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Perovskite nanocrystals are advantageous for interfacial passivation of perovskite solar cells (PSCs), but the insulating long alkyl chain surface ligands impede the charge transfer, while the conventional ligand exchange would possibly introduce surface defects to the nanocrystals. In this work, we reported novel in situ modification of CsPbBr3 nanocrystals using a short chain conjugated molecule 2-methoxyphenylethylammonium iodide (2-MeO-PEAI) for interfacial passivation of PSCs. Transmission electron microscopy studies with atomic resolution unveil the transformation from cubic CsPbBr3 to Ruddlesden-Popper phase (RPP) nanocrystals due to halogen exchange. Synergic passivation by the RPP nanocrystals and 2-MeO-PEA+ has led to suppressed interface defects and enhanced charge carrier transport. Consequently, PSCs with in situ modified RPP nanocrystals achieved a champion power conversion efficiency of 24.39%, along with an improvement in stability. This work brings insights into the microstructural evolution of perovskite nanocrystals, providing a novel and feasible approach for interfacial passivation of PSCs.
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Uniform tensile ductility (UTD) is crucial for the forming/machining capabilities of structural materials. Normally, planar-slip induced narrow deformation bands localize the plastic strains and hence hamper UTD, particularly in body-centred-cubic (bcc) multi-principal element high-entropy alloys (HEAs), which generally exhibit early necking (UTD < 5%). Here we demonstrate a strategy to tailor the planar-slip bands in a Ti-Zr-V-Nb-Al bcc HEA, achieving a 25% UTD together with nearly 50% elongation-to-failure (approaching a ductile elemental metal), while offering gigapascal yield strength. The HEA composition is designed not only to enhance the B2-like local chemical order (LCO), seeding sites to disperse planar slip, but also to generate excess lattice distortion upon deformation-induced LCO destruction, which promotes elastic strains and dislocation debris to cause dynamic hardening. This encourages second-generation planar-slip bands to branch out from first-generation bands, effectively spreading the plastic flow to permeate the sample volume. Moreover, the profuse bands frequently intersect to sustain adequate work-hardening rate (WHR) to large strains. Our strategy showcases the tuning of plastic flow dynamics that turns an otherwise-undesirable deformation mode to our advantage, enabling an unusual synergy of yield strength and UTD for bcc HEAs.
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Diluents have been extensively employed to overcome the disadvantages of high viscosity and sluggish kinetics of high-concentration electrolytes, but generally do not change the pristine solvation structure. Herein, a weakly coordinating diluent, hexafluoroisopropyl methyl ether (HFME), is applied to regulate the coordination of Na+ with diglyme and anion and form a diluent-participated solvate. This unique solvation structure promotes the accelerated decomposition of anions and diluents, with the construction of robust inorganic-rich electrode-electrolyte interphases. In addition, the introduction of HFME reduces the desolvation energy of Na+, improves ionic conductivity, strengthens the antioxidant, and enhances the safety of the electrolyte. As a result, the assembled Na||Na symmetric cell achieves a stable cycle of over 1800â h. The cell of Na||P'2-Na0.67MnO2 delivers a high capacity retention of 87.3 % with a high average Coulombic efficiency of 99.7 % after 350â cycles. This work provides valuable insights into solvation chemistry for advanced electrolyte engineering.
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Sodium-ion batteries (SIBs) have garnered significant interest as one of the most promising energy suppliers for power grid energy storage. However, the poor electrode/electrolyte interfacial stability leads to continual electrolyte decomposition and transition metal dissolution, resulting in rapid performance degradation of SIBs. In this work, we propose a strategy integrating multiple functional bonds to regulate electrode/electrolyte interphase by triple-coupling of succinonitrile (SN), sodium hexafluorophosphate (NaPF6) and fluorinated ethylene carbonate (FEC). Theoretical calculation and experiment results show that the solvation structure of Na+ and ClO4 - is effectively reconfigured by the solvated FEC, SN and PF6 - in PC-based carbonate electrolyte. The newly developed electrolyte demonstrates increased Na+-FEC coordination, weakened interaction of Na+-PC and participation of SN and PF6 - anions in solvation, resulting in the formation of a conformal interfacial layer comprising of sodium oxynitrides (NaNxOy), sodium fluoride (NaF) and phosphorus oxide compounds (NaPxOy). Consequently, a 3â Ah pouch full cell of hard carbon//NaNi1/3Fe1/3Mn1/3O2 exhibits an excellent capacity retention of 90.4 % after 1000â cycles. Detailed postmortem analysis of interface chemistry is further illustrated by multiple characterization methods. This study provides a new avenue for developing electrolyte formulations with multiple functional bonds integrated interphases to significantly improve the long-term cycling stability of SIBs.
