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1.
ACS Sens ; 9(4): 1809-1819, 2024 Apr 26.
Artículo en Inglés | MEDLINE | ID: mdl-38587867

RESUMEN

While most of the research in graphene-based materials seeks high electroactive surface area and ion intercalation, here, we show an alternative electrochemical behavior that leverages graphene's potential in biosensing. We report a novel approach to fabricate graphene/polymer nanocomposites with near-record conductivity levels of 45 Ω sq-1 and enhanced biocompatibility. This is realized by laser processing of graphene oxide in a sandwich structure with a thin (100 µm) polyethylene terephthalate film on a textile substrate. Such hybrid materials exhibit high conductivity, low polarization, and stability. In addition, the nanocomposites are highly biocompatible, as evidenced by their low cytotoxicity and good skin adhesion. These results demonstrate the potential of graphene/polymer nanocomposites for smart clothing applications.


Asunto(s)
Grafito , Rayos Láser , Textiles , Grafito/química , Humanos , Técnicas Electroquímicas/métodos , Nanocompuestos/química , Conductividad Eléctrica , Tereftalatos Polietilenos/química , Animales , Materiales Biocompatibles/química , Técnicas Biosensibles/métodos
2.
Nanomaterials (Basel) ; 14(5)2024 Mar 06.
Artículo en Inglés | MEDLINE | ID: mdl-38470809

RESUMEN

Tungsten diselenide (WSe2) has emerged as a promising ambipolar semiconductor material for field-effect transistors (FETs) due to its unique electronic properties, including a sizeable band gap, high carrier mobility, and remarkable on-off ratio. However, engineering the contacts to WSe2 remains an issue, and high contact barriers prevent the utilization of the full performance in electronic applications. Furthermore, it could be possible to tune the contacts to WSe2 for effective electron or hole injection and consequently pin the threshold voltage to either conduction or valence band. This would be the way to achieve complementary metal-oxide-semiconductor devices without doping of the channel material.This study investigates the behaviour of two-dimensional WSe2 field-effect transistors with multi-layer palladium diselenide (PdSe2) as a contact material. We demonstrate that PdSe2 contacts favour hole injection while preserving the ambipolar nature of the channel material. This consequently yields high-performance p-type WSe2 devices with PdSe2 van der Waals contacts. Further, we explore the tunability of the contact interface by selective laser alteration of the WSe2 under the contacts, enabling pinning of the threshold voltage to the valence band of WSe2, yielding pure p-type operation of the devices.

3.
Polymers (Basel) ; 15(24)2023 Dec 05.
Artículo en Inglés | MEDLINE | ID: mdl-38139874

RESUMEN

Flexible electronics have sparked significant interest in the development of electrically conductive polymer-based composite materials. While efforts are being made to fabricate these composites through laser integration techniques, a versatile methodology applicable to a broad range of thermoplastic polymers remains elusive. Moreover, the underlying mechanisms driving the formation of such composites are not thoroughly understood. Addressing this knowledge gap, our research focuses on the core processes determining the integration of reduced graphene oxide (rGO) with polymers to engineer coatings that are not only flexible and robust but also exhibit electrical conductivity. Notably, we have identified a particular range of laser power densities (between 0.8 and 1.83 kW/cm2), which enables obtaining graphene polymer composite coatings for a large set of thermoplastic polymers. These laser parameters are primarily defined by the thermal properties of the polymers as confirmed by thermal analysis as well as numerical simulations. Scanning electron microscopy with elemental analysis and X-ray photoelectron spectroscopy showed that conductivity can be achieved by two mechanisms-rGO integration and polymer carbonization. Additionally, high-speed videos allowed us to capture the graphene oxide (GO) modification and melt pool formation during laser processing. The cross-sectional analysis of the laser-processed samples showed that the convective flows are present in the polymer substrate explaining the observed behavior. Moreover, the practical application of our research is exemplified through the successful assembly of a conductive wristband for wearable devices. Our study not only fills a critical knowledge gap but also offers a tangible illustration of the potential impact of laser-induced rGO-polymer integration in materials science and engineering applications.

