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1.
J Environ Sci (China) ; 148: 437-450, 2025 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-39095178

RESUMEN

For environmental applications, it is crucial to rationally design and synthesize photocatalysts with positive exciton splitting and interfacial charge transfer. Here, a novel Ag-bridged dual Z-scheme Ag/g-C3N4/CoNi-LDH plasmonic heterojunction was successfully synthesized using a simple method, with the goal of overcoming the common drawbacks of traditional photocatalysts such as weak photoresponsivity, rapid combination of photo-generated carriers, and unstable structure. These materials were characterized by XRD, FT-IR, SEM, TEM UV-Vis/DRS, and XPS to verify the structure and stability of the heterostructure. The pristine LDH, g-C3N4, and Ag/g-C3N4/CoNi-LDH composite were investigated as photocatalysts for water remediation, an environmentally motivated process. Specifically, the photocatalytic degradation of tetracycline was studied as a model reaction. The performance of the supports and composite catalyst were determined by evaluating both the degradation and adsorption phenomenon. The influence of several experimental parameters such as catalyst loading, pH, and tetracycline concentration were evaluated. The current study provides important data for water treatment and similar environmental protection applications.


Asunto(s)
Nanocompuestos , Fotólisis , Plata , Contaminantes Químicos del Agua , Purificación del Agua , Nanocompuestos/química , Contaminantes Químicos del Agua/química , Purificación del Agua/métodos , Plata/química , Catálisis , Nitrilos/química , Compuestos de Nitrógeno/química , Adsorción , Grafito
2.
Artículo en Inglés | MEDLINE | ID: mdl-39267343

RESUMEN

The defect design strategy has been extensively employed to enhance the reaction kinetics of layered double hydroxide (LDH) electrode materials. Furthermore, it is anticipated to improve the cyclic stability of LDHs through this approach, serving a dual purpose. However, the potential mechanisms of cation vacancies' impact on the electrochemical performance of electrodes at the atomic scale still need further clarification. In this study, a typical aluminum-vacancy LDH material via a simple alkaline etching method was demonstrated. Electrochemical in situ Raman spectroscopy, ex situ X-ray diffraction (XRD), and first-principles calculations were utilized to elucidate the mechanism of Faradaic reactions. The findings indicate that this cation vacancy strategy not only enhances the electrochemical reaction kinetics of the electrodes but also effectively reduces the energy barrier for the α to γ phase transition of LDHs during the charge-discharge processes, thereby enhancing its longevity. To further validate the practical application of this defect design, an asymmetric solid-state supercapacitor was formed, which maintains 93.9% capacity after 20 000 charge-discharge cycles. This research offers technical guidance for the development of a new generation of high-performance and long-life LDH electrode materials based on a cation vacancy strategy.

3.
J Colloid Interface Sci ; 678(Pt A): 920-936, 2024 Aug 28.
Artículo en Inglés | MEDLINE | ID: mdl-39226833

RESUMEN

Layered double hydroxide (LDH) material with abundant OH was successfully prepared by co-precipitation method, and a water purification system of Ni2Fe0.25Al0.75-LDH activated peroxymonosulfate (PMS) was constructed to rapidly degrade sulfamethoxazole (SMX) pollutants. The optimal conditions for the degradation of SMX in the system were as follows: 0.30 g/L Ni2Fe0.25Al0.75-LDH, 0.30 mM PMS, pH = 7 and 90 % SMX was removed in 10 min and almost completely in 40 min, which was consistent with the predicted results of response surface methodology (RSM) analysis. The abundant OH in Ni2Fe0.25Al0.75-LDH could form M(O)OSO3 complexes with PMS, accelerating the generation of reactive oxygen species (ROS) and promoting the removal of SMX. Quenching experiments and electron paramagnetic resonance (EPR) spectra showed that SO4-, OH, O2- and 1O2 also existed in the system. The surface-bound SO4- and O2- contributed greatly to the removal of SMX and the electron transfer between metals was also conducive to the production of active substances. The possible degradation pathways and intermediates of SMX were proposed. The toxicity assessment software tool (T.E.S.T) and total organic carbon (TOC) results indicated that the Ni2Fe0.25Al0.75-LDH/PMS system could reduce the overall environmental risk of SMX to some extent. This study provided a new strategy for the practical application of heterogeneous catalysts in sewage treatment.

