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1.
Biomaterials ; 313: 122761, 2025 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-39241550

RESUMO

Biofilm-associated infections (BAIs) continue to pose a major challenge in the medical field. Nanomedicine, in particular, promises significant advances in combating BAIs through the introduction of a variety of nanomaterials and nano-antimicrobial strategies. However, studies to date have primarily focused on the removal of the bacterial biofilm and neglect the subsequent post-biofilm therapeutic measures for BAIs, rendering pure anti-biofilm strategies insufficient for the holistic recovery of affected patients. Herein, we construct an emerging dual-functional composite nanosheet (SiHx@Ga) that responds to pHs fluctuation in the biofilm microenvironment to enable a sequential therapy of BAIs. In the acidic environment of biofilm, SiHx@Ga employs the self-sensitized photothermal Trojan horse strategy to effectively impair the reactive oxygen species (ROS) defense system while triggering oxidative stress and lipid peroxidation of bacteria, engendering potent antibacterial and anti-biofilm effects. Surprisingly, in the post-treatment phase, SiHx@Ga adsorbs free pathogenic nucleic acids released after biofilm destruction, generates hydrogen with ROS-scavenging and promotes macrophage polarization to the M2 type, effectively mitigating damaging inflammatory burst and promoting tissue healing. This well-orchestrated strategy provides a sequential therapy of BAIs by utilizing microenvironmental variations, offering a conceptual paradigm shift in the field of nanomedicine anti-infectives.


Assuntos
Antibacterianos , Biofilmes , Gálio , Espécies Reativas de Oxigênio , Biofilmes/efeitos dos fármacos , Animais , Antibacterianos/farmacologia , Antibacterianos/uso terapêutico , Espécies Reativas de Oxigênio/metabolismo , Gálio/química , Gálio/farmacologia , Camundongos , Portadores de Fármacos/química , Células RAW 264.7 , Humanos , Staphylococcus aureus/efeitos dos fármacos , Staphylococcus aureus/fisiologia
2.
ACS Nano ; 18(39): 26911-26919, 2024 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-39350686

RESUMO

Two-dimensional van der Waals semiconductors are promising for future nanoelectronics. However, integrating high-k gate dielectrics for device applications is challenging as the inert van der Waals material surfaces hinder uniform dielectric growth. Here, we report a liquid metal oxide-assisted approach to integrate ultrathin, high-k HfO2 dielectric on 2D semiconductors with atomically smooth interfaces. Using this approach, we fabricated 2D WS2 top-gated transistors with subthreshold swings down to 74.5 mV/dec, gate leakage current density below 10-6 A/cm2, and negligible hysteresis. We further demonstrate a one-step van der Waals integration of contacts and dielectrics on graphene. This can offer a scalable approach toward integrating entire prefabricated device stack arrays with 2D materials. Our work provides a scalable solution to address the crucial dielectric engineering challenge for 2D semiconductor-based electronics.

3.
Nano Lett ; 24(40): 12353-12360, 2024 Oct 09.
Artigo em Inglês | MEDLINE | ID: mdl-39351895

RESUMO

The experimental demonstration of a p-type 2D WSe2 transistor with a ferroelectric perovskite BaTiO3 gate oxide is presented. The 30 nm thick BaTiO3 gate stack shows a robust ferroelectric hysteresis with a remanent polarization of 20 µC/cm2 and further enables a capacitance equivalent thickness of 0.5 nm in the hybrid WSe2/BaTiO3 stack due to its high dielectric constant of 323. We demonstrate one of the best ON currents for perovskite gate 2D transistors in the literature. This is enabled by high-quality epitaxial growth of BaTiO3 and a single 2D layer transfer based fabrication method that is shown to be amenable to silicon platforms. This demonstration is an important milestone toward the integration of crystalline complex oxides with 2D channel materials for scaled CMOS and low-voltage ferroelectric logic applications.