4.
Inorg Chem ; 62(48): 19677-19689, 2023 Dec 04.
Artículo en Inglés | MEDLINE | ID: mdl-37977192

RESUMEN

We report the synthesis and comprehensive characterization of organic-inorganic hybrid salts formed by bis-cationic N,N'-bis(2-(trimethylammonium)ethylene)perylene-3,4,9,10-tetracarboxylic acid bisimide (PTCD2+) and Keggin-type [XW12O40]n- (X = Si, n = 4; X = P, n = 3) polyoxometalates. (PTCD)3[PW12O40]2·3DMSO·2H2O (2) and (PTCD)2[SiW12O40]·DMSO·2H2O (3) were structurally characterized by single crystal X-ray diffraction. The cations in both structures exhibited infinite chainlike arrangements through π-π interactions, contrasting with the previously reported cation-anion stacking observed in naphthalene diimide derivatives. A detailed theoretical study employing topological analysis of the electron density distribution within the quantum theory of atoms in molecules approach provided further insights into this structural dualism. Atomic force microscopy analyses revealed the formation of self-assembled supramolecular structures on graphite from molecular monolayers (3 nm of thick) to submicrometer aggregates for 2. Hyperspectral Raman spectroscopy imaging revealed that such heterostructures are likely formed by an enhanced π-π interactions. Both complexes demonstrated interesting electrochemical behavior, photoluminescence and X-ray-induced luminescence. Electron spin resonance analysis confirmed charge separation in both compounds, with enhanced efficiency observed in compound 2. Our findings of these perylene-based organic-inorganic hybrid salts offer the potential for their application in optoelectronic devices and functional materials.

5.
Mater Today Bio ; 22: 100784, 2023 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-37731959

RESUMEN

Smart implants are increasingly used to treat various diseases, track patient status, and restore tissue and organ function. These devices support internal organs, actively stimulate nerves, and monitor essential functions. With continuous monitoring or stimulation, patient observation quality and subsequent treatment can be improved. Additionally, using biodegradable and entirely excreted implant materials eliminates the need for surgical removal, providing a patient-friendly solution. In this review, we classify smart implants and discuss the latest prototypes, materials, and technologies employed in their creation. Our focus lies in exploring medical devices beyond replacing an organ or tissue and incorporating new functionality through sensors and electronic circuits. We also examine the advantages, opportunities, and challenges of creating implantable devices that preserve all critical functions. By presenting an in-depth overview of the current state-of-the-art smart implants, we shed light on persistent issues and limitations while discussing potential avenues for future advancements in materials used for these devices.

6.
Commun Chem ; 6(1): 166, 2023 Aug 14.
Artículo en Inglés | MEDLINE | ID: mdl-37580376

RESUMEN

Metallic nanoparticles are widely explored for boosting light-matter coupling, optoelectronic response, and improving photocatalytic performance of two-dimensional (2D) materials. However, the target area is restricted to either top or bottom of the 2D flakes. Here, we introduce an approach for edge-specific nanoparticle decoration via light-assisted reduction of silver ions and merging of silver seeds. We observe arrays of the self-limited in size silver nanoparticles along tungsten diselenide WSe2 nanoribbon edges. The density of nanoparticles is tunable by adjusting the laser fluence. Scanning electron microscopy, atomic force microscopy, and Raman spectroscopy are used to investigate the size, distribution, and photo-response of the deposited plasmonic nanoparticles on the quasi-one-dimensional nanoribbons. We report an on-surface synthesis path for creating mixed-dimensional heterostructures and heterojunctions with potential applications in opto-electronics, plasmonics, and catalysis, offering improved light matter coupling, optoelectronics response, and photocatalytic performance of 2D materials.

