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The pursuit of high-performance electronic devices has driven the research focus toward 2D semiconductors with high electron mobility and suitable band gaps. Previous studies have demonstrated that quasi-2D Bi2O2Se (BOSe) has remarkable physical properties and is a promising candidate for further exploration. Building upon this foundation, the present work introduces a novel concept for achieving nonvolatile and reversible control of BOSe's electronic properties. The approach involves the epitaxial integration of a ferroelectric PbZr0.2Ti0.8O3 (PZT) layer to modify BOSe's band alignment. Within the BOSe/PZT heteroepitaxy, through two opposite ferroelectric polarization states of the PZT layer, we can tune the Fermi level in the BOSe layer. Consequently, this controlled modulation of the electronic structure provides a pathway to manipulate the electrical properties of the BOSe layer and the corresponding devices.
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In addressing the generalization issue faced by data-driven methods in food origin traceability, especially when encountering diverse input variable sets, such as elemental contents (C, N, S), stable isotopes (C, N, S, H and O) and 43 elements measured under varying laboratory conditions. We introduce an innovative, versatile deep learning-based framework incorporating explainable analysis, adept at determining feature importance through learned neuron weights. Our proposed framework, validated using three rice sample batches from four Asian countries, totaling 354 instances, exhibited exceptional identification accuracy of up to 97%, surpassing traditional reference methods like decision tree and support vector machine. The adaptable methodological system accommodates various combinations of traceability indicators, facilitating seamless replication and extensive applicability. This groundbreaking solution effectively tackles generalization challenges arising from disparate variable sets across distinct data batches, paving the way for enhanced food origin traceability in real-world applications.
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Aprendizaje Profundo , Oryza , Oligoelementos , Isótopos de Carbono/análisis , Asia , Oligoelementos/análisisRESUMEN
Quasi van der Waals epitaxy is an approach to constructing the combination of 2D and 3D materials. Here, we quantify and discuss the 2D/3D interface structure and the corresponding features in metal/muscovite systems. High-resolution scanning transmission electron microscopy reveals the atomic arrangement at the interface. The theoretical results explain the formation mechanism and predict the mechanical robustness of these metal/muscovite quasi van der Waals epitaxies. The evidence of superior interface quality is delivered according to the outstanding performance of the designed systems in both retention (>105 s) and cycling tests (>105 cycles) through electromechanical measurements. With high-temperature X-ray reciprocal space mapping, the unique anisotropy of thermal expansion is discovered and predicted to sustain the thermal stress with a sizable thermal actuation. A maximum bending curvature of 264 m-1 at 243 °C can be obtained in the silver/muscovite heteroepitaxy. The electrothermal and photothermal methods show a fast response to thermal stress and demonstrate the interface robustness.
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Metal-organic frameworks (MOFs) and covalent organic frameworks (COFs) have been attracting tremendous attention in various applications due to their unique structural properties. Recent interest has been focused on their combination as hybrids to enable the engineering of new classes of frameworks with complementary properties. This review gives a comprehensive summary on the interfacial chemistries in MOF/COF hybrids, which play critical roles in their hybridization. The challenges and perspectives in the field of MOF/COF hybrids are also provided to inspire more efforts in diversifying this hybrid family and their cross-disciplinary applications.
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A high configurational entropy, achieved through a proper design of compositions, can minimize the Gibbs free energy and stabilize the quasi-equilibrium phases in a solid-solution form. This leads to the development of high-entropy materials with unique structural characteristics and excellent performance, which otherwise could not be achieved through conventional pathways. This work develops a high-entropy nonlinear dielectric system, based on the expansion of lead magnesium niobate-lead titanate. A dense and uniform distribution of nano-polar regions is observed in the samples owing to the addition of Ba, Hf, and Zr ions, which lead to enhanced performance of nonlinear dielectrics. The fact that no structural phase transformation is detected up to 250 °C, and no noticeable change or a steep drop in structural and electrical characteristics is observed at high temperatures suggests a robust thermal stability of the dielectric systems developed. With these advantages, these materials hold vast potential for applications such as dielectric energy storage, dielectric tunability, and electrocaloric effect. Thus, this work offers a new high-entropy configuration with elemental modulation, with enhanced dielectric material features.
