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1.
Analyst ; 149(11): 3245-3262, 2024 May 28.
Artigo em Inglês | MEDLINE | ID: mdl-38687206

RESUMO

Artificial superhydrophobic surfaces that do not absorb water, like the lotus leaf, show tremendous promise in numerous applications. However, superhydrophobic surfaces are rarely used because of their low stability and endurance. A stable organic superhydrophobic surface (SHS) composed of novel morphology Ag-nanoparticles (NPs) has been fabricated on a copper alloy via etching, immersion, spraying, and annealing treatment, along with a static water contact angle (WCA) of 158 ± 1° and sliding angle (SA) less than 2°. The surface texture, composition, and morphology of the substrate surfaces were explored by using X-ray diffraction, X-ray photoelectron spectroscopy, scanning electron microscopy, energy dispersive spectroscopy, and DFT-based Ag atom distribution. The anti-corrosion study of non-coated and Ag-NP-coated copper alloy was undertaken using electrochemical impedance spectroscopy. Ag-NPs +SA@SHS enhanced the corrosion resistance as compared with bare Cu alloy. The water droplet rolled down the coated Cu alloy, removed the chalk powder from the surface, and indicated an excellent self-cleaning function. Photodegradation of Congo red (CR) and methylene blue (MB) dye samples was assessed by measuring the absorbance through UV-Visible spectrophotometry, where the Ag-NPs coated on the copper alloy were used as a catalyst. The performance of the SHS@Ag-NPs in the aqueous solution was 99.31% and 98.12% for industrial pollutants (CR and MB), with degradation rates of 5.81 × 10-2 s-1 and 5.89 × 10-2 s-1, respectively. These findings demonstrated a simple, rapid, and low-energy fabrication technique for SHS@Ag-NPs. This research reveals a valuable approach for the fabrication of SHS@Ag-NPs on various substrates to extend the superhydrophobic surfaces with ultra-fast self-healing properties, for outdoor applications such as anti-corrosion, for an innovative approach for the remediation of polluted water treatment, and for industrial applications.

2.
Molecules ; 29(9)2024 May 02.
Artigo em Inglês | MEDLINE | ID: mdl-38731594

RESUMO

The current study explores the prospective of a nitrogen-doped graphene (NG) incorporated into ZnSe-TiO2 composites via hydrothermal method for supercapacitor electrodes. Structural, morphological, and electronic characterizations are conducted using XRD, SEM, Raman, and UV analyses. The electrochemical study is performed and galvanostatic charge-discharge (GCD) and cyclic voltammetry (CV) are evaluated for the supercapacitor electrode material. Results demonstrate improved performance in the ZnSe-NG-TiO2 composite, indicating its potential for advanced supercapacitors with enhanced efficiency, stability, and power density. Specific capacity calculations and galvanic charge-discharge experiments confirmed the promising electrochemical activity of ZnSe-NG-TiO2, which has a specific capacity of 222 C/g. The negative link among specific capacity and current density demonstrated the composite's potential for high energy density and high-power density electrochemical devices. Overall, the study shows that composite materials derived from multiple families can synergistically improve electrode characteristics for advanced energy storage applications.

3.
Nanotechnology ; 33(50)2022 Oct 03.
Artigo em Inglês | MEDLINE | ID: mdl-36103847

RESUMO

The present study demonstrates the crucial role of agave americana extract in enhancing the optical properties of zinc oxide (ZnO) through thermal treatment method. Various analytical and surface science techniques have been used to identify the morphology, crystalline structure, chemical composition, and optical properties, including scanning electron microscopy, x-ray diffraction, high resolution transmission electron microscopy (HRTEM), x-ray spectroscopy (EDS) and UV-visible spectroscopy techniques. The physical studies revealed the transformation of ZnO nanorods into nanosheets upon addition of an optimized amount of agave americana extract, which induced large amount of amorphous carbon deposited onto ZnO nanostructures as confirmed by HRTEM analysis. The use of increasing amount of americana extract has significantly reduced the average crystallite size of ZnO nanostructures. The resultant hybrid system of C@ZnO has produced a significant effect on the ultraviolet light-assisted photodegradation of malachite green (MG) dye. The photocatalyst dose was fixed at 10 mg for each study whereas the amount of agave americana extract and MG dye concentration are varied. The functionality of hybrid system was greatly enhanced when the amount of agave americana extract increased while dye concentration kept at lower level. Ultimately, almost 100% degradation efficiency was achieved via the prepared hybrid material, revealing combined contribution from synergy, stabilization of ZnO due to excess of carbon together with the high charge separation rate. The obtained results suggest that the driving role of agave americana extract for surface modification of photocatalyst can be considered for other nanostructured photocatalysts.