4.
ACS Appl Mater Interfaces ; 16(37): 49868-49879, 2024 Sep 18.
Artículo en Inglés | MEDLINE | ID: mdl-39231011

RESUMEN

The supercapacitor-diode (CAPode) is a device that integrates the functionality of an ionic diode with that of a conventional supercapacitor. The unique combination of energy storage and rectification properties in CAPodes is relevant for iontronics, alternate current rectifiers, logic operations, grid stabilization, and even biomedical applications. Here, we propose a novel aqueous-phase supercapattery-diode with excellent energy storage [total specific capacity (CT) = 162 C g-1, energy density = 34 W h kg-1 at 1.0 A g-1] as well as rectifying properties [rectification ratio I (RRI) of 23, and rectification ratio II (RRII) of 0.98]; the unidirectional energy storage is achieved by the utilization of an ion-selective redox reaction of battery-type layered double hydroxide (LDH) nanosheets serving as the electroactive material as well as asymmetric device configuration of supercapattery-diode in the KOH electrolyte. This work expands the types of CAPodes and importantly exemplifies the significance of integrating battery-type LDH and their redox chemistry, allowing a simultaneous increase in charge storage and rectification properties.

5.
J Colloid Interface Sci ; 678(Pt C): 393-408, 2024 Sep 14.
Artículo en Inglés | MEDLINE | ID: mdl-39303558

RESUMEN

Given the notoriously poor wear performance of Ti6Al4V (TC4) alloys, two types of MgAl layered double hydroxides (LDHs) were synthesized as lubrication additives. Systematic tribological tests were conducted to explore the performance of the TC4 alloy with these MgAl LDHs at varying concentrations in oil. It was found that, with increasing additive concentration, the wear resistance of TC4 significantly improved. Notably, MgAl LDHs with a hexagonal nanosheet structure exhibited superior lubrication performance, reducing the coefficient of friction (COF) by approximately 67.94 % compared to dry friction, and markedly enhancing the anti-wear characteristics of the TC4 alloy. Furthermore, to improve the utility of TC4 alloy in industrial applications, titanium nitride (TiN) coatings with excellent mechanical properties were deposited onto the TC4 substrate using arc ion deposition. A comprehensive analysis of the tribological behavior and wear mechanisms of TiN coating with the two MgAl LDHs additives was also conducted. Results indicated that the combination of TiN hard coatings and MgAl LDHs lubricants achieved high wear resistance for the TC4 substrate. In conclusion, a low-wear synergistic protection system integrating TiN coatings and high-performance MgAl LDHs lubricants was developed, demonstrating effective protection for TC4 alloys. This strategy not only presents a novel approach for reducing wear in TC4 alloys but also provides a reliable method for safeguarding and ensuring the long-term stability of titanium alloys mechanical components under demanding conditions.

6.
Small ; : e2404927, 2024 Sep 10.
Artículo en Inglés | MEDLINE | ID: mdl-39252634

RESUMEN

Heterostructures of layered double hydroxides (LDHs) and MXenes have shown great promise for oxygen evolution reaction (OER) catalysts, owing to their complementary physical properties. Coupling LDHs with MXenes can potentially enhance their conductivity, stability, and OER activity. In this work, a scalable and straightforward in situ guided growth of CoFeLDH on Ti3C2Tx is introduced, where the surface chemistry of Ti3C2Tx dominates the resulting heterostructures, allowing tunable crystal domain sizes of LDHs. Combined simulation results of Monte Carlo and density functional theory (DFT) validate this guided growth mechanism. Through this way, the optimized heterostructures allow the highest OER activity of the overpotential = 301 mV and Tafel slope = 43 mV dec-1 at 10 mA cm-2, and a considerably durable stability of 0.1% decay over 200 h use, remarkably outperforming all reported LDHs-MXenes materials. DFT calculations indicate that the charge transfer in heterostructures can decrease the rate-limiting energy barrier for OER, facilitating OER activity. The combined experimental and theoretical efforts identify the participation role of MXene in heterostructures for OER reactions, providing insights into designing advanced heterostructures for robust OER electrocatalysis.