7.
ACS Nano ; 17(17): 16501-16516, 2023 09 12.
Artículo en Inglés | MEDLINE | ID: mdl-37616178

RESUMEN

The healing of tendon injury is often hindered by peritendinous adhesion and poor regeneration caused by the accumulation of reactive oxygen species (ROS), development of inflammatory responses, and the deposition of type-III collagen. Herein, an extracellular vesicles (EVs)-cloaked enzymatic nanohybrid (ENEV) was constructed to serve as a multifaceted biocatalyst for ultrasound (US)-augmented tendon matrix reconstruction and immune microenvironment regulation. The ENEV-based biocatalyst exhibits integrated merits for treating tendon injury, including the efficient catalase-mimetic scavenging of ROS in the injured tissue, sustainable release of Zn2+ ions, cellular uptake augmented by US, and immunoregulation induced by EVs. Our study suggests that ENEVs can promote tenocyte proliferation and type-I collagen synthesis at an early stage by protecting tenocytes from ROS attack. The ENEVs also prompted efficient immune regulation, as the polarization of macrophages (Mφ) was reversed from M1φ to M2φ. In a rat Achilles tendon defect model, the ENEVs combined with US treatment significantly promoted functional recovery and matrix reconstruction, restored tendon morphology, suppressed intratendinous scarring, and inhibited peritendinous adhesion. Overall, this study offers an efficient nanomedicine for US-augmented tendon regeneration with improved healing outcomes and provides an alternative strategy to design multifaceted artificial biocatalysts for synergetic tissue regenerative therapies.


Asunto(s)
Vesículas Extracelulares , Traumatismos de los Tendones , Animales , Ratas , Especies Reactivas de Oxígeno , Colágeno Tipo I , Tendones
8.
ACS Appl Mater Interfaces ; 15(32): 38946-38955, 2023 Aug 16.
Artículo en Inglés | MEDLINE | ID: mdl-37466067

RESUMEN

The concept of wearables is rapidly evolving from flexible polymer-based devices to textile electronics. The reason for this shift is the ability of textiles to ensure close contact with the skin, resulting in comfortable, lightweight, and compact "always with you" sensors. We are contributing to this polymer-textile transition by introducing a novel and simple way of laser intermixing of graphene with synthetic fabrics to create wearable sensing platforms. Our hybrid materials exhibit high electrical conductivity (87.6 ± 36.2 Ω/sq) due to the laser reduction of graphene oxide and simultaneous laser-induced graphene formation on the surface of textiles. Furthermore, the composite created between graphene and nylon ensures the durability of our materials against sonication and washing with detergents. Both of these factors are essential for real-life applications, but what is especially useful is that our free-form composites could be used as-fabricated without encapsulation, which is typically required for conventional laser-scribed materials. We demonstrate the exceptional versatility of our new hybrid textiles by successfully recording muscle activity, heartbeat, and voice. We also show a gesture sensor and an electrothermal heater embedded within a single commercial glove. Additionally, the use of these textiles could be extended to personal protection equipment and smart clothes. We achieve this by implementing self-sterilization with light and laser-induced functionalization with silver nanoparticles, which results in multifunctional antibacterial textiles. Moreover, incorporating silver into such fabrics enables their use as surface-enhanced Raman spectroscopy sensors, allowing for the direct analysis of drugs and sweat components on the clothing itself. Our research offers valuable insights into simple and scalable processes of textile-based electronics, opening up new possibilities for paradigms like the Internet of Medical Things.

9.
Nanomaterials (Basel) ; 13(5)2023 Mar 02.
Artículo en Inglés | MEDLINE | ID: mdl-36903801

RESUMEN

Structural electronics, as well as flexible and wearable devices are applications that are possible by merging polymers with metal nanoparticles. However, using conventional technologies, it is challenging to fabricate plasmonic structures that remain flexible. We developed three-dimensional (3D) plasmonic nanostructures/polymer sensors via single-step laser processing and further functionalization with 4-nitrobenzenethiol (4-NBT) as a molecular probe. These sensors allow ultrasensitive detection with surface-enhanced Raman spectroscopy (SERS). We tracked the 4-NBT plasmonic enhancement and changes in its vibrational spectrum under the chemical environment perturbations. As a model system, we investigated the sensor's performance when exposed to prostate cancer cells' media over 7 days showing the possibility of identifying the cell death reflected in the environment through the effects on the 4-NBT probe. Thus, the fabricated sensor could have an impact on the monitoring of the cancer treatment process. Moreover, the laser-driven nanoparticles/polymer intermixing resulted in a free-form electrically conductive composite that withstands over 1000 bending cycles without losing electrical properties. Our results bridge the gap between plasmonic sensing with SERS and flexible electronics in a scalable, energy-efficient, inexpensive, and environmentally friendly way.