4.
Artigo em Inglês | MEDLINE | ID: mdl-39453717

RESUMO

Tungsten diselenide (WSe2) field-effect transistors (FETs) are promising for emerging electronics because of their tunable polarity, enabling complementary transistor technology, and their suitability for flexible electronics through material transfer. In this work, we demonstrate flexible p-type WSe2 FETs with absolute drain currents |ID| up to 7 µA/µm. We achieve this by fabricating flexible top-gated FETs with a combined WSe2 and metal contact transfer approach using WSe2 grown by metal-organic chemical vapor deposition on sapphire. Despite moderate WSe2 crystal grain size, our devices show similar or higher |ID| and ID on/off ratio (∼105) compared to most devices with exfoliated single-crystal WSe2 from the literature. We analyze charge trapping in our devices using pulsed and bias stress measurements. Notably, the high |ID| values are preserved during pulsing, where charge trapping is minimized. Overall, we demonstrate a fabrication approach advantageous for high drain currents in flexible 2D transistors.

5.
Artigo em Inglês | MEDLINE | ID: mdl-39353172

RESUMO

Graphene oxide (GO) is a promising material widely utilized in advanced materials engineering, such as in the development of soft robotics, sensors, and flexible devices. Considering that GOs are often processed using solution-based methods, a comprehensive understanding of the fundamental characteristics of GO in dispersion states becomes crucial given their significant influence on the ultimate properties of the device. GOs inherently exhibit polydispersity in solution, which plays a critical role in determining the mechanical behavior and flowability. However, research in the domain of 2D colloids concerning the effects of GO's polydispersity on its rheological properties and microstructure is relatively scant. Consequently, gaining a comprehensive understanding of how GO's polydispersity affects these critical aspects remains a pressing concern. In this study, we aim to investigate the dispersions and structure of GOs and clarify the effect of polydispersity on the rheological properties and yielding behavior. Using a rheometer, polarized optical microscopy, and small-angle X-ray scattering, we found that higher polydispersity in the same average size leads to overall improved rheological properties and higher flowability during yielding. Thus, our study can be beneficial in the employment of polydispersity in the processing of GO such as 3D printing and fiber spinning.

6.
Nano Lett ; 2024 Oct 18.
Artigo em Inglês | MEDLINE | ID: mdl-39423349

RESUMO

Demystifying the molecular mechanism of growth is vital for the rational design, synthesis, and optimization of functional nanomaterials. Despite the promising perspectives and extensive efforts, the growth mechanism of atomically thin TiO2(B) nanosheets remains unclear, hence it is difficult to tune their band and surface structures. Herein, we report an oriented attachment-based crystallization mechanism of TiO2(B) nanosheets from a 1D titanium glycolate coordination polymer through hydrolysis and condensation. With time-tracking experiments, this 1D coordination polymer is found to be an intermediate in the synthesis of TiO2(B) nanosheets by using Ti alkoxides and chlorides as precursors, suggesting the universality of the 1D-to-2D growth mechanism. Such a side-to-side attachment pathway bridges the classical and nonclassical interpretations of crystallization, and meanwhile hints at the possibility of other 1D complexes as potential precursors for 2D materials.

7.
Nanotechnology ; 2024 Oct 22.
Artigo em Inglês | MEDLINE | ID: mdl-39436393

RESUMO

Two-dimensional (2D) materials are widely studied due to their unique physical, optical, electrical properties and good compatibility with various synthesis methods. Tin disulfide (SnS2) has high uniformity and conformality even at low process temperatures and is a two-dimensional material with accurate thickness control using atomic layer deposition (ALD). However, since the crystallinity of thin film is low at a low process temperature, various post-annealing methods are being studied to compensate for film quality. In this work, we compared the crystal structures, chemical binding energies, and electrical properties of post-annealed SnS2 thin films at hydrogen sulfide concentrations of 4.00 % and 99.99 %. The crystallinity, grain size, and carrier concentrations of the SnS2 thin film were highest at a post-annealing temperature of 350 ℃ and a hydrogen sulfide concentration of 99.99 %, and the chemical binding energies corresponded with the standard Sn4+ states, forming a pure 2D-hexagonal SnS2 phase. In addition, SnS2 thin films deposited via ALD showed high uniformity and conformality in large-scale wafers and trench structure wafers.