Assuntos
Agave , Nanocompostos , Óxido de Zinco , Carbono , Catálise , Fotólise , Extratos Vegetais/química , Corantes de Rosanilina , Óxido de Zinco/química
4.
Phys Chem Chem Phys ; 24(48): 29609-29615, 2022 Dec 14.
Artigo em Inglês | MEDLINE | ID: mdl-36448740

RESUMO

The high demand for renewable and clean energy has driven the exploration of advanced energy storage systems. Sodium-ion batteries (SIBs) are considered to be potential substitutes for Li-ion batteries (LIBs) because they are manufactured from raw materials that are cheap, less toxic, and abundantly available. Recent developments have demonstrated that two-dimensional (2D) materials have gained increasing interest as electrode candidates for efficient SIBs because of their enormous surface area and sufficient accommodating sites for the storage of Na ions. Herein, we explore the binding and diffusion mechanisms of Na on a 2D SnS sheet using density functional theory (DFT). The outcomes reveal that Na has a strong binding strength with SnS as well as charge transfer from Na to SnS, which affirms an excellent electrochemical performance. A transition from semiconducting (1.4 eV band gap) to metallic has been noted in the electronic structure after loading a minor amount of Na. In addition, a low open-circuit voltage (OCV) of 0.87 V and a high storage capacity of 357 mA h g-1 show the suitability of the SnS monolayer for SIBs. In addition, the low activation barrier for Na migration (0.13 eV) is attractive for a fast sodiation/desodiation process. Henceforth, these encouraging outcomes suggest the application of the SnS sheet as an excellent anode for next-generation SIBs.

5.
Molecules ; 28(1)2022 Dec 29.
Artigo em Inglês | MEDLINE | ID: mdl-36615478

RESUMO

To satisfy the ever-increasing energy demands, it is of the utmost importance to develop electrochemical materials capable of producing and storing energy in a highly efficient manner. Titanium dioxide (TiO2) has recently emerged as a promising choice in this field due to its non-toxicity, low cost, and eco-friendliness, in addition to its porosity, large surface area, good mechanical strength, and remarkable transport properties. Here, we present titanium dioxide nanoplates/polyvinylidene fluoride (TiO2/PVDF) membranes prepared by a straightforward hydrothermal strategy and vacuum filtration process. The as-synthesized TiO2/PVDF membrane was applied for energy storage applications. The fabricated TiO2/PVDF membrane served as the negative electrode for supercapacitors (SCs). The electrochemical properties of a TiO2/PVDF membrane were explored in an aqueous 6 M KOH electrolyte that exhibited good energy storage performance. Precisely, the TiO2/PVDF membrane delivered a high specific capacitance of 283.74 F/g at 1 A/g and maintained capacitance retention of 91% after 8000 cycles. Thanks to the synergistic effect of TiO2 and PVDF, the TiO2/PVDF membrane provided superior electrochemical performance as an electrode for a supercapacitor. These superior properties will likely be used in next-generation energy storage technologies.


Assuntos
Polivinil , Titânio , Polivinil/química , Titânio/química , Água
6.
J Mol Graph Model ; 131: 108808, 2024 Jun 04.
Artigo em Inglês | MEDLINE | ID: mdl-38852428

RESUMO

Hydrogen energy has attracted a lot of interest from researchers as a sustainable and renewable energy source, but there are some technical challenges related to its storage. Hydride materials demonstrate the ability to store hydrogen adequately and safely. In the current study, we have investigated the structural and optoelectronic properties of the XCuH3 (where X = Li, Na and K) perovskite-type hydride using LDA and GGA formalisms for hydrogen storage application. Electronic properties such as band structure, density of states reveal the metallic character of the studied XCuH3 hydrides. Various optical parameters such as the complex dielectric function, refractive index, extinction coefficient, absorption coefficient, reflectivity, optical conductivity, energy loss function, and joint density of states have been computed and compared. The gravimetric hydrogen storage capacity for LiCuH3, NaCuH3 and KCuH3 are found to be 4.11, 3.37 and 2.86 wt%, respectively. The computed values of the gravimetric ratio manifest that XCuH3 hydrides are potential candidates for hydrogen storage applications. These calculations are made for the first time for XCuH3 hydrides and will be inspirational in the future for comparison and for hydrogen storage purposes.