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Conversion-type electrode materials have gained massive research attention in sodium-ion batteries (SIBs), but their limited reversibility hampers practical use. Herein, we report a bifunctional nanoreactor to boost highly reversible sodium-ion storage, wherein a record-high reversible degree of 85.65% is achieved for MoS2 anodes. Composed of nitrogen-doped carbon-supported single atom Mn (NC-SAMn), this bifunctional nanoreactor concurrently confines active materials spatially and catalyzes reaction kinetics. In-situ/ex-situ characterizations including spectroscopy, microscopy, and electrochemistry, combined with theoretical simulations containing density functional theory and molecular dynamics, confirm that the NC-SAMn nanoreactors facilitate the electron/ion transfer, promote the distribution and interconnection of discharging products (Na2S/Mo), and reduce the Na2S decomposition barrier.As a result, the nanoreactor-promoted MoS2 anodes exhibit ultra-stable cycling with a capacity retention of 99.86% after 200 cycles in the full cell. This work demonstrates the superiority of bifunctional nanoreactors with two-dimensional confined and catalytic effects, providing a feasible approach to improve the reversibility for a wide range of conversion-type electrode materials, thereby enhancing the application potential for long-cycled SIBs.
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Atomically dispersed nitrogen-coordinated 3d transition-metal site on carbon support (M-NC) are promising alternatives to Pt group metal-based catalysts toward oxygen reduction reaction (ORR). However, despite the excellent activities of most of M-NC catalysts, such as Fe-NC, Co-NC et al., their durability is far from satisfactory due to Fenton reaction. Herein, this work reports a novel Si-doped Ni-NC catalyst (Ni-SiNC) that possesses high activity and excellent stability. X-ray absorption fine structure and aberration-corrected transmission electron microscopy uncover that the single-atom Ni site is coordinated with one Si atom and three N atoms, constructing Ni-Si1 N3 moiety. The Ni-SiNC catalyst exhibits a half-wave potential (E1/2 ) of 0.866 V versus RHE, with a distinguished long-term durability in alkaline media of only 10 mV negative shift in E1/2 after 35 000 cycles, which is also validated in Zn-air battery. Density functional theory calculations reveal that the Ni-Si1 N3 moiety facilitates ORR kinetics through optimizing the adsorption of intermediates.
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Polymer electrolyte membrane fuel cells (PEMFCs) running on hydrogen are attractive alternative power supplies for a range of applications, with in situ release of the required hydrogen from a stable liquid offering one way of ensuring its safe storage and transportation before use. The use of methanol is particularly interesting in this regard, because it is inexpensive and can reform itself with water to release hydrogen with a high gravimetric density of 18.8 per cent by weight. But traditional reforming of methanol steam operates at relatively high temperatures (200-350 degrees Celsius), so the focus for vehicle and portable PEMFC applications has been on aqueous-phase reforming of methanol (APRM). This method requires less energy, and the simpler and more compact device design allows direct integration into PEMFC stacks. There remains, however, the need for an efficient APRM catalyst. Here we report that platinum (Pt) atomically dispersed on α-molybdenum carbide (α-MoC) enables low-temperature (150-190 degrees Celsius), base-free hydrogen production through APRM, with an average turnover frequency reaching 18,046 moles of hydrogen per mole of platinum per hour. We attribute this exceptional hydrogen production-which far exceeds that of previously reported low-temperature APRM catalysts-to the outstanding ability of α-MoC to induce water dissociation, and to the fact that platinum and α-MoC act in synergy to activate methanol and then to reform it.
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Copper is known as a conductive metal but an inert catalyst for the hydrogen evolution reaction due to its inappropriate electronic structure. In this work, an active copper catalyst is prepared with high-energy surfaces by adopting the friction stir welding (FSW) technique. FSW can mix the immiscible Fe and Cu materials homogenously and heat them to a high temperature. Resultantly, α-Fe transforms into γ-Fe, and low-energy γ-Fe (100) and (110) surfaces induce the epitaxial growth of high-energy Cu (110) and (100) planes, respectively. After the removal of γ-Fe by acid etching, the copper electrode exposes high-energy surface and exhibits excellent acidic HER activity, even being superior to Pt foil at high current densities (>66 mA cm-2 ). Density functional theory calculation reveals that the high-energy surface favors the adsorption of hydrogen intermediate, thus accelerating the hydrogen evolution reaction. The epitaxial growth induced by FSW opens a new avenue toward engineering high-performance catalysts. In addition, FSW makes it possible to massively fabricate low-cost catalyst, which is advantageous to industrial application.