7.
Environ Sci Technol ; 2024 Sep 16.
Artículo en Inglés | MEDLINE | ID: mdl-39279665

RESUMEN

Conventional approaches for in situ remediation of mercury (Hg)-contaminated soils and sediments rely mostly on precipitation or adsorption. However, this can generate Hg-rich surfaces that facilitate microbial production of methylmercury (MeHg), a potent, bioaccumulative neurotoxin. Herein, we prove the concept that the risk of mercury methylation can be effectively minimized by adding sulfur-intercalated layered double hydroxide (S-LDH) to Hg-contaminated soils. Hg bound to S-LDH has minimal methylation potential when incubated with model methylating bacteria Pseudodesulfovibrio mercurii ND132 and Geobacter sulfurreducens PCA. With a combination of spectroscopic and microscopic evidence, as well as theoretical calculations, we confirm that dissolved Hg(II) tends to enter the interlayers of S-LDH to bind to the sulfur groups intercalated within, leading to the formation of nanoscale metacinnabar (ß-HgS). This not only physically blocks the contact of methylating microorganisms but also inhibits secondary release of bound mercury in the presence of strong binding ligands in porewater. This study highlights the promising concept of in situ risk reduction of heavy metal contamination by inducing precipitation within (nano)confined domains, achieving a sustainable outcome of enhanced removal and reduced bioaccessibility for pollutants that may otherwise be bioavailable in the form of nanoprecipitates.

8.
J Colloid Interface Sci ; 678(Pt B): 1036-1048, 2024 Sep 06.
Artículo en Inglés | MEDLINE | ID: mdl-39276513

RESUMEN

The development of efficient and stable electrocatalysts is crucial for the advancement of green and clean hydrogen energy technologies. In this work, we synthesized a nanocomposite of nickel-iron layered double hydroxide/molybdenum titanium carbide (NiFe-LDHs/Mo2Ti2C3) using a deep eutectic solvent (DESs) by the solvothermal method. The formation of NiFe-LDHs/Mo2Ti2C3 nanocomposite was confirmed by various electron microscopic and spectroscopic techniques. The synthesized nanocomposite was investigated as a bifunctional electrocatalyst for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) under the alkaline condition. The NiFe-LDHs/Mo2Ti2C3-based electrodes exhibit small overpotentials of 204 and 306 mV for HER and OER at a current density of 10 mA cm-2. The anchor of NiFe-LDHs on the surface of Mo2Ti2C3 induces an interfacial synergistic effect, leading to a significantly improvement in electrochemical performance. Remarkably, the proposed NiFe-LDHs/Mo2Ti2C3 modified electrode demonstrates superior performance compared to many recently reported LDHs and MXenes-based electrocatalysts in an alkaline environment. Furthermore, a symmetrical two-electrode water splitting setup employing the NiFe-LDHs/Mo2Ti2C3 electrocatalyst requires an electrolysis voltage of 1.65 V to achieve a current density of 10 mA cm-2. The findings provide a new perspective on the rational design and synthesis of multifunctional electrocatalysts for electrochemical applications.

9.
Artículo en Inglés | MEDLINE | ID: mdl-39264097

RESUMEN

The layered double hydroxides (LDHs) have demonstrated significant potential as non-noble-metal electrocatalysts for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Their unique compositional and structural properties contribute to their efficiency and stability as catalysts. In this study, CoCuFe-LDH composites were grown on graphene (G) via a cost-effective and straightforward one-step hydrothermal process. A 2-level full-factorial model was employed to determine the impact of Co (1.5, 3, and 4.5 mmol) and graphene (10, 30, and 50 mg) concentrations on the onset potential of OER and HER, which were the chosen response variables. OER and HER activity variabilities were assessed in triplicate using Co[3]Cu[3]Fe[3]-LDH/G[30] (central point), which were determined at 0.01% and 0.02%, respectively. Statistical analyses demonstrated that Co[4.5]Cu[3]Fe[3]-LDH/G[10] and Co[1.5]Cu[3]Fe[3]-LDH/G[10] showed the lowest onset potential at 1.52 V and -0.32 V (V vs RHE) for the OER and HER, respectively, suggesting that a high cobalt concentration enhances OER performance, while optimal HER catalysis was achieved with lower cobalt concentrations. Moreover, the trimetallic composites exhibited good stability with negligible loss of catalytic activity over 24 h.