7.
Heliyon ; 10(1): e24107, 2024 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-38226290

RESUMO

Perovskite photovoltaics have an immense contribution toward the all-round development of the solar cell. Apart from the flexibility, stability, and high efficiency, more stress has been given to using lead-free as well as eco-friendly, inexpensive materials in the fabrication of PSC devices. The utilization of non-volatile material, such as cesium tin iodide (CsSnI3), can be proposed for designing the PSC device, which not only makes it eco-friendly but also offers better optoelectronic characteristics due to its smaller bandgap of 1.27 eV. The inclusion of Sn in the perovskite material also functions as an increment in the stability of the perovskite. In the present simulation, CsSnI3 is used as an active absorber layer while the ZnMgO is used as an ETL for a cost-effective nature. Similarly, graphene oxide (GO) is used as HTL for a superior collection of holes. The comprehensive numerical modeling of the ZnMgO can be utilized in solar cell designing with appropriate CsSnI3 thickness, working temperature, total defectivity, and resistance impact, respectively. The presently simulated device offers an excellent efficiency of 17.37 % with CsSnI3-based PSC. These results of the study also show an effective route to develop highly efficient lead-free PSC devices.

8.
RSC Adv ; 14(9): 5981-5993, 2024 Feb 14.
Artigo em Inglês | MEDLINE | ID: mdl-38362074

RESUMO

In the current study, the association and phase separation of cationic tetradecyltrimethylammonium bromide (TTAB) and nonionic Triton X-100 (TX-100) surfactants with promethazine hydrochloride (PMH) were investigated in aqueous ammonium-based solutions. The micellization nature of the TTAB and PMH drug mixture was examined by evaluating critical micelle concentration (CMC) and counterion binding extent (ß) at different salt contents and temperatures (298.15-323.15 K). Micelle formation in the TTAB + PMH mixture was enhanced in the presence of ammonium salts, whereas the process was delayed with an increase in temperature in the respective salt solution. With an increase in salt content, the cloud point (CP) of the TX-100 + PMH mixture decreased, which revealed that the respective progression occurred through the salting out phenomenon. In micellization and clouding processes, the changes in free energies ΔG0m and ΔG0c were found to be negative and positive, respectively, demonstrating that the corresponding processes are spontaneous and non-spontaneous. Standard enthalpies (ΔH0m/ΔH0c) and standard entropies (ΔS0m/ΔS0c) for the association and clouding processes, respectively, were also calculated and discussed. The core forces amid TTAB/TX-100 and PMH in the manifestation of electrolytes are dipole-dipole and hydrophobic forces among the employed components according to the values for ΔH0m/ΔH0c and ΔS0m/ΔS0c, respectively.

9.
Heliyon ; 9(11): e20937, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-37928007

RESUMO

In this study, an electro-polymerized valine (VLN) stimulated carbon paste electrode (CPE) was used to create a straightforward, inexpensive, and renewable electrochemical sensor for accurate and selective indigotin (IGN) determination. Comparing the CPE, to the modified electrode, it exhibits excellent sensibility for the IGN oxidation-reduction reaction. Multiple techniques, including cyclic voltammetry (CV), differential pulse voltammetry (DPV), electrochemical impedance spectroscopy (EIS), and scanning electron microscopy (SEM) were utilized in this case to characterize the electrode materials. IGN was analyzed using CPE and poly(valine) modified carbon paste electrodes (P(VLN)MCPE) taking a 6.5 pH in 0.2 M phosphate buffer solution (PBS). Because it has more active spots than the CPE and a strong electrocatalytic nature, P(VLN)MCPE exhibits excellent electrochemical performance. The impact of pH, scan rate, numerous interferents, and fluctuation in analyte concentration were only a few of the important electrochemical factors that were investigated. The variation in scan rate proves that the IGN oxidation-reduction reaction on the surface of P(VLN)MCPE is as follows an adsorption-controlled pathway. The P(VLN)MCPE displays a good electrochemical nature for IGN in the 0.2 to 5.0 µM range, with a low limit of detection (LOD) is 0.0069 µM and a limit of quantification (LOQ) is 0.023 µM. P(VLN)MCPE shows good reproducibility, stability, and repeatability for the detection of IGN. Additionally, P(VLN)MCPE's analytical applicability for IGN detection in water sample was assessed with impressive recovery.

