different initial sampling methods. The results were examined with respect to those of the accurate multiconfigurational time-dependent Hartree (MCTDH) quantum dynamics. For both the models, the SQC-LM method more-or-less gives a reasonable description of the population dynamics, while the influence of the initial sampling approaches on the final results is noticeable. It seems that the suitable initial sampling methods should be determined by the system under study. This indicates that the combination of the SQC-LM method with a suitable sampling approach may be a potential method in the description of nonadiabatic dynamics.

Giant spontaneous exchange bias obtained by tuning magnetic compensation in samarium ferrite single crystals.

Spontaneous exchange bias (SEB) under zero field cooling (ZFC) has recently attracted lots of attention due to its underlying physics and potential applications. Here we report the giant SEB (GSEB) of SmFeO3 single crystals by tuning magnetic compensation by temperature, which is rather convenient. A SEB field of up to 1 T at 3.9 K after ZFC (-1.4 T at 3.9 K after field cooling) was obtained. The SEB shows reciprocal relationship with remnant magnetization.

Piezoluminescence from ferroelectric Ca3Ti2O7:Pr3+ long-persistent phosphor.

A variety of up-and-coming applications of piezoluminescence in artificial skins, structural health diagnosis, and mechano-driven lightings and displays recently have triggered an intense research effort to design and develop new piezoluminescent materials. In this work, we deduced and verified an efficient piezoluminescence in ferroelectric Ca3Ti2O7:Pr3+ long-persistent phosphor, in view of three fundamental elements forming piezoluminescence - piezoelectricity, luminescent centers and carrier traps. Under the stimulation of mechanical actions including compression and friction, Ca3Ti2O7:Pr3+ shows an intense red emission from 1D2-3H4 transition of Pr3+. On the basis of investigations on structural and optical characteristics especially photoluminescence, persistent luminescence and thermoluminescence, we finally proposed a possible piezoluminescent mechanism in Ca3Ti2O7:Pr3+. Our research is expected to expand the horizon of existing piezoluminescent materials, accelerating the development and application of new materials.

Multicolor Tuning in Room-Temperature Self-Activated Ca2 Nb2 O7 Submicroplates by Lanthanide Doping.

Self-activated phosphors are capable of generating optical emissions from the internal ion groups of host lattice before externally introducing luminescent ions. However, numerous self-activated phosphors only show luminescence at low temperature due to the thermally activated energy migration among ion groups at room temperature, severely confining their application conditions. In this letter, we propose a strategy to converting the low-temperature luminescence to a room-temperature one through changing the synthesis conditions to induce structural distortions and thus to limit energy migration. Room-temperature self-activated luminescence of Ca2 Nb2 O7 was accordingly achieved in submicroplates synthesized using the sol-gel method. By further coupling the blue broadband emission from Ca2 Nb2 O7 submicroplates with the characteristic luminescence of Ln3+ (Pr3+ , Sm3+ , and Dy3+ ) dopants, multicolor emissions were successively tuned through adjusting the concentration of Ln3+ . Our results are expected to expand the scope of designing room-temperature self-activated phosphors and tuning multicolor emission.

Ag/alginate nanofiber membrane for flexible electronic skin.

Flexible electronic skin has stimulated significant interest due to its widespread applications in the fields of human-machine interactivity, smart robots and health monitoring. As typical elements of electrical skin, the fabrication process of most pressure sensors combined nanomaterials and PDMS films are redundant, expensive and complicated, and their unknown biological toxicity could not be widely used in electronic skin. Hence, we report a novel, cost-effective and antibacterial approach to immobilizing silver nanoparticles into-electrospun Na-alginate nanofibers. Due to the unique role of carboxyl and hydroxyl groups in Na-alginate, the silver nanopaticles with 30 nm size in diameter were uniformly distributed inside and outside the alginate nanofibers, which obtained pressure sensor shows stable response, including an ultralow detection limited (1 pa) and high durability (>1000 cycles). Notably, the pressure sensor fabricated by these Ag/alginate nanofibers could not only follow human respiration but also accurately distinguish words like 'Nano' and 'Perfect' spoke by a tester. Interestingly, the pixelated sensor arrays based on these Ag/alginate nanofibers could monitor distribution of objects and reflect their weight by measuring the different current values. Moreover, these Ag/alginate nanofibers exhibit great antibacterial activity, implying the great potential application in artificial electronic skin.

Electrical conduction mechanism of an individual polypyrrole nanowire at low temperatures.