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The application of high-entropy oxide (HEO) has attracted significant attention in recent years owing to their unique structural characteristics, such as excellent electrochemical properties and long-term cycling stability. However, the application of resistive random-access memory (RRAM) has not been extensively studied, and the switching mechanism of HEO-based RRAM has yet to be thoroughly investigated. In this study, HEO (Cr, Mn, Fe, Co, Ni)3 O4 with a spinel structure is epitaxially grown on a Nb:STO conductive substrate, and Pt metal is deposited as the top electrode. After the resistive-switching operation, some regions of the spinel structure are transformed into a rock-salt structure and analyzed using advanced transmission electron microscopy and scanning transmission electron microscopy. From the results of X-ray photoelectron spectroscopy and electron energy loss spectroscopy, only specific elements would change their valence state, which results in excellent resistive-switching properties with a high on/off ratio on the order of 105 , outstanding endurance (>4550 cycles), long retention time (>104 s), and high stability, which suggests that HEO is a promising RRAM material.
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Self-assembled systems have recently attracted extensive attention because they can display a wide range of phase morphologies in nanocomposites, providing a new arena to explore novel phenomena. Among these morphologies, a bicontinuous structure is highly desirable based on its high interface-to-volume ratio and 3D interconnectivity. A bicontinuous nickel oxide (NiO) and tin dioxide (SnO2) heteroepitaxial nanocomposite is revealed here. By controlling their concentration, we fabricated tuneable self-assembled nanostructures from pillars to bicontinuous structures, as evidenced by TEM-energy-dispersive X-ray spectroscopy with a tortuous compositional distribution. The experimentally observed growth modes are consistent with predictions by first-principles calculations. Phase-field simulations are performed to understand 3D microstructure formation and extract key thermodynamic parameters for predicting microstructure morphologies in SnO2:NiO nanocomposites of other concentrations. Furthermore, we demonstrate significantly enhanced photovoltaic properties in a bicontinuous SnO2:NiO nanocomposite macroscopically and microscopically. This research shows a pathway to developing innovative solar cell and photodetector devices based on self-assembled oxides.
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Pathogenic bacteria pose a great threat to global public health from environmental and public health perspectives, especially regarding the impact of the COVID-19 pandemic worldwide. As a result, the increased risk of pathogenic bioaerosol exposure imposes a considerable health burden and raises specific concerns about the layout and location of vaccine manufacturers. This study proposed a grid computing method based on the CALPUFF modelling system and population-based environmental risks to reduce bioaerosol-related potential risks. We previously used the CALPUFF model to quantify the diffusion level, the spatial distribution of emissions, and potential environmental risks of bioaerosol leakage in Gansu province's Zhongmu Lanzhou biopharmaceutical plant from July 24, 2019, to August 20, 2019. By combining it with publicly available test data, the credibility was confirmed. Based on our previous research, the CALPUFF model application combined with the environmental population-based environmental risks in two scenarios: the layout and site selection, was explored by using the leakage accident of Zhongmu Lanzhou biopharmaceutical plant of Gansu province as a case study. Our results showed that the site selection method of scenario 2 coupled with the buffer area was more reasonable than scenario 1, and the final layout site selection point of scenario 2 was grid 157 as the optimal layout point. The simulation results demonstrated agreement with the actual survey. Our findings could assist global bioaerosol manufacturers in developing appropriate layout and site selection strategies to reduce bioaerosol-related potential environmental risks.
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Productos Biológicos , COVID-19 , Humanos , Pandemias , Aerosoles y Gotitas Respiratorias , Salud Pública , ChinaRESUMEN
Recently various topological polar structures have been discovered in oxide thin films. Despite the increasing evidence of their switchability under electrical and/or mechanical fields, the dynamic property of isolated ones, which is usually required for applications such as data storage, is still absent. Here, we show the controlled nucleation and motion of isolated three-fold vertices under an applied electric field. At the PbTiO3/SrRuO3 interface, a two-unit-cell thick SrTiO3 layer provides electrical boundary conditions for the formation of three-fold vertices. Utilizing the SrTiO3 layer and in situ electrical testing system, we find that isolated three-fold vertices can move in a controllable and reversible manner with a velocity up to ~629 nm s-1. Microstructural evolution of the nucleation and propagation of isolated three-fold vertices is further revealed by phase-field simulations. This work demonstrates the ability to electrically manipulate isolated three-fold vertices, shedding light on the dynamic property of isolated topological polar structures.