8.
Small ; : e2405870, 2024 Oct 13.
Artigo em Inglês | MEDLINE | ID: mdl-39396387

RESUMO

2D transition metal borides (MBenes) have garnered significant attention from researchers due to their exceptional electrical conductivity, strong mechanical rigidity, excellent dynamic and thermodynamic stability, which stimulates the enthusiasm of researchers for the study of MBenes. Over the past few years, extensive research efforts have been dedicated to the study of MBenes, resulting in a growing number of synthesis methods being developed. However, there remains a scarcity of comprehensive reviews on MBenes, particularly in relation to the synthesis techniques employed. To address this gap, this review aims to provide a comprehensive summary of the latest research findings on MBenes. An exhaustive exploration of the crystal structure types of MBenes is presented, highlighting the greater structural diversity compared to MXenes. Furthermore, a comprehensive review of the recent advancements in MBenes synthesis methodologies is provided. The review also delves into the physical and chemical properties of MBenes, while elucidating their applications in the realms of energy conversion and energy storage. Lastly, this review concludes by summarizing and offering insights on MBenes from three angles: synthesis, structure-property relationships, and application prospects.

9.
Materials (Basel) ; 17(19)2024 Sep 29.
Artigo em Inglês | MEDLINE | ID: mdl-39410376

RESUMO

Hydrogen boride (HB) sheets are emerging as a promising two-dimensional (2D) boron material, with potential applications as unique electrodes, substrates, and hydrogen storage materials. The 2D layered structure of HB was successfully synthesized using an ion-exchange method. The chemical bonding and structure of the HB sheets were investigated using Fourier Transform Infrared (FT-IR) spectroscopy and Transmission Electron Microscopy (TEM), respectively. X-ray photoelectron spectroscopy (XPS) was employed to study the chemical states and transformation of the components before and after atomic hydrogen adsorption, thereby elucidating the atomic hydrogen adsorption process on HB sheets. Our results indicate that, upon atomic hydrogen adsorption onto the HB sheets, the B-H-B bonds were broken and converted into B-H bonds. This research highlights and demonstrates the changes in chemical states and component transformations of the boron element on the HB sheets' surface before and after atomic hydrogen adsorption, thus providing a clearer understanding of the unique bonding and structural characteristics of the HB sheets.

10.
Heliyon ; 10(17): e37008, 2024 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-39281565

RESUMO

Material design is essential for the development and preparation of new materials. In this paper, a new two-dimensional heterostructure material (B@Si) consisting of boronene and silicene is designed and used as an anode material for lithium-ion batteries in order to improve the performance of lithium-ion batteries, and the structural properties, stability, electronic properties, and performance as an anode material for lithium-ion batteries are systematically investigated by first-principle calculations of the B@Si heterostructure. The results show that the B@Si heterostructure is energetically, thermodynamically and dynamically stable, and although the Dirac cone in the energy band structure of silicene disappears after the formation of the heterojunction, the overall electrical conductivity of the material improves considerably and the electron transport rate is faster. Due to the synergistic effect, Li has more stable adsorption sites and lower diffusion barriers than boronene and silicene in the B@Si heterostructure, higher theoretical specific capacity (1208 mAhg-1), and stronger mechanical properties (C11 = 296.6 N/m, C22 = 142.8 N/m). The volume expansion in the fully lithiated state is also only 8 %. These advantages indicate that B@Si heterostructures are good potential anode materials for high-performance Li-ion batteries.

11.
Angew Chem Int Ed Engl ; : e202413932, 2024 Sep 20.
Artigo em Inglês | MEDLINE | ID: mdl-39304931

RESUMO

Phase engineering is a critical strategy in electrocatalysis, as it allows for the modulation of electronic, geometric, and chemical properties to directly influence the catalytic performance. Despite its potential, phase engineering remains particularly challenging in thermodynamically stable perovskites, especially in a 2D structure constraint. Herein, we report phase engineering in 2D LaNiO3 perovskite using the strongly non-equilibrium microwave shock method. This approach enables the synthesis of conventional hexagonal and unconventional trigonal and cubic phases in LaNiO3 by inducing selective phase transitions at designed temperatures, followed by rapid quenching to allow precise phase control while preserving the 2D porous structure. These phase transitions induce structural distortions in the [LaO]+ layers and the hybridization between Ni 3d and O 2p states, thus modifying local charge distribution and enhancing electron transport during the six-electron urea oxidation reaction (UOR). The cubic LaNiO3 offers optimal electron transport and active site accessibility due to its high structural symmetry and open interlayer spacing, resulting in a low onset potential of 1.27 V and a Tafel slope of 33.1 mV dec-1 for UOR, outperforming most current catalysts. Our strategy features high designability in phase engineering, enabling various electrocatalysts to harness the power of unconventional phases.