10.
Heliyon ; 9(3): e14378, 2023 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-36942251

RESUMO

In the present research work, selective and sensitive catechol (CT) detection and quantification were shown in the presence of resorcinol (RS) in 0.2 M phosphate buffer (PB) solution by preparing a low-cost, simple, and green carbon nanotube paste electrode (CNTPE) surface activated with electropolymerized riboflavin (PRF). The morphological, conductivity, and electrochemical features of the modified electrode (PRFMCNTPE) and bare carbon nanotube paste electrode (BCNTPE) materials were analyzed using electrochemical impedance spectroscopy (EIS), field emission scanning electron microscopy (FE-SEM), cyclic voltammetry (CV), and differential pulse voltammetry (DPV). The PRF-activated electrode displays outstanding sensitivity, stability, selectivity, reproducibility, and repeatability for the redox feature of CT with improved electrochemical current and declined electrochemical potential compared to BCNTPE. The peak currents of CT are correlated to the different CT concentrations (CV method: 6.0-60.0 µM & DPV method: 0.5-7.0 µM), and the obtained detection limit (DL) and quantification limit (QL) are found to be 0.025 µM and 0.085 µM (CV method) and 0.0039 µM and 0.0132 µM (DPV method), respectively. The prepared PRFMCNTPE material was advantageous for the examination of CT in environmentally important tap water sample as a real-time application.

11.
Nanoscale ; 15(12): 5712-5719, 2023 Mar 23.
Artigo em Inglês | MEDLINE | ID: mdl-36880499

RESUMO

Metal halide perovskite nanocrystals (NCs) are promising for photovoltaic and light-emitting applications. Due to the softness of their crystal lattice, structural modifications have a critical impact on their optoelectronic properties. Here we investigate the size-dependent optoelectronic properties of CsPbI3 NCs ranging from 7 to 17 nm, employing temperature and pressure as thermodynamic variables to modulate the energetics of the system and selectively tune the interatomic distances. By temperature-dependent photoluminescence spectroscopy, we have found that luminescence quenching channels exhibit increased non-radiative losses and weaker exciton-phonon coupling in bigger particles, in turn affecting the luminescence efficiency. Through pressure-dependent measurements up to 2.5 GPa, supported by XRD characterization, we revealed a NC-size dependent solid-solid phase transition from the γ-phase to the δ-phase. Importantly, the optical response to these structural changes strongly depends on the size of the NC. Our findings provide an interesting guideline to correlate the size and structural and optoelectronic properties of CsPbI3 NCs, important for engineering the functionalities of this class of soft semiconductors.

12.
ACS Energy Lett ; 8(9): 3876-3882, 2023 Sep 08.
Artigo em Inglês | MEDLINE | ID: mdl-37705702

RESUMO

Halide alloying in tin-based perovskites allows for photostable bandgap tuning between 1.3 and 2.2 eV. Here, we elucidate how the band edge energetics and associated defect activity impact the optoelectronic properties of this class of materials. We find that by increasing the bromide:iodide ratio, a simultaneous destabilization of acceptor defects (tin vacancies and iodine interstitials) and stabilization of donor defects (iodine vacancies and tin interstitials) occurs, with strong changes arising for Br contents exceeding 50%. This translates into a decreased doping which is, however, accompanied by a higher density of nonradiative recombination channels. Films with high Br content show a high degree of disorder and trap state densities, with the best optoelectronic quality being found for Br contents of around 33%. These observations match the open circuit voltage trend of tin-based mixed halide perovskite solar cells, supporting the relevance of optoelectronic properties and chemistry of defects to optimize wide-bandgap tin perovskite devices.

