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1.
Nanomicro Lett ; 17(1): 24, 2024 Sep 27.
Artículo en Inglés | MEDLINE | ID: mdl-39331290

RESUMEN

Defects-rich heterointerfaces integrated with adjustable crystalline phases and atom vacancies, as well as veiled dielectric-responsive character, are instrumental in electromagnetic dissipation. Conventional methods, however, constrain their delicate constructions. Herein, an innovative alternative is proposed: carrageenan-assistant cations-regulated (CACR) strategy, which induces a series of sulfides nanoparticles rooted in situ on the surface of carbon matrix. This unique configuration originates from strategic vacancy formation energy of sulfides and strong sulfides-carbon support interaction, benefiting the delicate construction of defects-rich heterostructures in MxSy/carbon composites (M-CAs). Impressively, these generated sulfur vacancies are firstly found to strengthen electron accumulation/consumption ability at heterointerfaces and, simultaneously, induct local asymmetry of electronic structure to evoke large dipole moment, ultimately leading to polarization coupling, i.e., defect-type interfacial polarization. Such "Janus effect" (Janus effect means versatility, as in the Greek two-headed Janus) of interfacial sulfur vacancies is intuitively confirmed by both theoretical and experimental investigations for the first time. Consequently, the sulfur vacancies-rich heterostructured Co/Ni-CAs displays broad absorption bandwidth of 6.76 GHz at only 1.8 mm, compared to sulfur vacancies-free CAs without any dielectric response. Harnessing defects-rich heterostructures, this one-pot CACR strategy may steer the design and development of advanced nanomaterials, boosting functionality across diverse application domains beyond electromagnetic response.

2.
Water Res ; 261: 121985, 2024 Sep 01.
Artículo en Inglés | MEDLINE | ID: mdl-38968734

RESUMEN

This study introduces a novel approach to transport modelling by integrating experimentally derived causal priors into neural networks. We illustrate this paradigm using a case study of metformin, a ubiquitous pharmaceutical emerging pollutant, and its transport behaviour in sandy media. Specifically, data from metformin's sandy column transport experiment was used to estimate unobservable parameters through a physics-based model Hydrus-1D, followed by a data augmentation to produce a more comprehensive dataset. A causal graph incorporating key variables was constructed, aiding in identifying impactful variables and estimating their causal dynamics or "causal prior." The causal priors extracted from the augmented dataset included underexplored system parameters such as the type-1 sorption fraction F, first-order reaction rate coefficient α, and transport system scale. Their moderate impact on the transport process has been quantitatively evaluated (normalized causal effect 0.0423, -0.1447 and -0.0351, respectively) with adequate confounders considered for the first time. The prior was later embedded into multilayer neural networks via two methods: causal weight initialization and causal prior regularization. Based on the results from AutoML hyperparameter tuning experiments, using two embedding methods simultaneously emerged as a more advantageous practice since our proposed causal weight initialization technique can enhance model stability, particularly when used in conjunction with causal prior regularization. amongst those experiments utilizing both techniques, the R-squared values peaked at 0.881. This study demonstrates a balanced approach between expert knowledge and data-driven methods, providing enhanced interpretability in black-box models such as neural networks for environmental modelling.


Asunto(s)
Metformina , Redes Neurales de la Computación , Porosidad , Contaminantes Químicos del Agua/química
3.
Biochem Genet ; 2024 Jul 30.
Artículo en Inglés | MEDLINE | ID: mdl-39080126

RESUMEN

As a tool for acquiring uncharacterized genomic DNA adjacent to characterized DNA, genome-walking is integral to bioscience-related research works. Herein, a new genome-walking tool known as N7-ended walker PCR (polymerase chain reaction) is presented. The key aspect for this method is the use of a degenerate walker primer in secondary/tertiary PCR. The 7 nt 5' tail of this primer completely degenerates to N7 relative to its corresponding primary walker primer. The degeneracy reduces the efficiency of annealing this primer to its predecessor site. Clearly, primary nontarget DNA defined by the primary walker primer prefers to form a hairpin structure via the inverted ends rather than hybridizing with the degenerate primer. As a result, N7-ended walker PCR achieves genome-walking by selectively boosting the DNA of interest. The feasibility of the N7-ended walker PCR method was proven by acquiring uncharacterized DNAs flanking several characterized DNAs.