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In condensed matter physics, oxide materials show various intriguing physical properties. Therefore, many efforts are made in this field to develop functional oxides. Due to the excellent potential for tin-based perovskite oxides, an expansion of new related functional compounds is crucial. This work uses a heteroepitaxial approach supported by theoretical calculation to stabilize PbSnO3 thin films with different orientations. The analyses of X-ray diffraction and transmission electron microscopy unveil the structural information. A typical antiferroelectric feature with double hysteresis and butterfly loops is observed through electrical characterizations consistent with the theoretical prediction. The phase transition is monitored, and the transition temperatures are determined based on temperature-dependent structural and electrical characterizations. Furthermore, the microscopic antiferroelectric order is noticed under atomic resolution images via scanning transmission electron microscopy. This work offers a breakthrough in synthesizing epitaxial PbSnO3 thin films and comprehensively understanding its anisotropic antiferroelectric behavior.
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Relaxor ferroelectric-based energy storage systems are promising candidates for advanced applications as a result of their fast speed and high energy storage density. In the research field of ferroelectrics and relaxor ferroelectrics, the concept of solid solution is widely adopted to modify the overall properties and acquire superior performance. However, the combination between antiferroelectric and paraelectric materials was less studied and discussed. In this study, paraelectric barium hafnate (BaHfO3) and antiferroelectric lead hafnate (PbHfO3) are selected to demonstrate such a combination. A paraelectric to relaxor ferroelectric, to ferroelectric, and to antiferroelectric transition is observed by varying the composition x in the (Ba1-xPbx)HfO3 solid solution from 0 to 100%. It is noteworthy that ferroelectric phases can be realized without primal ferroelectric material. This study creates an original solid solution system with a rich spectrum of competing phases and demonstrates an approach to design relaxor ferroelectrics for energy storage applications and beyond.
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Polar domain walls in centrosymmetric ferroelastics induce inhomogeneity that is the origin of advantageous multifunctionality. In particular, polar domain walls promote charge-carrier separation and hence are promising for energy conversion applications that overcome the hurdles of the rate-limiting step in the traditional photoelectrochemical water splitting processes. Yet, while macroscopic studies investigate the materials at the device scale, the origin of this phenomenon in general and the emergence of polar domain walls during the structural phase transition in particular has remained elusive, encumbering the development of this attractive system. Here, it is demonstrated that twin domain walls arise in centrosymmetric BiVO4 films and they exhibit localized piezoelectricity. It is also shown that during the structural phase transition from the tetragonal to monoclinic, the symmetry reduction is accompanied by an emergence of strain gradient, giving rise to flexoelectric effect and the polar domain walls. These results not only expose the emergence of polar domain walls at centrosymmetric systems by means of direct observation, but they also expand the realm of potential application of ferroelastics, especially in photoelectrochemistry and local piezoelectricity.
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Amorphous materials have attracted increasing attention in diverse fields due to their unique properties, yet their controllable fabrications still remain great challenges. Here, we demonstrate a top-down strategy for the fabrications of amorphous oxides through the amorphization of hydroxides. The versatility of this strategy has been validated by the amorphizations of unitary, binary and ternary hydroxides. Detailed characterizations indicate that the amorphization process is realized by the variation of coordination environment during thermal treatment, where the M-OH octahedral structure in hydroxides evolves to M-O tetrahedral structure in amorphous oxides with the disappearance of the M-M coordination. The optimal amorphous oxide (FeCoSn(OH)6-300) exhibits superior oxygen evolution reaction (OER) activity in alkaline media, where the turnover frequency (TOF) value is 39.4 times higher than that of FeCoSn(OH)6. Moreover, the enhanced OER performance and the amorphization process are investigated with density functional theory (DFT) and molecule dynamics (MD) simulations. The reported top-down fabrication strategy for fabricating amorphous oxides, may further promote fundamental research into and practical applications of amorphous materials for catalysis.
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Sacrifiers-promoted photocatalysis is a useful way to achieve high efficiency photoreduction and photocatalytic hydrogen production for photocatalysts of weak reductive power such as TiO2. Herein we report a new method to fabricate a unique dyadic hybrid consisting of closely compacted crystalline (anatase) and titanium glycerolate (TiG)-derived organic group-retained amorphous nanoparticles to validate adsorption-stored sacrifiers-promoted photocatalysis instead of using sacrifiers in bulk solution. It was found that ascorbic acid (AA)-modified TiG prepared at a small fraction of glycerol, characterized by peculiar cocoon/open nanocontainer-type morphologies, varieties of oxygen containing groups, and remarkably high specific surface area, is suitable for precursing such hybrids. AA can change crystallization processes and particle morphologies by terminating chain linkages in TiG structure, which increases porosity and brings about visible light responsive photocatalysis for the dyadic hybrid. Benefiting from good adsorption affinity to organic sacrifiers, the sacrifier-prestored hybrid can catalyze significantly enhanced photoreduction with good reproducibility toward dye molecules via the synergy of sacrifier enrichment and photocatalysis. AA modified TiG also exhibits good self-reducibility enabling pre-loading of highly dispersed and localized platinum nanoparticles, and the resulted dyadic hybrid facilitates photocatalytic hydrogen production of extremely higher turn-off frequency and better impurities interference-resistivity compared to the P25-based commercial catalyst.