13.
Nanomaterials (Basel) ; 13(23)2023 Nov 27.
Artigo em Inglês | MEDLINE | ID: mdl-38063722

RESUMO

Ti3C2-MXene material, known for its strong electronic conductivity and optical properties, has emerged as a promising alternative to noble metals as a cocatalyst for the development of efficient photocatalysts used in environmental cleanup. In this study, we investigated the photodegradation of crystal-violet (CV) dye when exposed to UV light using a newly developed photocatalyst known as Ti3C2-MXene/NiO nanocomposite-decorated CsPbI3 perovskite, which was synthesized through a hydrothermal method. Our research investigation into the structural, morphological, and optical characteristics of the Ti3C2-MXene/NiO/CsPbI3 composite using techniques such as FTIR, XRD, TEM, SEM-EDS mapping, XPS, UV-Vis, and PL spectroscopy. The photocatalytic efficacy of the Ti3C2-MXene/NiO/CsPbI3 composite was assessed by evaluating its ability to degrade CV dye in an aqueous solution under UV-light irradiation. Remarkably, the Ti3C2-MXene/NiO/CsPbI3 composite displayed a significant improvement in both the degradation rate and stability of CV dye when compared to the Ti3C2-MXene/NiO nanocomposite and CsPbI3 perovskite materials. Furthermore, the UV-visible absorption spectrum of the Ti3C2-MXene/NiO/CsPbI3 composite demonstrated a reduced band gap of 2.41 eV, which is lower than that of Ti3C2-MXene/NiO (3.10 eV) and Ti3C2-MXene (1.60 eV). In practical terms, the Ti3C2-MXene/NiO/CsPbI3 composite achieved an impressive 92.8% degradation of CV dye within 90 min of UV light exposure. We also confirmed the significant role of photogenerated holes and radicals in the CV dye removal process through radical scavenger trapping experiments. Based on our findings, we proposed a plausible photocatalytic mechanism for the Ti3C2-MXene/NiO/CsPbI3 composite. This research may open up new avenues for the development of cost-effective and high-performance MXene-based perovskite photocatalysts, utilizing abundant and sustainable materials for environmental remediation.

14.
Chemosphere ; 313: 137424, 2023 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-36495985

RESUMO

The efficacy of novel polycarbonate ultrafiltration, aluminum oxide nanoparticle (Al2O3-NPs) volume fraction, temperature, and water/ethylene glycol (EG) ratio were evaluated to determine the thermophysical properties of the membrane. 5%-10% of Al2O3-NPs have been added to the PC. A machine learning approach was used to compare the volume fraction of Al2O3-NPs, the temperature, and the water-to-ethylene glycol (EG) ratio. To determine the impact of Al2O3-NPs loading on the Response Surface Method (RSM), DOE, ANOVA, ANN, MLP, and NSGA-II, the number of aluminum oxide nanoparticles (Al2O3-NPs), temperature, and water/ethylene glycol (EG) on membranes in PC ultrafiltration are evaluated. Based on the Relative Thermal Conductivity Model (RSM), the regression coefficient of Al2O3 in water and EG was 0.9244 and 0.9170 with adjusted regression coefficients. A higher concentration of EG enhances the thermal conductivity of the membrane when the effective parameters are considered. The effect of temperature on the relative viscosity of the membrane led to the conclusion that Al2O3 water/EG can cool at high temperatures while providing no viscosity change. When Al2O3 is dissolved in water and EG, more EG is necessary to optimize the mode of reactivity. Using the MLP model, the calculated R-value is 0.9468, the MSE is 0.001752989 (mean square error), and the MAE is 0.01768558 (mean absolute error). RSM predicted the average thermal conductivity behavior of nanofluid better. The ANN model, however, has proven to be more effective than the RSM in simulating the relative viscosity of nanofluids. The NSGA-II optimized results showed that the minimum relative viscosity and maximum coefficient of thermal conductivity occurred at the lowest water ratio and maximum temperature.


Assuntos
Nanopartículas , Água , Temperatura , Ultrafiltração , Óxido de Alumínio , Etilenoglicóis
15.
ACS Appl Mater Interfaces ; 14(30): 34180-34188, 2022 Aug 03.
Artigo em Inglês | MEDLINE | ID: mdl-34585916