12.
Discov Nano ; 19(1): 151, 2024 Sep 17.
Artigo em Inglês | MEDLINE | ID: mdl-39289310

RESUMO

With the size of the aging population increasing worldwide, the effective diagnosis and treatment of neurodegenerative diseases (NDDs) has become more important. Two-dimensional (2D) materials offer specific advantages for the diagnosis and treatment of NDDs due to their high sensitivity, selectivity, stability, and biocompatibility, as well as their excellent physical and chemical characteristics. As such, 2D materials offer a promising avenue for the development of highly sensitive, selective, and biocompatible theragnostics. This review provides an interdisciplinary overview of advanced 2D materials and their use in biosensors, drug delivery, and tissue engineering/regenerative medicine for the diagnosis and/or treatment of NDDs. The development of 2D material-based biosensors has enabled the early detection and monitoring of NDDs via the precise detection of biomarkers or biological changes, while 2D material-based drug delivery systems offer the targeted and controlled release of therapeutics to the brain, crossing the blood-brain barrier and enhancing treatment effectiveness. In addition, when used in tissue engineering and regenerative medicine, 2D materials facilitate cell growth, differentiation, and tissue regeneration to restore neuronal functions and repair damaged neural networks. Overall, 2D materials show great promise for use in the advanced treatment of NDDs, thus improving the quality of life for patients in an aging population.

13.
Small Methods ; : e2400955, 2024 Sep 20.
Artigo em Inglês | MEDLINE | ID: mdl-39300866

RESUMO

Extrinsic dilute magnetic semiconductors achieve magnetic functionality through tailored interaction between a semiconducting matrix and a non-magnetic dopant. The absence of intrinsic magnetic impurities makes this approach promising to investigate the newly emerging field of 2D dilute magnetic semiconductors. Here the first realization of an extrinsic 2D DMS in Pt-doped WS2 is demonstrated. A bottom-up synthesis approach yields a uniform and highly crystalline monolayer where platinum selectively occupies the tungsten sub-lattice. The orbital overlap between W 4d and Pt 5d results in spin-selective hybrid states that produce a strong valley-Zeeman splitting. Combined experimental and theoretical results show that this interaction yields a sizable ferromagnetic response with a Curie temperature ≈375 K. These results open up a new route toward 2D magnetic properties through tailoring of atomic interactions for future applications in spintronics and magnetic nanoactuation.

14.
Small ; : e2404986, 2024 Sep 23.
Artigo em Inglês | MEDLINE | ID: mdl-39308318

RESUMO

Hydrogen boride (HB) sheet is a new class of 2D materials comprising hydrogen and boron, synthesized through ion-exchange and exfoliation techniques. HB sheets can release hydrogen (H2) under light irradiation and is predicted to be a promising H2 storage material. However, its application is limited to the UV region. One approach to enable a visible-light-driven system is the utilization of plasmonic metallic nanoparticles. The present study reports H2 release from copper (Cu) nanoparticle-modified HB sheet (HB/Cu) under visible-light irradiation. Copper nanoparticles possess unique and strong plasmonic responses in the visible-light range, making them ideal light absorbers in this system. HB/Cu nanocomposites are synthesized using a simple mixture of copper acetate and HB sheets in acetonitrile, where HB sheets reduced copper ions to metal copper nanoparticles. The photoirradiation results shows that HB/Cu nanocomposites released more H2 than the bare HB sheets under visible-light irradiation. This is probably due to the plasmonic photothermal effect of copper metal, which enhances H2 generation from the HB sheets. This material offers a viable and cost-effective approach for developing visible-light-sensitive systems.