10.
Chemosphere ; 364: 143070, 2024 Aug 13.
Artículo en Inglés | MEDLINE | ID: mdl-39142393

RESUMEN

Lead (Pb) contamination in water requires improved decontamination technologies. The addition of phosphate to precipitate Pb2+ is a widely used method for remediating Pb in soil and water, though it has certain limitations. This study focuses on novel 3D mesoporous layered double hydroxide (LDH) sorbents functionalized with phosphate anions for Pb2+ removal from contaminated waters. Our innovative strategy involves converting a sacrificial template metal-organic frameworks (MOFs) structure (MIL-88A(Fe)) into NixFe LDH, followed by an anion exchange reaction with phosphate anions. This process preserves the 3D microrod architecture of MIL-88A and prevents deleterious LDH particle aggregation. The synthesis results in stable microrod crystals, 1-2 µm long, composed of 3D assemblies of NixFe-PO4 LDH nanoplatelets with a specific surface area exceeding 110 m2/g. The novel LDH materials display fast adsorption kinetics (pseudo-second order model) and remarkably high Pb2+ removal performances (Langmuir isotherm model) with a capacity of 538 mg/g, surpassing other reported adsorbents. LDH-PO4 exhibits high selectivity for Pb2+ over competing ions like Ni2+ and Cd2+ (selectivity order is: Pb2+ > Ni2+ > Cd2+). Removal of Pb2+ from NixFeLDH/88A-PO4 involves various mechanisms, including surface complexation and surface precipitation of lead phosphate or lead hydroxide phases as revealed by structural characterization techniques.

11.
Environ Sci Pollut Res Int ; 31(42): 54832-54853, 2024 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-39215915

RESUMEN

In this study, Ag2CrO4@NiFe-LDH nanoparticles were synthesized by hydrothermal method for photocatalytic degradation of Alizarin Red (AR) dye. Three composites with different molar percentages were prepared, among which 50%Ag2CrO4@50%NiFe-LDH composite was the best sample with a removal rate of 97.1% in AR degradation. Also, the properties, structure, and characteristics of pure Ag2CrO4 and NiFe-LDH and their composites were determined by XRD, FESEM, FTIR, EDX mapping, and UV-visible analyses. It was found that Ag2CrO4@NiFe-LDH composites with the formation of heterogeneous structure of Z-scheme, in addition to increasing the active sites and increasing the specific surface, decrease the recombination rate of pure Ag2CrO4 and NiFe-LDH. Also, the Box-Behnken design technique, which is one of the most common designs used in response surface methodology, was used to optimize the operating conditions and investigate the effect of 4 independent parameters: catalyst amount, solution concentration, pH, and light intensity. The importance of independent parameters and their interactions were determined by ANOVA. By means of numerical optimization, the optimal values of the selected parameters equal to 1.34 g/L of catalyst, concentration of 16.45 mg/L, pH = 10.74, and light intensity of 15.53 W were obtained as optimal conditions with a desirability coefficient of 1.00 and an absorption value of 89.34%. The closeness of adjusted R2 (0.9838) and predicted R2 (0.9507) values show that this model can be successfully used for prediction.


Asunto(s)
Antraquinonas , Luz , Antraquinonas/química , Catálisis , Contaminantes Químicos del Agua/química
12.
Small Methods ; : e2400519, 2024 Aug 07.
Artículo en Inglés | MEDLINE | ID: mdl-39108187

RESUMEN

The development of nanomaterials for energy storage and conversion has always been important. Layered double hydroxide (LDH) is a promising material due to its high capacity, tunable composition and easy synthesis. In this work, the morphology of NiCo-LDH is tuned with surfactants including sodium dodecyl sulfate (SDS) and cetyltrimethylammonium bromide (CTAB), and investigated the correlation between morphology and electrochemical properties. NiCo-LDH-SDS with a layered structure exhibited a specific capacitance of 1004 C g-1 at 1 A g-1, which is higher than that of the needle-like NiCo-LDH-CTAB (678 C g-1) and the rod-like NiCo-LDH (279 C g-1). Meanwhile, NiCo-LDH-SDS and NiCo-LDH-CTAB showed a reduction of 36 and 19 mV, respectively, in their overpotentials at 10 mA cm-2 compared to NiCo-LDH. Contact angle and adhesive force measurements proved the influence of morphology on the interfacial properties that layered structure is favorable for the timely detachment of the bubbles. Therefore, rational morphology regulation of LDH can effectively alter the gas-liquid-solid interface and thereby accelerate the reaction kinetics. The connections between morphologies, bubbles releasing and electrochemical performance are well established in this work, which can be applied in the investigation of nanomaterials for energy-related activities, especially the ones concerning bubbles releasing processes.