10.
ACS Nano ; 17(3): 2943-2957, 2023 02 14.
Artículo en Inglés | MEDLINE | ID: mdl-36688804

RESUMEN

The microenvironments with high reactive-oxygen-species (ROS) levels, inflammatory responses, and oxidative-stress effects in diabetic ulcer wounds, leading to poor proliferation and differentiation of stem cells, severely inhibit their efficient healing. Here, to overcome the unbalanced multielectron reactions in ROS catalysis, we develop a cobalt selenide-based biocatalyst with an amorphous Ru@CoSe nanolayer for ultrafast and broad-spectrum catalytic ROS-elimination. Owing to the enriched electrons and more unoccupied orbitals of Ru atoms, the amorphous Ru@CoSe nanolayer-equipped biocatalyst displays excellent catalase-like kinetics (maximal reaction velocity, 23.05 µM s-1; turnover number, 2.00 s-1), which exceeds most of the currently reported metal compounds. The theoretical studies show that Ru atoms act as "regulators" to tune the electronic state of the Co sites and modulate the interaction of oxygen intermediates, thus improving the reversible redox properties of active sites. Consequently, the Ru@CoSe can efficiently rescue the proliferation of mesenchymal stem cells and maintain their angiogenic potential in the oxidative stress environment. In vivo experiments reveal the superior ROS-elimination ability of Ru@CoSe on the inflammatory diabetic wound. This study offers an effective nanomedicine for catalytic ROS-scavenging and ultrafast healing of inflammatory wounds and also provides a strategy to design biocatalytic metal compounds via bringing amorphous catalytic structures.


Asunto(s)
Diabetes Mellitus , Cicatrización de Heridas , Humanos , Especies Reactivas de Oxígeno , Cicatrización de Heridas/fisiología , Estrés Oxidativo , Metales , Oxígeno
11.
Adv Mater ; 34(43): e2206877, 2022 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-36038983

RESUMEN

Glass electronics inspire the emergence of smart functional surfaces. To evolve this concept to the next level, developing new strategies for scalable, inexpensive, and electrically conductive glass-based robust nanocomposites is crucial. Graphene is an attractive material as a conductive filler; however, integrating it firmly into a glass with no energy-intensive sintering, melting, or harsh chemicals has not been possible until now. Moreover, these methods have very limited capability for fabricating robust patterns for electronic circuits. In this work, a conductive (160 OΩ sq-1 ) and resilient nanocomposite between glass and graphene is achieved via single-step laser-induced backward transfer (LIBT). Beyond conventional LIBT involving mass transfer, this approach simultaneously drives chemical transformations in glass including silicon compound formation and graphene oxide (GO) reduction. These processes take place together with the generation and transfer of the highest-quality laser-reduced GO (rGO) reported to date (Raman intensity ratio ID /IG  = 0.31) and its integration into the glass. The rGO-LIBT nanocomposite is further functionalized with silver to achieve a highly sensitive (10-9  m) dual-channel plasmonic optical and electrochemical sensor. Besides the electrical circuit demonstration, an electrothermal heater is fabricated that reaches temperatures above 300 °C and continuously operates for over 48 h.

12.
Crit Rev Anal Chem ; : 1-25, 2022 Apr 18.
Artículo en Inglés | MEDLINE | ID: mdl-35435777

RESUMEN

One of the lessons we learned from the COVID-19 pandemic is that the need for ultrasensitive detection systems is now more critical than ever. While sensors' sensitivity, portability, selectivity, and low cost are crucial, new ways to couple synergistic methods enable the highest performance levels. This review article critically discusses the synergetic combinations of optical and electrochemical methods. We also discuss three key application fields-energy, biomedicine, and environment. Finally, we selected the most promising approaches and examples, the open challenges in sensing, and ways to overcome them. We expect this work to set a clear reference for developing and understanding strategies, pros and cons of different combinations of electrochemical and optical sensors integrated into a single device.