RESUMO

The instability of halide perovskites toward moisture is one of the main challenges in the field that needs to be overcome to successfully integrate these materials in commercially viable technologies. One of the most popular ways to ensure device stability is to form 2D/3D interfaces by using bulky organic molecules on top of the 3D perovskite thin film. Despite its promise, it is unclear whether this approach is able to avoid 3D bulk degradation under accelerated aging conditions, i.e., thermal stress and light soaking. In this regard, it is crucial to know whether the interface is structurally and electronically stable or not. In this work, we use the bulky phenethylammonium cation (PEA+) to form 2D layers on top of 3D single- and triple-cation halide perovskite films. The dynamical change of the 2D/3D interface is monitored under thermal stress and light soaking by in situ photoluminescence. We find that under pristine conditions the large organic cation diffuses only in 3D perovskite thin films of poor structural stability, i.e., single-cation MAPbI3. The same diffusion and a dynamical change of the crystalline structure of the 2D/3D interface are observed even on high-quality 3D films, i.e., triple-cation MAFACsPbI3, upon thermal stress at 85 °C and light soaking. Importantly, under such conditions, the resistance of the thin film to moisture is lost.

16.
ACS Omega ; 7(39): 35191-35203, 2022 Oct 04.
Artigo em Inglês | MEDLINE | ID: mdl-36211035

RESUMO

This study shows the electrical conductivity-dependent gas sensing characteristics of spray-deposited rare earth (RE) metal ion (Sm3+, Ce3+, Pr3+, La3+)-doped cadmium oxide (CdO) thin films on soda-lime microscope glass substrates at 300 °C. We examined the deposited films' structural, surface microstructural, DC electrical, and gas sensing features. The X-ray diffraction study indicates that all samples were polycrystalline, with the favored growth direction shifting from the (111) plane to the (200) plane. The highest root-mean-square values were obtained for the Pr-doped CdO thin film (5.86 nm). The surface microstructure of CdO thin films was significantly influenced by the RE metal ion dopant, with typical grain size values ranging from 64 nm to 134 nm depending on the dopant. The carrier concentration and resistivity of CdO films vary based on the RE metal ions used as dopants. Low resistivity (3.01 × 10-4 Ω.cm) was achieved for the CdO thin film doped with La. High gas sensitivity (71.42%) was achieved for CdO thin films doped with La. The donor dopant regulated the electrical conductivity and gas sensing capabilities of CdO thin films.

17.
Diagnostics (Basel) ; 12(12)2022 Dec 09.
Artigo em Inglês | MEDLINE | ID: mdl-36553121

RESUMO

Rutin (RU) is one of the best-known natural antioxidants with various physiological functions in the human body and other plant species. In this work, an efficient voltammetric sensor to detect RU in food samples was explicated using a poly (glutamic acid)-modified graphene paste electrode (PGAMGPE). In order to detect RU, the proposed sensor diminishes material resistance and overpotential while increasing kinetic rate, peak currents, and material conductance. Using differential pulse voltammetry (DPV) and cyclic voltammetry (CV), the analysing efficiency of a PGAMGPE and a Bare graphene paste electrode (BGPE) was evaluated in 0.2 M phosphate buffer (PB) at an ideal pH of 6.5. in a potential window of -0.25 V to 0.6 V. Electrochemical impedance spectroscopy (EIS) was used to analyse the prepared electrode materials' conductivity, charge transfer resistance, and the kinetics of electron transport. Field emission scanning electron microscopy (FE-SEM) images were considered to compare the exterior morphology of the PGAMGPE and the BGPE. It was discovered that the PGAMGPE and the BGPE have electroactive surfaces of 0.062 cm2 and 0.04 cm2, respectively. It was determined that two protons and two electrons participated in the redox process. The resultant limit of detection (LOD) was found to be 0.04 µM and 0.06 µM, respectively, using DPV and CV methods. In spite of common interferents such as metal ions and chemical species, the developed sensor's selectivity for RU detection was impressive. For the simultaneous analysis of RU in the presence of caffeine (CF), the PGAMGPE affords a good electrochemical nature for RU with good selectivity. Due to the good stability, repeatability, reproducibility, and ease of use of the present RU sensor, it is useful for real sample analysis such as food and medicinal samples with recovery ranging from 94 to 100%.