13.
J Chromatogr A ; 1731: 465174, 2024 Aug 30.
Artículo en Inglés | MEDLINE | ID: mdl-39111195

RESUMEN

The present work describes a quick, simple, and efficient method based on the use of layered double hydroxides (LDH) coupled to dispersive solid phase micro-extraction (DSPME) to remove α-naphthol (α-NAP) and ß-naphthol (ß-NAP) isomers from water samples. Three different LDHs (MgAl-LDH, NiAl-LDH, and CoAl-LDH) were used to study how the interlayer anion and molar ratio affected the removal performance. The critical factors in the DSPME procedure (pH, LDH amount, contact time) were optimized by the univariate method under the optimal conditions: pH, 4-8; LDH amount, 5 mg; and contact time, 2.5 min. The method can be successfully applied in real sample waters, removing NAP isomers even in ultra-trace concentrations. The large volume sample stacking (LVSS-CE) technique provides limits of detections (LODs) of 5.52 µg/L and 6.36 µg/L for α-naphthol and ß-naphthol, respectively. The methodology's precision was evaluated on intra- and inter-day repeatability, with %RSD less than 10% in all cases. The MgAl/Cl--LDH selectivity was tested in the presence of phenol and bisphenol A, with a removal rate of >92.80%. The elution tests suggest that the LDH MgAl/Cl--LDH could be suitable for pre-concentration of α-naphthol and ß-naphthol in future works.


Asunto(s)
Electroforesis Capilar , Límite de Detección , Naftoles , Microextracción en Fase Sólida , Contaminantes Químicos del Agua , Naftoles/química , Naftoles/análisis , Naftoles/aislamiento & purificación , Contaminantes Químicos del Agua/análisis , Contaminantes Químicos del Agua/aislamiento & purificación , Contaminantes Químicos del Agua/química , Electroforesis Capilar/métodos , Microextracción en Fase Sólida/métodos , Hidróxidos/química , Isomerismo , Reproducibilidad de los Resultados , Concentración de Iones de Hidrógeno
14.
Adv Sci (Weinh) ; : e2403347, 2024 Aug 09.
Artículo en Inglés | MEDLINE | ID: mdl-39120546

RESUMEN

The highly immunosuppressive tumor microenvironment (TME) restricts the efficient activation of immune responses. To restore the surveillance of the immune system for robust activation, vast efforts are devoted to normalizing the TME. Here, a manganese-doped layered double hydroxide (Mn-LDH) is developed for potent anti-tumor immunity by reversing TME. Mn-LDH is synthesized via a one-step hydrothermal method. In addition to the inherent proton neutralization capacity of LDH, the introduction of manganese oxide endows LDH with an additional ability to produce oxygen. Mn-LDH effectively releases Mn2+ and Mg2+ upon exposure to TME with high levels of H+ and H2O2, which activates synthase-stimulator of interferon genes pathway and maintains the cytotoxicity of CD8+ T cells respectively, achieving a cascade-like role in innate and adaptive immunity. The locally administered Mn-LDH facilitated a "hot" network consisting of mature dendritic cells, M1-phenotype macrophages, as well as cytotoxic and helper T cells, significantly inhibiting the growth of primary and distal tumors. Moreover, the photothermal conversion capacity of Mn-LDH sparks more robust therapeutic effects in large established tumor models with a single administration and irradiation. Overall, this study guides the rational design of TME-modulating immunotherapeutics for robust immune activation, providing a clinical candidate for next-generation cancer immunotherapy.