13.
Inorg Chem ; 61(3): 1571-1589, 2022 Jan 24.
Artículo en Inglés | MEDLINE | ID: mdl-34982539

RESUMEN

δ-Bi2O3:M (M = S, Se, and Re) with an oxygen-defective fluorite-type structure is obtained by a coprecipitation method starting from the bismuth oxido cluster [Bi38O45(OMc)24(dmso)9]·2dmso·7H2O (A) in the presence of additives such as Na2SO4, Na2SeO4, NH4ReO4, Na2SeO3·5H2O, and Na2SO3. The coprecipitation of the starting materials with aqueous NaOH results in the formation of alkaline reaction mixtures, and the cubic bismuth(III)-based oxides Bi14O20(SO4) (1c), Bi14O20(SeO4) (2c), Bi14O20(ReO4.5) (3c), Bi12.25O16.625(SeO3)1.75 (4c), and Bi10.51O14.765(SO3)0.49(SO4)0.51 (5c) are obtained after microwave-assisted heating; formation of compound 5c is the result of partial oxidation of sulfur. The compounds 1c, 2c, 4c, and 5c absorb UV light only, whereas compound 3c absorbs in the visible-light region of the solar spectrum. Thermal treatment of the as-prepared metastable bismuth(III) oxide chalcogenates 1c and 2c at T = 600 °C provides a monotropic phase transition into their tetragonal polymorphs Bi14O20(SO4) (1t) and Bi14O20(SeO4) (2t), while compound 3c is transformed into the tetragonal modification of Bi14O20(ReO4.5) (3t) after calcination at T = 700 °C. Compounds of the systems Bi2O3-SOx (x = 2 and 3) and Bi2O3-Re2O7 are thermally stable up to T = 800 °C, whereas compounds of the system Bi2O3-SeO3 completely lose SeO3. Thermal treatment of 4c and 5c in air results in the oxidation of the tetravalent to hexavalent sulfur and selenium, respectively, upon heating to T = 400-500 °C. The as-prepared cubic bismuth(III)-based oxides 1c-5c were studied with regard to the photocatalytic decomposition of rhodamine B under visible-light irradiation with compound 3c showing the highest turnover and efficiency.

14.
Anal Chim Acta ; 1187: 338978, 2021 Dec 01.
Artículo en Inglés | MEDLINE | ID: mdl-34753586

RESUMEN

With the continuous growth of the human population and new challenges in the quality of life, it is more important than ever to diagnose diseases and pathologies with high accuracy, sensitivity and in different scenarios from medical implants to the operation room. Although conventional methods of diagnosis revolutionized healthcare, alternative analytical methods are making their way out of academic labs into clinics. In this regard, surface-enhanced Raman spectroscopy (SERS) developed immensely with its capability to achieve single-molecule sensitivity and high-specificity in the last two decades, and now it is well on its way to join the arsenal of physicians. This review discusses how SERS is becoming an essential tool for the clinical investigation of pathologies including inflammation, infections, necrosis/apoptosis, hypoxia, and tumors. We critically discuss the strategies reported so far in nanoparticle assembly, functionalization, non-metallic substrates, colloidal solutions and how these techniques improve SERS characteristics during pathology diagnoses like sensitivity, selectivity, and detection limit. Moreover, it is crucial to introduce the most recent developments and future perspectives of SERS as a biomedical analytical method. We finally discuss the challenges that remain as bottlenecks for a routine SERS implementation in the medical room from in vitro to in vivo applications. The review showcases the adaptability and versatility of SERS to resolve pathological processes by covering various experimental and analytical methods and the specific spectral features and analysis results achieved by these methods.


Asunto(s)
Calidad de Vida , Espectrometría Raman , Humanos
15.
Sensors (Basel) ; 21(12)2021 Jun 16.
Artículo en Inglés | MEDLINE | ID: mdl-34208587

RESUMEN

Electrochemical sensors play a significant role in detecting chemical ions, molecules, and pathogens in water and other applications. These sensors are sensitive, portable, fast, inexpensive, and suitable for online and in-situ measurements compared to other methods. They can provide the detection for any compound that can undergo certain transformations within a potential window. It enables applications in multiple ion detection, mainly since these sensors are primarily non-specific. In this paper, we provide a survey of electrochemical sensors for the detection of water contaminants, i.e., pesticides, nitrate, nitrite, phosphorus, water hardeners, disinfectant, and other emergent contaminants (phenol, estrogen, gallic acid etc.). We focus on the influence of surface modification of the working electrodes by carbon nanomaterials, metallic nanostructures, imprinted polymers and evaluate the corresponding sensing performance. Especially for pesticides, which are challenging and need special care, we highlight biosensors, such as enzymatic sensors, immunobiosensor, aptasensors, and biomimetic sensors. We discuss the sensors' overall performance, especially concerning real-sample performance and the capability for actual field application.