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Despite the rapid development of perovskite solar cells (PSCs) over the past few years, the conversion of solar energy into electricity is not efficient enough or cost-competitive yet. The principal energy loss in the conversion of solar energy to electricity fundamentally originates from the non-absorption of low-energy photons ascribed to Shockley-Queisser limits and thermalization losses of high-energy photons. Enhancing the light-harvesting efficiency of the perovskite photoactive layer by developing efficient photo management strategies with functional materials and arrays remains a long-standing challenge. Here, we briefly review the historical research trials and future research trends to overcome the fundamental loss mechanisms in PSCs, including upconversion, downconversion, scattering, tandem/graded structures, texturing, anti-reflection, and luminescent solar concentrators. We will deeply emphasize the availability and analyze the importance of a fine device structure, fluorescence efficiency, material proportion, and integration position for performance improvement. The unique energy level structure arising from the 4fn inner shell configuration of the trivalent rare-earth ions gives multifarious options for efficient light-harvesting by upconversion and downconversion. Tandem or graded PSCs by combining a series of subcells with varying bandgaps seek to rectify the spectral mismatch. Plasmonic nanostructures function as a secondary light source to augment the light-trapping within the perovskite layer and carrier transporting layer, enabling enhanced carrier generation. Texturing the interior using controllable micro/nanoarrays can realize light-matter interactions. Anti-reflective coatings on the top glass cover of the PSCs bring about better transmission and glare reduction. Photon concentration through perovskite-based luminescent solar concentrators offers a path to increase efficiency at reduced cost and plays a role in building-integrated photovoltaics. Distinct from other published reviews, we here systematically and hierarchically present all of the photon management strategies in PSCs by presenting the theoretical possibilities and summarizing the experimental results, expecting to inspire future research in the field of photovoltaics, phototransistors, photoelectrochemical sensors, photocatalysis, and especially light-emitting diodes. We further assess the overall possibilities of the strategies based on ultimate efficiency prospects, material requirements, and developmental outlook.
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BACKGROUND: Fast identification of damaged soybean seeds has undeniable importance in seed sorting and food quality. Mechanical vibration is generally used in soybean seed sorting, but this can seriously damage soybean seeds. The convolutional neural network (CNN) is considered an effective method for location and segmentation tasks. However, a CNN requires a large amount of ground truth data and has high computational cost. RESULTS: First, we propose a self-supervision manner to automatically generate ground truths, which can theoretically create an almost unlimited number of labeled images. Second, instead of using popular CNNs, a novel invertible convolution (involution)-enabled scheme is proposed by using the bottleneck block of the residual networks. Third, a feature selection feature pyramid network (FS-FPN) based on involution is designed, which selects features more flexibly and adaptively. We further merge involution-based backbones and FS-FPN into a unified network, achieving an end-to-end seed location and segmentation model; the best mean average precision of location and segmentation achieved was 85.1% and 81% respectively. CONCLUSION: The experimental results demonstrate that the proposed method greatly improves the performance of the baseline network with faster speed and fewer parameters, enabling it to detect soybean seeds more effectively. © 2022 Society of Chemical Industry.
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Glycine max , Processamento de Imagem Assistida por Computador , Processamento de Imagem Assistida por Computador/métodos , Redes Neurais de Computação , SementesRESUMO
Atomically ordered bimetal interfaces typically develop in near-equilibrium epitaxial growth (bottom-up processing) of nanolayered composite films and have been considered responsible for a number of intriguing material properties. Here, we discover that interfaces of such atomic level order can also emerge ubiquitously in large-scale layered nanocomposites fabricated by extreme strain (top down) processing. This is a counterintuitive result, which we propose occurs because extreme plastic straining creates new interfaces separated by single crystal layers of nanometer thickness. On this basis, with atomic-scale modeling and crystal plasticity theory, we prove that the preferred bimetal interface arising from extreme strains corresponds to a unique stable state, which can be predicted by two controlling stability conditions. As another testament to its stability, we provide experimental evidence showing that this interface maintains its integrity in further straining (strains > 12), elevated temperatures (> 0.45 Tm of a constituent), and irradiation (light ion). These results open a new frontier in the fabrication of stable nanomaterials with severe plastic deformation techniques.