15.
Angew Chem Int Ed Engl ; : e202412425, 2024 Sep 18.
Artigo em Inglês | MEDLINE | ID: mdl-39292963

RESUMO

Ferromagnetic metal Fe3GeTe2 (FGT), whose structure exhibits weak van-der-Waals interactions between 5-atom thick layers, was subjected to liquid-phase exfoliation (LPE) in N-methyl pyrrolidone (NMP) to yield a suspension of nanosheets that were separated into several fractions by successive centrifugation at different speeds. Electron microscopy confirmed successful exfoliation of bulk FGT to nanosheets as thin as 6 nm. The ferromagnetic ordering temperature for the nanosheets gradually decreased with the increase in the centrifugation speed used to isolate the 2D material. These nanosheets were resuspended in NMP and treated with an organic acceptor, 7,7,8,8-tetracyano-quinodimethane (TCNQ), which led to precipitation of FGT-TCNQ composite. The formation of the composite material is accompanied by charge transfer from the FGT nanosheets to TCNQ molecules, generating TCNQ•- radical anions, as revealed by experimental vibrational spectra and supported by first principles calculations. Remarkably, a substantial increase in magnetic anisotropy was observed, as manifested by the increase in the coercive field from nearly zero in bulk FGT to 1.0 kOe in the exfoliated nanosheets and then to 5.4 kOe in the FGT-TCNQ composite. The dramatic increase in coercivity of the composite suggests that functionalization with redox-active molecules provides an appealing pathway to enhancing magnetic properties of 2D materials.

16.
J Phys Condens Matter ; 36(48)2024 Sep 05.
Artigo em Inglês | MEDLINE | ID: mdl-39191291

RESUMO

Through the accurate calculation of density functional theory, reveal the excellent photoelectric properties of the AlN/WSSe and WSSe/AlN heterojunction. Especially, the hole mobility of the AlN/WSSe heterojunction is as high as 3919 cm2Vs-1in armchair direction, and the hole mobility of the WSSe/AlN heterojunction is as high as 4422 cm2Vs-1in the zigzag direction. Interestingly, when two H atoms are adsorbed in the WSSe surface, the Gibbs free energy change are -0.093 eV and -0.984 eV, which tends to zero, which can promote the spontaneous reaction of electrocatalytic water decomposition to produce H2. In addition, the AlN/WSSe heterojunction exhibits significant photoelectric effect photocurrent (1.15 a02/photon) in the armchair direction and the heterojunctions have lower threshold voltage (1.5 V), that indicate the AlN/WSSe and WSSe/AlN heterojunction have great application prospect in manufacturing high-performance optoelectronic devices with fast response and low power consumption.

17.
ACS Appl Mater Interfaces ; 16(34): 45422-45432, 2024 Aug 28.
Artigo em Inglês | MEDLINE | ID: mdl-39102678

RESUMO

Implantable polymeric biodegradable devices, such as biodegradable vascular scaffolds, cannot be fully visualized using standard X-ray-based techniques, compromising their performance due to malposition after deployment. To address this challenge, we describe a new radiopaque and photocurable liquid polymer-ceramic composite (mPDC-MoS2) consisting of methacrylated poly(1,12 dodecamethylene citrate) (mPDC) and molybdenum disulfide (MoS2) nanosheets. The composite was used as an ink with microcontinuous liquid interface production (µCLIP) to fabricate bioresorbable vascular scaffolds (BVS). Prints exhibited excellent crimping and expansion mechanics without strut failures and, importantly, with X-ray visibility in air and muscle tissue. Notably, MoS2 nanosheets displayed physical degradation over time in phosphate-buffered saline solution, suggesting the potential for producing radiopaque, fully bioresorbable devices. mPDC-MoS2 is a promising bioresorbable X-ray-visible composite material suitable for 3D printing medical devices, such as vascular scaffolds, that require noninvasive X-ray-based monitoring techniques for implantation and evaluation. This innovative biomaterial composite system holds significant promise for the development of biocompatible, fluoroscopically visible medical implants, potentially enhancing patient outcomes and reducing medical complications.