Asunto(s)
Técnicas Biosensibles , Nanocompuestos , Técnicas Electroquímicas , Agua , Calidad del Agua
16.
Adv Mater ; 33(8): e2005477, 2021 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-33475193

RESUMEN

Besides the pandemic caused by the coronavirus outbreak, many other pathogenic microbes also pose a devastating threat to human health, for instance, pathogenic bacteria. Due to the lack of broad-spectrum antibiotics, it is urgent to develop nonantibiotic strategies to fight bacteria. Herein, inspired by the localized "capture and killing" action of bacteriophages, a virus-like peroxidase-mimic (V-POD-M) is synthesized for efficient bacterial capture (mesoporous spiky structures) and synergistic catalytic sterilization (metal-organic-framework-derived catalytic core). Experimental and theoretical calculations show that the active compound, MoO3 , can serve as a peroxo-complex-intermediate to reduce the free energy for catalyzing H2 O2 , which mainly benefits the generation of •OH radicals. The unique virus-like spikes endow the V-POD-M with fast bacterial capture and killing abilities (nearly 100% at 16 µg mL-1 ). Furthermore, the in vivo experiments show that V-POD-M possesses similar disinfection treatment and wound skin recovery efficiencies to vancomycin. It is suggested that this inexpensive, durable, and highly reactive oxygen species (ROS) catalytic active V-POD-M provides a promising broad-spectrum therapy for nonantibiotic disinfection.


Asunto(s)
Antibacterianos/síntesis química , Materiales Biomiméticos/síntesis química , Óxidos/síntesis química , Peroxidasa/química , Antibacterianos/farmacología , Materiales Biocompatibles/química , Materiales Biomiméticos/farmacología , Catálisis , Humanos , Peróxido de Hidrógeno/metabolismo , Estructuras Metalorgánicas/química , Estructuras Metalorgánicas/farmacología , Simulación de Dinámica Molecular , Molibdeno/farmacología , Óxidos/farmacología , Peroxidasa/metabolismo , Esterilización , Vancomicina/farmacología
17.
Dalton Trans ; 49(31): 11010-11018, 2020 Aug 11.
Artículo en Inglés | MEDLINE | ID: mdl-32734976

RESUMEN

The development and application of photocatalysts with strong redox ability to degrade refractory pesticides is the key to eliminating pesticide contamination. In this work, we develop a facile, time-saving, and surfactant-assisted method to fabricate a new Z-scheme heterojunction based on TiO2/BiOCl. This photocatalyst is rich in oxygen vacancy defects (TiO2-OV-BiOCl), and displays an excellent photocatalytic degradation performance for imidacloprid (IMD), and a possible degradation pathway of IMD is provided. The surfactant F127 plays an essential role in regulating the oxygen vacancy defects (OVDs) of TiO2-OV-BiOCl, where the OVD mainly exists in 5 layer BiOCl ultrathin nanosheets. Free radical trapping experiments demonstrate that the introduction of an OVD in BiOCl as a 'charge mediator' changes the charge-transfer mode from a type-II mechanism to a Z-scheme mechanism. The formation of a Z-scheme heterojunction leads to an excellent light utilization and higher separation efficiency of photogenerated charge carriers with a prolonged lifetime compared to those of BiOCl and TiO2/BiOCl. This work highlights the critical role of an OVD in the construction of a Z-scheme heterojunction of TiO2/BiOCl, and it can be applied to construct efficient photocatalytic systems for pesticide degradation.


Asunto(s)
Bismuto/química , Insecticidas/química , Neonicotinoides/química , Nitrocompuestos/química , Luz Solar , Titanio/química , Titanio/efectos de la radiación , Contaminantes Químicos del Agua/química , Catálisis , Oxígeno
18.
ACS Omega ; 5(17): 10183-10190, 2020 May 05.
Artículo en Inglés | MEDLINE | ID: mdl-32391506