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Underwater image enhancement has become the requirement for more people to have a better visual experience or to extract information. However, underwater images often suffer from the mixture of color distortion and blurred quality degradation due to the external environment (light attenuation, background noise and the type of water). To solve the above problem, we design a Divide-and-Conquer network (DC-net) for enhancing underwater image, which mainly consists of a texture network, a color network and a refinement network. Specifically, the multi-axis attention block is presented in the texture network, which combine different region/channel features into a single stream structure. And the color network employs an adaptive 3D look-up table method to obtain the color enhanced results. Meanwhile, the refinement network is presented to focus on image features of ground truth. Compared to state-of-the-art (SOTA) underwater image enhance methods, our proposed method can obtain the better visual quality of underwater images and better qualitative and quantitative performance. The code is publicly available at https://github.com/zhengshijian1993/DC-Net.
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Aumento da Imagem , Decoração de Interiores e Mobiliário , Humanos , ÁguaRESUMO
The instability of palladium-based binary alloys hinders their wide application in the oxygen reduction processes. Here, we prepared Mo-doped PdCu nanoparticles with controllable dopant content and valence. Further research has revealed that Mo, particularly Mo5+, may effectively suppress the oxidation of Pd and Cu, optimize the oxygen binding of Pd, and increase catalytic activity and stability. In particular, Mo-PdCu-1/C with the highest Mo5+ content shows the best oxygen reduction reaction (ORR) mass activity (1.20 A mg-1Pd), which is 4.8 times higher than that of PdCu/C. It also exhibits outstanding stability, retaining 80.8% of the original mass activity after 20 000 cycles. This study clearly explains the mechanism by which Mo doping affects the performance and provides a reference for further optimization of catalyst performance for fuel cell industrialization.
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The oxygen evolution reaction is known to be a kinetic bottleneck for water splitting. Triggering the lattice oxygen oxidation mechanism (LOM) can break the theoretical limit of the conventional adsorbate evolution mechanism and enhance the oxygen evolution reaction kinetics, yet the unsatisfied stability remains a grand challenge. Here, we report a high-entropy MnFeCoNiCu layered double hydroxide decorated with Au single atoms and O vacancies (AuSA-MnFeCoNiCu LDH), which not only displays a low overpotential of 213 mV at 10 mA cm-2 and high mass activity of 732.925 A g-1 at 250 mV overpotential in 1.0 M KOH, but also delivers good stability with 700 h of continuous operation at ~100 mA cm-2. Combining the advanced spectroscopic techniques and density functional theory calculations, it is demonstrated that the synergistic interaction between the incorporated Au single atoms and O vacancies leads to an upshift in the O 2p band and weakens the metal-O bond, thus triggering the LOM, reducing the energy barrier, and boosting the intrinsic activity.
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Pest disaster severely reduces crop yield and recognizing them remains a challenging research topic. Existing methods have not fully considered the pest disaster characteristics including object distribution and position requirement, leading to unsatisfactory performance. To address this issue, we propose a robust pest detection network by two customized core designs: multi-scale super-resolution (MSR) feature enhancement module and Soft-IoU (SI) mechanism. The MSR (a plug-and-play module) is employed to improve the detection performance of small-size, multi-scale, and high-similarity pests. It enhances the feature expression ability by using a super-resolution component, a feature fusion mechanism, and a feature weighting mechanism. The SI aims to emphasize the position-based detection requirement by distinguishing the performance of different predictions with the same Intersection over Union (IoU). In addition, to prosper the development of agricultural pest detection, we contribute a large-scale light-trap pest dataset (named LLPD-26), which contains 26-class pests and 18,585 images with high-quality pest detection and classification annotations. Extensive experimental results over multi-class pests demonstrate that our proposed method achieves the best performance by 67.4% of mAP on the LLPD-26 while being 15.0 and 2.7% gain than state-of-the-art pest detection AF-RCNN and HGLA respectively. Ablation studies verify the effectiveness of the proposed components.
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Wheat spike detection has important research significance for production estimation and crop field management. With the development of deep learning-based algorithms, researchers tend to solve the detection task by convolutional neural networks (CNNs). However, traditional CNNs equip with the inductive bias of locality and scale-invariance, which makes it hard to extract global and long-range dependency. In this paper, we propose a Transformer-based network named Multi-Window Swin Transformer (MW-Swin Transformer). Technically, MW-Swin Transformer introduces the ability of feature pyramid network to extract multi-scale features and inherits the characteristic of Swin Transformer that performs self-attention mechanism by window strategy. Moreover, bounding box regression is a crucial step in detection. We propose a Wheat Intersection over Union loss by incorporating the Euclidean distance, area overlapping, and aspect ratio, thereby leading to better detection accuracy. We merge the proposed network and regression loss into a popular detection architecture, fully convolutional one-stage object detection, and name the unified model WheatFormer. Finally, we construct a wheat spike detection dataset (WSD-2022) to evaluate the performance of the proposed methods. The experimental results show that the proposed network outperforms those state-of-the-art algorithms with 0.459 mAP (mean average precision) and 0.918 AP50. It has been proved that our Transformer-based method is effective to handle wheat spike detection under complex field conditions.