15.
Adv Sci (Weinh) ; : e2401236, 2024 Aug 01.
Artículo en Inglés | MEDLINE | ID: mdl-39090836

RESUMEN

Anionic redox allows the direct formation of O─O bonds from lattice oxygens and provides higher catalytic in the oxygen evolution reaction (OER) than does the conventional metal ion mechanism. While previous theories have predicted and experiments have suggested the possible O─O bond, it has not yet been directly observed in the OER process. In this study, operando soft X-ray absorption spectroscopy (sXAS) at the O K-edge and the operando Raman spectra is performed on layered double CoFe hydroxides (LDHs) after intercalation with [Cr(C2O4)3]3-, and revealed a three-step oxidation process, staring from Co2+ to Co3+, further to Co4+ (3d6L), and ultimately leading to the formation of O─O bonds and O2 evolution above a threshold voltage (1.4 V). In contrast, a gradual oxidation of Fe is observed in CoFe LDHs. The OER activity exhibits a significant enhancement, with the overpotential decreasing from 300 to 248 mV at 10 mA cm-2, following the intercalation of [Cr(C2O4)3]3- into CoFe LDHs, underscoring a crucial role of anionic redox in facilitating water splitting.

16.
Fundam Res ; 4(4): 926-933, 2024 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-39156582

RESUMEN

Combining photodynamic therapy (PDT) with chemodynamic therapy (CDT) has been proven to be a promising strategy to improve the treatment efficiency of cancer, because of the synergistic therapeutic effect arising between the two modalities. Herein, we report an inorganic nanoagent based on ternary NiCoTi-layered double hydroxide (NiCoTi-LDH) nanosheets to realize highly efficient photodynamic/chemodynamic synergistic therapy. The NiCoTi-LDH nanosheets exhibit oxygen vacancy-promoted electron-hole separation and photogenerated hole-induced O2-independent reactive oxygen species (ROS) generation under acidic circumstances, realizing in situ pH-responsive PDT. Moreover, due to the effective conversion between Co3+ and Co2+ caused by photogenerated electrons, the NiCoTi-LDH nanosheets catalyze the release of hydroxyl radicals (·OH) from H2O2 through Fenton reactions, resulting in CDT. Laser irradiation enhances the catalyzed ability of the NiCoTi-LDH nanosheets to promote the ROS generation, resulting in a better performance than TiO2 nanoparticles at pH 6.5. In vitro and in vivo experimental results show conclusively that NiCoTi-LDH nanosheets plus irradiation lead to efficient cell apoptosis and significant inhibition of tumor growth. This study reports a new pH-responsive inorganic nanoagent with oxygen vacancy-promoted photodynamic/chemodynamic synergistic performance, offering a potentially appealing clinical strategy for selective tumor elimination.

17.
Adv Sci (Weinh) ; : e2403009, 2024 Aug 19.
Artículo en Inglés | MEDLINE | ID: mdl-39159063

RESUMEN

Periprosthetic infection and prosthetic loosing stand out as prevalent yet formidable complications following orthopedic implant surgeries. Synchronously addressing the two complications is long-time challenging. Herein, a bioactive glass scaffold (BGS) functionalized with MgCuFe-layered double hydroxide (LDH)-derived sulfide nanosheets (BGS/MCFS) is developed for vascularized osteogenesis and periprosthetic infection prevention/treatment. Apart from the antibacterial cations inhibiting bacterial energy and material metabolism, the exceptional near-infrared-II (NIR-II) photothermal performance empowers BGS/MCFS to eliminate periprosthetic infections, outperforming previously reported functionalized BGS. The rough surface topography and the presence of multi-bioactive metal ions bestow BGS/MCFS with exceptional osteogenic and angiogenic properties, with 8.5-fold and 2.3-fold enhancement in bone mass and neovascularization compared with BGS. Transcriptome sequencing highlights the involvement of the TGF-ß signaling pathway in these processes, while single-cell sequencing reveals a significant increase in osteoblasts and endothelial cells around BGS/MCFS compared to BGS.