RESUMEN

We report the high-powered laser modification of the chemical, physical, and structural properties of the two-dimensional (2D) van der Waals material GaSe. Our results show that contrary to expectations and previous reports, GaSe at the periphery of a high-power laser beam does not entirely decompose into Se and Ga2O3. In contrast, we find unexpectedly that the Raman signal from GaSe gets amplified around regions where it was not expected to exist. Atomic force microscopy (AFM), dielectric force microscopy (DFM), scanning electron microscopy (SEM), and energy-dispersive X-ray spectroscopy (EDX) results show that laser irradiation induces the formation of nanoparticles. Our analyses demonstrate that, except for a fraction of Ga2Se3, these nanoparticles still belong to the GaSe phase but possess different electrical and optical properties. These changes are evidenced in the increased Raman intensity attributed to the near-resonance conditions with the Raman excitation laser. The elemental analysis of nanoparticles shows that the relative selenium content increased to as much as 70% from a 50:50 value in stoichiometric GaSe. This elemental change is related to the formation of the Ga2Se3 phase identified by Raman spectroscopy at some locations near the edge. Further, we exploit the localized high-power laser processing of GaSe to induce the formation of Ag-GaSe nanostructures by exposure to a solution of AgNO3. The selective reaction of AgNO3 with laser-irradiated GaSe gives rise to composite nanostructures that display photocatalytic activity originally absent in the pristine 2D material. The photocatalytic activity was investigated by the transformation of 4-nitrobenzenethiol to its amino and dimer forms detected in situ by Raman spectroscopy. This work improves the understanding of light-matter interaction in layered systems, offering an approach to the formation of laser-induced composites with added functionality.

19.
Nanomaterials (Basel) ; 10(2)2020 Jan 29.
Artículo en Inglés | MEDLINE | ID: mdl-32013163

RESUMEN

The properties and applications of Ag nanowires (AgNWs) are closely related to their morphology and composition. Therefore, controlling the growth process of AgNWs is of great significance for technological applications and fundamental research. Here, silver nanowires (AgNWs) were synthesized via a typical polyol method with the synergistic effect of Cl-, Br-, and Fe3+ mediated agents. The synergistic impact of these mediated agents was investigated intensively, revealing that trace Fe3+ ions provided selective etching and hindered the strong etching effect from Cl- and Br- ions. Controlling this synergy allowed the obtainment of highly uniform AgNWs with sub-30 nm diameter and an aspect ratio of over 3000. Transparent conductive films (TCFs) based on these AgNWs without any post-treatment showed a very low sheet resistance of 4.7 Ω sq-1, a low haze of 1.08% at a high optical transmittance of 95.2% (at 550 nm), and a high figure of merit (FOM) of 1210. TCFs exhibited a robust electrical performance with almost unchanged resistance after 2500 bending cycles. These excellent high-performance characteristics demonstrate the enormous potential of our AgNWs in the field of flexible and transparent materials.

20.
ACS Appl Mater Interfaces ; 12(8): 9797-9805, 2020 Feb 26.
Artículo en Inglés | MEDLINE | ID: mdl-31999093

RESUMEN

Graphitic carbon nitride (gCN) has a broad range of promising applications, from energy harvesting and storage to sensing. However, most of the applications are still restricted due to gCN poor dispersibility and limited functional groups. Herein, a direct photografting of gCN using various polymer brushes with tailorable functionalities via UV photopolymerization at ambient conditions is demonstrated. The systematic study of polymer brush-functionalized gCN reveals that the polymerization did not alter the inherent structure of gCN. Compared to the pristine gCN, the gCN-polymer composites show good dispersibility in various solvents such as water, ethanol, and tetrahydrofuran (THF). Patterned polymer brushes on gCN can be realized by employing photomask and microcontact printing technology. The polymer brushes with incorporated silver nanoparticles (AgNPs) on gCN can act as a multifunctional recyclable active sensing layer for surface-enhanced Raman spectroscopy (SERS) detection and photocatalysis. This multifunctionality is shown in consecutive cycles of SERS and photocatalytic degradation processes that can be applied to in situ monitor pollutants, such as dyes or pharmaceutical waste, with high chemical sensitivity as well as to water remediation. This dual functionality provides a significant advantage to our AgNPs/polymer-gCN with regard to state-of-the-art systems reported so far that only allow SERS pollutant detection but not their decomposition. These results may provide a new methodology for the covalent functionalization of gCN and may enable new applications in the field of catalysis, biosensors, and, most interestingly, environmental remediation.

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