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Crystalline-amorphous composite have the potential to achieve high strength and high ductility through manipulation of their microstructures. Here, we fabricate a TiZr-based alloy with micrometer-size equiaxed grains that are made up of three-dimensional bicontinuous crystalline-amorphous nanoarchitectures (3D-BCANs). In situ tension and compression tests reveal that the BCANs exhibit enhanced ductility and strain hardening capability compared to both amorphous and crystalline phases, which impart ultra-high yield strength (~1.80 GPa), ultimate tensile strength (~2.3 GPa), and large uniform ductility (~7.0%) into the TiZr-based alloy. Experiments combined with finite element simulations reveal the synergetic deformation mechanisms; i.e., the amorphous phase imposes extra strain hardening to crystalline domains while crystalline domains prevent the premature shear localization in the amorphous phases. These mechanisms endow our material with an effective strength-ductility-strain hardening combination.
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The osteogenic activity of medical metal can be improved by lowering its surface stiffness and elastic modulus. However, it is very difficult to directly reduce the elastic modulus of medical metal surfaces. In this paper, with selected parameters, the titanium surface was treated via femtosecond laser irradiation. Micro indentation revealed that the femtosecond laser ablation can effectively reduce the surface Young's modulus and Vickers hardness of titanium. Besides, In order to explain the mechanical properties of degradation of titanium surface, Large-scale Atomic/Molecular Massively Parallel Simulator (LAMMPS) was used to simulate the process of laser ablation process of titanium surface, and it was found that after the ablation of titanium surface, voids were produced in the subsurface layer. The simulation showed that the voids are formed by the cavitation of metastable liquid induced by high tensile stress and high temperature during femtosecond laser irradiation. Subsurface voids with a thickness of about 40 nm were observed under the oxide layer in the experiment. Cell experiments showed that the surface with low Young's modulus was more conducive to cell proliferation and osteogenic differentiation.
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Nanoporos , Osteogênese , Lasers , Próteses e Implantes , Propriedades de Superfície , TitânioRESUMO
In advanced fission and fusion reactors, structural materials suffer from high dose irradiation by energetic particles and are subject to severe microstructure damage. He atoms, as a byproduct of the (n, α) transmutation reaction, could accumulate to form deleterious cavities, which accelerate radiation-induced embrittlement, swelling and surface deterioration, ultimately degrade the service lifetime of reactor materials. Extensive studies have been performed to explore the strategies that can mitigate He ion irradiation damage. Recently, nanostructured materials have received broad attention because they contain abundant interfaces that are efficient sinks for radiation-induced defects. In this review, we summarize and analyze the current understandings on interface effects on He ion irradiation in nanostructured materials. Some key challenges and research directions are highlighted for studying the interface effects on radiation damage in nanostructured materials.
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Electrocatalytic hydrogen evolution has attracted a great deal of attention due to the urgent need for clean energy. Herein, we demonstrate the synthesis of ternary pyrite-type cobalt phosphosulphide (CoPS) nanoparticles supported on a nitrogen-doped carbon matrix, CoPS/N-C, through carbonization and subsequent phosphosulfurization of Co-based zeolitic imidazolate frameworks (ZIF-67), as promising hydrogen evolution reaction (HER) electrocatalysts in both acidic and alkaline solutions. The polyhedral structure of ZIF-67 can be well maintained in the as-prepared CoPS/N-C nanocomposites. In particular, CoPS/N-C provides a geometric catalytic current density of -10 mA cm-2 at overpotentials of -80 and -148 mV vs. a reversible hydrogen electrode (RHE) and a Tafel slope of 68 and 78 mV dec-1 in 0.5 M H2SO4 and 1 M KOH, respectively, which is superior to most of the transition metal phosphosulfide materials. This MOF-derived synthesis of a transition metal phosphosulfide supported heteroatom-doped carbon matrix provides a promising opportunity for the development of highly efficient electrocatalysts for renewable energy devices.