18.
Small ; : e2404475, 2024 Aug 30.
Artículo en Inglés | MEDLINE | ID: mdl-39212201

RESUMEN

Novel inorganic sonosensitizers with excellent reactive oxygen species (ROS) generation activity and multifunctionality are appealing in sonodynamic therapy (SDT). Herein, amorphous bismuth (Bi)-doped CoFe-layered double hydroxide (a-CoBiFe-LDH) nanosheets are proposed via crystalline-to-amorphous phase transformation strategy as a new type of bifunctional sonosensitizer, which allows ultrasound (US) to trigger ROS generation for magnetic resonance imaging (MRI)-guided SDT. Importantly, a-CoBiFe-LDH nanosheets exhibit much higher ROS generation activity (≈6.9 times) than that of traditional TiO2 sonosensitizer under US irradiation, which can be attributed to the acid etching-induced narrow band gap, high electron (e-)/hole (h+) separation efficiency and inhibited e-/h+ recombination. In addition, the paramagnetic properties of Fe ion endow a-CoBiFe-LDH with excellent MRI contrast ability, making it a promising contrast agent for T2-weighted MRI. After modification with polyethylene glycol, a-CoBiFe-LDH nanosheets can function as a high-efficiency sonosensitizer to activate p53, MAPK, oxidative phosphorylation, and apoptosis-related signaling pathways, ultimately inducing cell apoptosis in vitro and tumor ablation in vivo under US irradiation, which shows great potential for clinical cancer treatment.

19.
Environ Pollut ; 361: 124850, 2024 Aug 29.
Artículo en Inglés | MEDLINE | ID: mdl-39216672

RESUMEN

This study evaluated the effects of post-calcination on the charge properties and active sites of Mg/Al layered double hydroxide-decorated spent coffee ground biochars (LDHMgAl@SCGB) governing adsorption behaviors and mechanisms of arsenic (AsV) and antimony (SbV) anions from aqueous phases. Post-calcinated LDHMgAl@SCGB (PLDHMgAl@SCGB) exhibited higher adsorption capacities for AsV and SbV compared to spent coffee ground biochars (SCGB) and LDHMgAl@SCGB as post-calcination of LDHMgAl@SCGB enhanced the charge properties (surface zeta potential at pH 7.0: SCGB = -21.8 mV, LDHMgAl@SCGB = 28.5 mV, and PLDHMgAl@SCGB = 34.4 mV) and increased active sites by eliminating the anions (i.e., Cl- ions) and water molecules at its interlayers. The calculated kinetic, intra-particle diffusion, and isotherm parameters indicated that the chemisorption and intra-particle diffusion were mainly responsible for the adsorption of AsV and SbV by SCGB, LDHMgAl@SCGB, and PLDHMgAl@SCGB. Moreover, post-calcination of LDHMgAl@SCGB enhanced its selectivity toward AsV and SbV by reinforcing the electrostatic surface complexation via its improvement of charge properties. Since PLDHMgAl@SCGB exhibited the excellent reusability for the adsorption of AsV (reuse efficiency >63.6%) and SbV (reuse efficiency >52.1%), it can be concluded that post-calcination of LDHMgAl@SCGB is a promising method for improving the adsorption capacities for AsV and SbV in real water matrices.

20.
Food Chem ; 461: 140915, 2024 Dec 15.
Artículo en Inglés | MEDLINE | ID: mdl-39181055

RESUMEN

The excessive use of nitrofurantoin (NFT) represents a threat to ecosystems and food safety, making it necessary to develop efficient and accurate detection methods. Herein, the Ru/NiFe-LDH-MXene/SPCE electrode was successfully synthesized by one-step electrodeposition and employed to the NFT electrochemical sensing. Combining 2D MXenes with multifunctional 2D layered double hydroxides (LDHs) creates synergistic interactions within the MXene-LDH heterostructures, modifying the electrochemical performance. Furthermore, the incorporation of noble metal nanoparticles and nanoclusters can significantly enhance electrochemical performance by promoting favorable interactions at the metal-carrier interface and optimizing the rearrangement of electronic structure. Based on this, the developed Ru/NiFe-LDH-MXene/SPCE sensor demonstrates remarkable sensitivity (152.44 µA µM-1 cm-2) and an ultralow detection limit (2.2 nM). Notably, the sensor was employed for NFT detection in food samples with satisfactory recoveries, making it a promising electrochemical sensor for the detection of NFT.


Asunto(s)
Técnicas Electroquímicas , Contaminación de Alimentos , Nanopartículas del Metal , Nitrofurantoína , Rutenio , Técnicas Electroquímicas/instrumentación , Contaminación de Alimentos/análisis , Nitrofurantoína/análisis , Nitrofurantoína/química , Nanopartículas del Metal/química , Rutenio/química , Límite de Detección , Hidróxidos/química , Electrodos , Níquel/química
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