Conducting polypyrrole (PPY) nanowires doped with p-toluene sulfonamide (PTSA) were synthesized by a template-free self-assembly method. Electrical transport characteristics, i.e. current-voltage (I-V) behavior, of an individual PPY/PTSA nanowire have been explored in a wide temperature range from 300 down to 40 K. The fitting results of I-V curves indicated that the electrical conduction mechanism can be explained by the space-charge-limited current (SCLC) theory from 300 down to 100 K. In this temperature range, traps play an important role for this non-crystalline system. The corresponding trap energy and trap concentration have also been calculated based on the SCLC theory. Interestingly, there is no trap at 160 K, different from other temperatures. The obtained carrier mobility for the polymer nanowires is 0.964 cm(2) V(-1) s(-1) on the basis of trap free SCLC theory. In the temperature range of 80-40 K, little current can flow through the nanowire especially at lower voltages, however, the current follows the equation I ∞ (V/Vt-1)(ζ) at higher bias, which could be attributed to Coulomb blockade effect. Additionally, the differential conductance dI/dV curves also show some clear Coulomb oscillations.

Amorphous Fe2O3 Anchored on N-Doped Graphene with Internal Micro-Channels as an Active and Durable Anode for Sodium-Ion Batteries.

The reduced graphene oxide (rGO) exhibits outstanding electrical conductivity and a high specific surface area, making it a promising material for various applications. Fe2O3 is highly desirable due to its significant theoretical capacity and cost-effectiveness, high abundance, and environmental friendliness. However, the performance of these r-GO/Fe2O3 composite electrodes still needs to be further improved, especially in terms of cycle stability. The composite of Fe2O3 anchored on N-doped graphene with inside micro-channels (Fe2O3@N-GIMC) was used to be efficiently prepared. Because the inside channels can furnish extra transmission pathways and absorption websites and the interconnected structure can efficaciously forestall pulverization and aggregation of electrode materials. In addition, N doping is also beneficial to improve its electrochemical performance. Thus, it demonstrates exceptional sodium storage characteristics, including notable electrochemical activity, impressive initial Coulombic efficiency, and favorable rate performance. The optimized Fe2O3@N-GIMC indicates outstanding discharge capacity (573.5 mAh g-1 at 1 A g-1), significant rate performance (333.6 mAh g-1 at 8 A g-1), and stable long-term cycle durability (308.9 mAh g-1 after 1000 cycles at 1 A g-1, 200.8 mAh g-1 after 4000 cycles at 1 A g-1) as a sodium-ion battery anode. This presents a new approach for preparing graphene-based high-functional composites and lays a stable basis for further expanding its application field.

In-situ electrospinning with precise deposition of antioxidant nanofiber facial mask loaded with Enteromorpha prolifera polysaccharides.

In order to fabricate a novel antioxidant nanofiber facial mask, a metal cone modified in-situ electrospinning with precise deposition was employed by utilizing Enteromorpha prolifera polysaccharides (EPPs). The metal cone could control the deposition area to achieve precise fabrication of facial mask on skin. The EPPs exhibited remarkable antioxidant ability, as evidenced by the half-maximal inhibitory concentrations (IC50) of 1.44 mg/mL and 0.74 mg/mL against DPPH and HO• free radicals, respectively. The antioxidant ability of the facial mask was improved by elevating the electrospinning voltage from 15 kV to 19 kV, due to the improved release capacity of EPPs by 7.09 %. Moreover, the facial mask demonstrated robust skin adhesion and moisture-retaining properties compared with commercial facial mask, which was benefited by the in-situ electrospinning technology. Furthermore, cytotoxicity assay, animal skin irritation test, and ocular irritation test collectively affirmed the safety of the facial mask. Thus, this research introduces a novel in situ electrospinning with precise deposition method and a natural antioxidant additive for preparing facial mask.

Preparation and Peculiar Magnetic Properties at Low Temperatures of La1.85Sr0.15CuO4 Nanofibers.

Herein, the preparation process, morphology, structure, and magnetic properties of La1.85Sr0.15CuO4 (LSCO) cobweb-like nanofibers are reported. LSCO nanofibers with a regular grain size distribution are successfully prepared via electrospinning, followed by calcination. We conducted morphology analysis and elemental distribution using electron microscopy and energy-dispersive X-ray spectroscopy (EDS), respectively. Additionally, magnetic property testing was performed using a vibrating sample magnetometer (VSM) to confirm the superconducting properties of the samples. Interestingly, our samples exhibited a superconducting transition temperature, Tc, of 25.21 K, which showed some disparity compared to similar works. Furthermore, we observed a ferromagnetic response at low temperatures in the superconducting nanofibers. We attribute these phenomena to the effects generated by surface states of nanoscale superconducting materials.