Assuntos
Citratos , Dissulfetos , Procedimentos Endovasculares , Molibdênio , Nanoestruturas , Alicerces Teciduais , Molibdênio/química , Molibdênio/metabolismo , Dissulfetos/química , Dissulfetos/metabolismo , Impressão Tridimensional , Citratos/química , Nanoestruturas/química , Materiais Biocompatíveis/química , Materiais Biocompatíveis/metabolismo , Polímeros/química
18.
Chemosphere ; 364: 143194, 2024 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-39209044

RESUMO

MXenes are a group of 2D material which have been derived from the layered transition metal nitrides and carbides and have the characteristics like electrical conductivity, high surface area and variable surface chemical composition. Self-assembly of clusters/metal ions and organic linkers forms metal organic framework (MOF). Their advantages of ultrahigh porosity, highly exposed active sites and many pore architectures have garnered them a lot of attention. But poor conductivity and instability plague several conventional MOF. To address the issue, MOF can be linked with MXenes that have rich surface functional groups and excellent electrical conductivity. In this review, different etching methods for exfoliation of MXene along with the synthesis methods of MXene/MOF composites are reviewed, including hydrothermal method, solvothermal method, in-situ growth method, and self-assembly method. Moreover, application of these MXene/MOF composites for catalytic water splitting and wastewater treatment were also discussed in details. In addition to increasing a single MOF conductivity and stability, MXenes can add a variety of new features, such the template effect. Due to these benefits, MXene/MOF composites can be effectively used in several applications, including photocatalytic/electrocatalytic water splitting, adsorption and degradation of pollutants from wastewater. Finally, the authors explored the current challenges and the future opportunities to improve the efficiency of MXene/MOF composites.


Assuntos
Estruturas Metalorgânicas , Águas Residuárias , Purificação da Água , Estruturas Metalorgânicas/química , Águas Residuárias/química , Catálise , Purificação da Água/métodos , Água/química , Adsorção , Poluentes Químicos da Água/química , Eliminação de Resíduos Líquidos/métodos
19.
Nanotechnology ; 35(48)2024 Sep 10.
Artigo em Inglês | MEDLINE | ID: mdl-39208809

RESUMO

The distinctive multi-ring structure and remarkable electrical characteristics of biphenylene render it a material of considerable interest, notably for its prospective utilization as an anode material in lithium-ion batteries. However, understanding the mechanical traits of biphenylene is essential for its application, particularly due to the volumetric fluctuations resulting from lithium ion insertion and extraction during charging and discharging cycles. In this regard, this study investigates the performance of pristine biphenylene and materials embedded with various types of hole defects under uniaxial tension utilizing molecular dynamics simulations. Specifically, from the stress‒strain curves, we obtained key mechanical properties, including toughness, strength, Young's modulus and fracture strain. It was observed that various near-circular hole (including circular, square, hexagonal, and octagonal) defects result in remarkably similar properties. A more quantitative scaling analysis revealed that, in comparison with the exact shape of the defect, the area of the defect is more critical for determining the mechanical properties of biphenylene. Our finding might be beneficial to the defect engineering of two-dimensional materials.

20.
Nano Lett ; 24(35): 10892-10898, 2024 Sep 04.
Artigo em Inglês | MEDLINE | ID: mdl-39167086

RESUMO

While experimental realization of multiple charge-density waves (CDWs) has been ascribed to monolayer 1T-NbTe2, their atomic structures are still largely unclear, preventing a deep understanding of their novel electronic structures. Here, comparing first-principles-calculated orbital textures with reported STM measurements, we successfully identify multiple CDWs in monolayer NbTe2. Surprisingly, we reveal that both 1T/1H phases could exist in monolayer NbTe2, which was incognizant before. Particularly, we find that the experimentally observed 4 × 1 and 4 × 4 CDWs could be attributed to 1H stacking, while the observed 19×19 phase could possess 1T stacking. The existence of 1T/1H phases results in competition between CDW, spin-density wave (SDW), and ferromagnetism in 1H stacking under an external field and results in CDW-induced quantum phase transitions from a Kramers-Weyl fermion to a topological insulator in 1T stacking. Our study suggests NbTe2 as an exotic platform to investigate the interplay between CDW, SDW, and topological phases, which are largely unexplored in current experiments.

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