4.
iScience ; 27(5): 109725, 2024 May 17.
Artículo en Inglés | MEDLINE | ID: mdl-38706866

RESUMEN

The growth of environmentally sensitive complex-shaped electronic devices (ECEDs) has led to a surging demand for flexible electromagnetic wave (EMW) absorbers. Herein, the water loss property of hydrogel was ingeniously applied for the flexible encapsulation (FE) of ECEDs. To be specific, saturated state (SGT) hydrogels were prepared by chemical cross-linking, and the hydrogen bond dissipation network promoted FE. Additionally, SGT has an effective absorption bandwidth (EAB) of 6.04 GHz at 1.65 mm due to the presence of dipole polarization. With the loss of water, SGT transitions to its natural state (NGT), and the decreasing conductivity leads to better impedance matching. NGT exhibited a broader EAB (9.20 GHz at 2.65 mm) and also strength and lightness (density of 0.3 g cm-3). Furthermore, the semi-automatic reversible cyclic transformation between SGT and NGT gels further broadens application scenarios. GT gel combines self-encapsulation and self-optimized performance as a potential EMW absorber for FE.

5.
Small ; 20(36): e2402078, 2024 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-38698575

RESUMEN

The strategic regulation of condensed state structures in multicomponent nanomaterials has emerged as an effective approach for achieving controllable electromagnetic (EM) properties. Herein, a novel conformation-mediated strategy is proposed to manipulate the condensed states of Co and C, as well as their interaction. The conformation of polyvinylpyrrolidone molecules is adjusted using a gradient methanol/water ratio, whereby the coordination dynamic equilibrium effectively governs the deposition of metal-organic framework precursors. This process ultimately influences the combined impact of derived Co and C in the resulting Co/C nanocomposites post-pyrolysis. The experimental results show that the condensed state structure of Co/C nanocomposites transitions from agglomerate state → to biphasic compact state → to loose packing state. Benefiting from the tunable collaboration between interfacial polarization and defects polarization, and the appropriate electrical conductivity, the diphasic compact state of Co/C nanocomposites achieves an effective absorbing bandwidth of 7.12 GHz (2.1 mm) and minimum reflection loss of -32.8 dB. This study highlights the significance of condensed state manipulation in comprehensively regulating the EM wave absorption characteristics of carbon-based magnetic metal nanocomposites, encompassing factors such as conductivity loss, magnetic loss, defect polarization, and interface polarization.

6.
Small ; 20(37): e2400756, 2024 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-38709225

RESUMEN

The direct application of liquid marbles in electromagnetic wave (EMW) absorption is challenging due to their poor stability, susceptibility to gravitational collapse, and shaping difficulties. To address this issue, a novel strategy is proposed to incorporate liquid marble microstructures (NaCl/nano-SiO2) encapsulated in organic phases (Octadecane) into the rubber-matrix (SEBS) using the ultrasound-assisted emulsion blending method. The resulting NaCl/SiO2/Octadecane microstructures anchored to SEBS offer a substantial solid-liquid interface consisting of NaCl solution and SiO2. When subjected to an alternating electromagnetic (EM) field, the water molecules and polysorbate within SiO2 exhibit heightened responsiveness to the EM field, and the movement of Na+ and Cl- within these microstructures leads to their accumulation at the solid-liquid interface, creating an asymmetric ion distribution. This phenomenon facilitates enhanced interfacial polarization, thereby contributing to the material's EMW absorption properties. Notably, the latex with 16 wt% SEBS (E-3), exhibiting a surface morphology similar to human cell tissues, achieves complete absorption of X-band (fE = 4.20 GHz, RLmin = -33.87 dB). Moreover, the latex demonstrates light density (0.78 g cm-3) and environmental stability. This study not only highlights the predominant loss mechanism in rubber-based wave-absorbing materials but also provides valuable insights into the design of multifunctional wave-absorbing materials.