18.
Mater Horiz ; 9(6): 1763-1773, 2022 Jun 06.
Artigo em Inglês | MEDLINE | ID: mdl-35510702

RESUMO

Tin halide perovskites have recently emerged as promising materials for low band gap solar cells. Much effort has been invested on controlling the limiting factors responsible for poor device efficiencies, namely self-p-doping and tin oxidation. Both phenomena are related to the presence of defects; however, full understanding of their implications in the optoelectronic properties of the material is still missing. We provide a comprehensive picture of the competing radiative and non-radiative recombination processes in tin-based perovskite thin films to establish the interplay between doping and trapping by combining photoluminescence measurements with trapped-carrier dynamic simulations and first-principles calculations. We show that pristine Sn perovskites, i.e. sample processed with commercially available SnI2 used as received, exhibit extremely high radiative efficiency due to electronic doping which boosts the radiative band-to-band recombination. Contrarily, thin films where Sn4+ species are intentionally introduced show drastically reduced radiative lifetime and efficiency due to a dominance of Auger recombination at all excitation densities when the material is highly doped. The introduction of SnF2 reduces the doping and passivates Sn4+ trap states but conversely introduces additional non-radiative decay channels in the bulk that fundamentally limit the radiative efficiency. Overall, we provide a qualitative model that takes into account different types of traps present in tin-perovskite thin films and show how doping and defects can affect the optoelectronic properties.

19.
Biosensors (Basel) ; 12(4)2022 Apr 10.
Artigo em Inglês | MEDLINE | ID: mdl-35448291

RESUMO

MXenes-Ti3C2Tx, based on their versatile surface characteristics, has rapidly advanced as an interactive substrate to develop electrochemical sensors for clinical applications. Herein, Ni embedded Ti3C2Tx (MX-Ni) composites were prepared using a self-assembly approach where Ti3C2Tx sheets served as an interactive conductive substrate as well as a protective layer to nickel nanoparticles (Ni NPs), preventing their surface oxidation and aggregation. The composite displayed a cluster-like morphology with an intimate interfacial arrangement between Ni, Ti3C2Tx and Ti3C2Tx-derived TiO2. The configuration of MX-Ni into an electrochemical sensor realized a robust cathodic reduction current against methylmalonic acid (MMA), a biomarker to vitamin B12 deficiency. The synergism of Ni NPs strong redox characteristics with conductive Ti3C2Tx enabled sensitive signal output in wide detection ranges of 0.001 to 0.003 µM and 0.0035 to 0.017 µM and a detection sensitivity down to 0.12 pM of MMA. Importantly, the sensor demonstrated high signal reproducibility and excellent operational capabilities for MMA in a complex biological matrix such as human urine samples.


Assuntos
Ácido Metilmalônico , Nanopartículas , Eletrodos , Humanos , Reprodutibilidade dos Testes , Titânio
20.
RSC Adv ; 12(29): 18321-18332, 2022 Jun 22.
Artigo em Inglês | MEDLINE | ID: mdl-35799920

RESUMO

In this study, we have used cotton silk as a source of abundant hydroxyl groups for the fast nucleation/growth of cobalt oxide (Co3O4) nanowires via a hydrothermal method. The crystal planes of the Co3O4 nanowires well matched the cubic phase. The as-synthesized Co3O4 nanowires mainly contained cobalt and oxygen elements and were found to be highly sensitive towards uric acid in 0.01 M phosphate buffer solution at pH 7.4. Importantly, the Co3O4 nanowires exhibited a large surface area, which was heavily utilized during the immobilization of the enzyme uricase via a physical adsorption method. The potentiometric response of the uricase-immobilizing Co3O4 nanowires was measured in the presence of uric acid (UA) against a silver/silver chloride (Ag/AgCl) reference electrode. The newly fabricated uric acid biosensor possessed a low limit of detection of 1.0 ± 0.2 nM with a wide linear range of 5 nM to 10 mM and sensitivity of 30.6 mV dec-1. Additionally, several related parameters of the developed uric acid biosensor were investigated, such as the repeatability, reproducibility, storage stability, selectivity, and dynamic response time, and these were found to be satisfactory. The good performance of the Co3O4 nanowires was verified based on the fast charge-transfer kinetics, as confirmed via electrochemical impedance spectroscopy. The successful practical use of the uric acid biosensor was demonstrated based on the recovery method. The observed performance of the uricase-immobilizing Co3O4 nanowires revealed that they could be considered as a promising and alternative tool for the detection of uric acid under both in vitro and in vivo conditions. Also, the use of cotton silk as a source of abundant hydroxyl groups may be considered for the remarkably fast nucleation/growth of other metal-oxide nanostructures, thereby facilitating the fabrication of functional electrochemical devices, such as batteries, water-splitting devices, and supercapacitors.

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