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1.
Small ; : e2402078, 2024 May 02.
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.

2.
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.

3.
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.

4.
Small Methods ; : e2301600, 2024 Jan 07.
Artículo en Inglés | MEDLINE | ID: mdl-38185797

RESUMEN

Over the past century, extensive research has been carried out on various types of microwave absorption (MA) materials, primarily emphasizing mechanism, performance, and even toward smart device. However, the deactivation, a crucial concern for practical applications, has long been long-neglected. In this work, an in-depth exploration of the deactivation mechanism reveals a significant competition between metal and oxygen, leading to the replacement of the S-M (M = Ni and Co) bond by a new S─O bond on the surface of absorber. This substitution initiates a series of collapse effect that introduces additional defective sites and diminishes the potential for charge transport. Subsequently, passive and active anti-deactivation strategies are developed to target the deactivation. The passive strategy involved intentionally creating electron-deficient structures at the initial Ni and Co sites in the crystal through the Fe doping engineering, with the objective of preventing the generation of S─O bonds. Furthermore, the active anti-deactivation strategy allows for the precise control of absorber deactivation and reactivation by employing accelerated thermodynamic and kinetic methods, enabling a reversible transformation of S-M through competitive reactions with S─O bonds. Finally, a fast deactivation and reactivation method is first proposed promising to stimulate further innovations and breakthroughs in practical applications.

5.
Adv Sci (Weinh) ; 11(6): e2307649, 2024 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-38044282

RESUMEN

The extremely weak heterointerface construction of high-entropy materials (HEM) hinders them being the electromagnetic wave (EMW) absorbers with ideal properties. To address this issue, this study proposes multiphase interfacial engineering and results in a multiphase-induced interfacial polarization loss in multielement sulfides. Through the selection of atoms with diverse reaction activities, the multiphase interfacial components of CuS (1 0 5), Fe0.5 Ni0.5 S2 (2 1 0), and CuFe2 S3 (2 0 0) are constructed to enhance the interfacial polarization loss in multielement Cu-based sulfides. Compared with single-phase high-entropy Zn-based sulfides (ZnFeCoNiCr-S), the multiphase Cu-based sulfides (CuFeCoNiCr-S) possess optimized EMW absorption properties (effective absorption bandwidth (EAB) of 6.70 GHz at 2.00 mm) due to the existence of specific interface of CuS (1 0 5)/CuFe2 S3 (2 0 0) with proper EM parameters. Furthermore, single-phase ZnFeCoNiCr-S into FeNi2 S4 (3 1 1)/(Zn, Fe)S (1 1 1) heterointerface through 400 °C heat-treated is decomposed. The EMW absorption properties are enhanced by strong interfacial polarization (EAB of 4.83 GHz at 1.45 mm). This work reveals the reasons for the limited EMW absorption properties of high-entropy sulfides and proposes multiphase interface engineering to improve charge accumulation and polarization between specific interfaces, leading to the enhanced EMW absorption properties.

6.
J Colloid Interface Sci ; 629(Pt B): 147-155, 2023 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-36152572

RESUMEN

Vacancy engineering has been shown to be an effective way to tune the electromagnetic parameters of electromagnetic wave (EMW) absorbers and improve their absorption properties. However, the current methods to induce the formation of sulfur vacancies are not enough, and the contribution of sulfur vacancies to EMW absorption has not been clearly described. This work proposes a method to induce sulfur vacancies generation in the Cu2ZnSnS4 (CZTS) system by cation doping. It is found that the formation of sulfur vacancies depends on reactivity with doping cations and the less reactive cation is more favorable for the formation of sulfur vacancies. Benefiting from the improved sulfur vacancies concentration, the defect-induced polarization and dipole polarization are greatly enhanced, which allows the EMW absorber to exhibit excellent EMW absorption performance. Therefore, the minimum reflection loss of the cation-doped CZTS reaches -61.80 dB at a thickness of 2.00 mm, and the effective absorption bandwidth reaches 6.29 GHz at 2.30 mm. This work not only expounds on the significant roles of sulfur vacancies in EMW absorption mechanism, but also presents a novel idea for defect construction of copper-based chalcogenide semiconductor materials.

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