7.
Small ; 20(31): e2309773, 2024 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-38461545

RESUMEN

An emerging carbothermal shock method is an ultra-convenient strategy for synthesizing high-entropy alloys (HEAs), in which the intelligent combination of carbon support and HEAs can be serve as a decisive factor for interpreting the trade-off relationship between conductive gene and dielectric gene. However, the feedback mechanism of HEAs ordering degree on electromagnetic (EM) response in 2-18 GHz has not been comprehensively demystified. Herein, while lignin-based carbon fiber paper (L-CFP) as carbon support, L-CFP/FeCoNiCuZn-X with is prepared by carbothermal shock method. The reflection loss of -82.6 dB with thickness of 1.31 mm is achieved by means of pointing electron enrichment within L-CFP/FeCoNiCuZn HEAs heterointerfaces verified by theoretical calculations. Simultaneously, low-frequency evolution with high-intensity and broadband EM response relies on a "sacrificing" strategy achieved by construction of polymorphic L-CFP/semi-disordered-HEAs heterointerfaces. The practicality of L-CFP/FeCoNiCuZn-X in complex environments is given prominence to thermal conductivity, hydrophobicity, and electrocatalytic property. This work is of great significance for insightful mechanism analysis of HEAs in the application of electromagnetic wave absorption.

8.
Adv Mater ; 36(23): e2314233, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38380795

RESUMEN

The electron migration polarization is considered as a promising approach to optimize electromagnetic waves (EMW) dissipation. However, it is still difficult to realize well-controlled electron migration and elucidate the related EMW loss mechanisms for current researches. Herein, a novel FexN@NGC/Ce system to construct an effective electron migration model based on the electron leaps among the 4f/5d/6s orbitals of Ce ions is explored. In Fe4N@NGC/CeSA+Cs+NPs, Ce single-atoms (SA) mainly represent a +3 valence state, which can feed the electrons to Ce4+ of clusters (Cs) and CeO2 nanoparticles (NPs) through a conductive network under EMW, leading to the electron migration polarization. Such electron migration loss combined with excellent magnetic loss provided by Fe4N core, results in the optimal EMW attenuation performance with a minimum reflection loss exceeds -85.1 dB and a broadened absorption bandwidth up to 7.5 GHz at 1.5 mm. This study clarifies the in-depth relationship between electron migration polarization and EMW dissipation, providing profound insights into developing well-coordinated magnetic-dielectric nanocomposites for EMW absorption engineering.

9.
Small ; 20(26): e2309806, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38243852

RESUMEN

The impedance matching and high loss capabilities of composites with homogeneous distribution are limited owing to high addition and lack of structural design. Developing composites with heterogeneous distribution can achieve strong and wide electromagnetic (EM) wave absorption. However, challenges such as complex design and unclear absorption mechanisms still exist. Herein, a novel composite with a heterogeneous distribution gradient is successfully constructed via MOF derivatives Co@ nitrogen-doped carbon (Co@NC) anchored on carbon foam (CF) matrix (MDCF). Notably, the concentration of MOF can easily control the gradient structure. In particular, the morphologies of MOF derivatives on the surface of CF undergo a transition from the collapse of the inner layer to the integrity of the outer layer, accompanied by a continuous reduction in the size of Co nanoparticles. Correspondingly, enhanced interface polarization from the core-shell of Co@NC and good impedance matching of MDCF can be obtained. The optimized MDCF exhibits the minimum reflection loss of -68.18 dB at 2.01 mm and effective absorption bandwidth covering the entire X-band. Moreover, MDCF exhibits lightweight characteristics, excellent compressive strength, and low radar cross-section reduction. This work highlights the immense potential of composites with heterogeneous distribution for achieving high-performance EM wave absorption.

10.
Adv Mater ; 36(19): e2311411, 2024 May.
Artículo en Inglés | MEDLINE | ID: mdl-38288859

RESUMEN

Heterointerface engineering, which plays a pivotal role in developing advanced microwave-absorbing materials, is employed to design zeolitic imidazolate framework (ZIF)-MXene nanocomposites. The ZIF-MXene composites are prepared by electrostatic self-assembly of negatively charged titanium carbide MXene flakes and positively charged Co-containing ZIF nanomaterials. This approach effectively creates abundant Mott-Schottky heterointerfaces exhibiting a robust built-in electric field (BIEF) effect, as evidenced by experimental and theoretical analyses, leading to a notable attenuation of electromagnetic energy. Systematic manipulation of the BIEF-exhibiting heterointerface, achieved through topological modulation of the ZIF, proficiently alters charge separation, facilitates electron migration, and ultimately enhances polarization relaxation loss, resulting in exceptional electromagnetic wave absorption performance (reflection loss RLmin = -47.35 dB and effective absorption bandwidth fE = 6.32 GHz). The present study demonstrates an innovative model system for elucidating the interfacial polarization mechanisms and pioneers a novel approach to developing functional materials with electromagnetic characteristics through spatial charge engineering.

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