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Nanopartículas del Metal , Titanio , Catálisis , Fotólisis , Platino (Metal) , Reproducibilidad de los ResultadosRESUMEN
Constructing highly efficient and cost-effective photocatalyst system has been a big challenge for photocatalysis. Herein, CdS nanosphere (N-CdS), hollow CdS (H-CdS) and a series of H-CdS@NiCoP core-shell nanospheres have been successfully prepared via a facile hydrothermal method. The activity test showed that H-CdS exhibited higher photocatalytic activity (3.34 mmol g-1h-1) compared with N-CdS (0.99 mmol g-1h-1) under visible light irradiation (λ ≥ 420 nm), suggesting that hollow structure could effectively improve photocatalytic activity. Moreover, the H-CdS@NiCoP-7 wt% displayed a maximum photocatalytic H2 evolution rate of 13.47 mmol g-1h-1, which was about 4 times and 2.5 times higher than that of pristine H-CdS and H-CdS@Pt-3 wt%, respectively. Furthermore, H-CdS@NiCoP-7 wt% exhibited a good stability during 20 h test. The physicochemical properties were characterized by XRD, SEM, TEM, XPS, UV-vis DRS, PL and photoelectrochemical technique. The results showed that NiCoP addition can construct p-n junction with H-CdS and effectively promote the charge transfer from CdS to NiCoP, which improved the photocatalytic hydrogen evolution activity. This work revealed that NiCoP could react as an excellent co-catalyst for enhancing H-CdS photocatalytic activity.
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Compuestos de Cadmio , Nanosferas , Catálisis , Hidrógeno , LuzRESUMEN
The ever-growing installation of solar power systems imposes severe challenges on the operations of local and regional power grids due to the inherent intermittency and variability of ground-level solar irradiance. In recent decades, solar forecasting methodologies for intra-hour, intra-day and day-ahead energy markets have been extensively explored as cost-effective technologies to mitigate the negative effects on the power grids caused by solar power instability. In this work, the progress in intra-hour solar forecasting methodologies are comprehensively reviewed and concisely summarized. The theories behind the forecasting methodologies and how these theories are applied in various forecasting models are presented. The reviewed mathematical tools include regressive methods, stochastic learning methods, deep learning methods, and genetic algorithm. The reviewed forecasting methodologies include data-driven methods, local-sensing methods, hybrid forecasting methods, and application orientated methods that generate probabilistic forecasts and spatial forecasts. Furthermore, suggestions to accelerate the development of future intra-hour forecasting methods are provided.
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The interaction of oxygen vacancies and ferroelectric domain walls is of great scientific interest because it leads to different domain-structure behaviors. Here, we use high-resolution scanning transmission electron microscopy to study the ferroelectric domain structure and oxygen-vacancy ordering in a compressively strained Bi0.9Ca0.1FeO3-δ thin film. It was found that atomic plates, in which agglomerated oxygen vacancies are ordered, appear without any periodicity between the plates in out-of-plane and in-plane orientation. The oxygen non-stoichiometry with δ ≈ 1 in FeO2-δ planes is identical in both orientations and shows no preference. Within the plates, the oxygen vacancies form 1D channels in a pseudocubic [010] direction with a high number of vacancies that alternate with oxygen columns with few vacancies. These plates of oxygen vacancies always coincide with charged domain walls in a tail-to-tail configuration. Defects such as ordered oxygen vacancies are thereby known to lead to a pinning effect of the ferroelectric domain walls (causing application-critical aspects, such as fatigue mechanisms and countering of retention failure) and to have a critical influence on the domain-wall conductivity. Thus, intentional oxygen vacancy defect engineering could be useful for the design of multiferroic devices with advanced functionality.
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The superparaelectric state delivers a new pathway for dielectric energy storage.