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1.
Int J Mol Sci ; 25(12)2024 Jun 09.
Article in English | MEDLINE | ID: mdl-38928099

ABSTRACT

Cobalt-aluminum-layered double hydroxides containing carboxymethyl ß-cyclodextrin (CMßCD) were synthesized by coprecipitation and evaluated as a cobalt source for the 4-nitrophenol reduction in an aqueous medium. Several physicochemical techniques (XRD, FTIR, TGA) indicated the intercalation of the anionic cyclodextrin without damages to the hydrotalcite-type structure. These lamellar cobalt-aluminum hybrid materials (CoAl_CMßCD) were evaluated in the 4-nitrophenol reduction and showed higher activities in comparison with the CMßCD-free standard material (CoAl_CO3). To rationalize these results, a set of experimental controls going from physical mixtures of CoAl_CO3 with different cyclodextrins to other cobalt-based materials were investigated, highlighting the beneficial effects of both the layered double hydroxide and CMßCD-based hybrid structures. CMßCD also showed a beneficial effect as an additive during the 4-nitrophenol reduction. CoAl_CO3, dispersed in a fresh CMßCD solution could be re-used for five successive cycles without the loss of activity.


Subject(s)
Cobalt , Hydroxides , Nitrophenols , Oxidation-Reduction , beta-Cyclodextrins , Nitrophenols/chemistry , Cobalt/chemistry , beta-Cyclodextrins/chemistry , Hydroxides/chemistry , Catalysis , X-Ray Diffraction , Spectroscopy, Fourier Transform Infrared
2.
ACS Appl Mater Interfaces ; 16(25): 31936-31949, 2024 Jun 26.
Article in English | MEDLINE | ID: mdl-38869429

ABSTRACT

Minimally invasive embolization greatly decreases the mortality resulting from vascular injuries while still suffering from a high risk of recanalization and systematic thrombosis due to the intrinsic hydrophobicity and poor adhesion of the clinically used liquid embolic agent of Lipiodol. In this study, a shape self-adaptive liquid embolic agent was developed by mixing biocompatible poly(acrylic acid) (PAA), two-dimensional magnesium-aluminum layered double hydroxide (LDH), and poly(ethylene glycol)200 (PEG200). Upon contact with blood, the injectable PAA-LDH@PEG200 would quickly absorb water to form an adhesive and mechanically strong PAA-LDH thin hydrogel within 5 s, which could firmly adhere to the blood vessel wall for ultrafast and durable embolization. In addition, benefiting from the "positively charged nucleic center effect" of LDH nanosheets, the liquid PAA-LDH@PEG200 could avoid vascular distension by PAA overexpansion and possess high shock-resistant mechanical strength from the blood flow. Furthermore, both in vitro and in vivo embolization experiments demonstrated the complete embolic capacity of liquid PAA-LDH@PEG200 without the occurrence of recanalization for 28 days and also the great potential to act as a platform to couple with chemotherapeutic drugs for the minimized transcatheter arterial chemoembolization (TACE) treatment of VX2 tumors without recurrence for 18 days. Thus, liquid PAA-LDH@PEG200 developed here possesses great potential to act as a shape self-adaptive liquid embolic agent for ultrafast and durable vascular embolization.


Subject(s)
Polyethylene Glycols , Animals , Polyethylene Glycols/chemistry , Mice , Acrylic Resins/chemistry , Embolization, Therapeutic/methods , Humans , Hydroxides/chemistry , Hydroxides/pharmacology , Hydrogels/chemistry , Hydrogels/pharmacology , Aluminum/chemistry
3.
ACS Sens ; 9(6): 3444-3454, 2024 Jun 28.
Article in English | MEDLINE | ID: mdl-38847105

ABSTRACT

Programmed death ligand-1 (PD-L1)-expressing exosomes are considered a potential marker for diagnosis and classification of lung adenocarcinoma (LUAD). There is an urgent need to develop highly sensitive and accurate chemiluminescence (CL) immunosensors for the detection of PD-L1-expressing exosomes. Herein, N-(4-aminobutyl)-N-ethylisopropanol-functionalized nickel-cobalt hydroxide (NiCo-DH-AA) with a hollow nanoflower structure as a highly efficient CL nanoprobe was synthesized using gold nanoparticles as a "bridge". The resulting NiCo-DH-AA exhibited a strong and stable CL emission, which was ascribed to the exceptional catalytic capability and large specific surface area of NiCo-DH, along with the capacity of AuNPs to facilitate free radical generation. On this basis, an ultrasensitive sandwich CL immunosensor for the detection of PD-L1-expressing exosomes was constructed by using PD-L1 antibody-modified NiCo-DH-AA as an effective signal probe and rabbit anti-CD63 protein polyclonal antibody-modified carboxylated magnetic bead as a capture platform. The immunosensor demonstrated outstanding analytical performance with a wide detection range of 4.75 × 103-4.75 × 108 particles/mL and a low detection limit of 7.76 × 102 particles/mL, which was over 2 orders of magnitude lower than the reported CL method for detecting PD-L1-expressing exosomes. Importantly, it was able to differentiate well not only between healthy persons and LUAD patients (100% specificity and 87.5% sensitivity) but also between patients with minimally invasive adenocarcinoma and invasive adenocarcinoma (92.3% specificity and 52.6% sensitivity). Therefore, this study not only presents an ultrasensitive and accurate diagnostic method for LUAD but also offers a novel, simple, and noninvasive approach for the classification of LUAD.


Subject(s)
Adenocarcinoma of Lung , B7-H1 Antigen , Cobalt , Exosomes , Lung Neoplasms , Nickel , Humans , Nickel/chemistry , Cobalt/chemistry , B7-H1 Antigen/analysis , Adenocarcinoma of Lung/diagnosis , Adenocarcinoma of Lung/immunology , Lung Neoplasms/diagnosis , Exosomes/chemistry , Immunoassay/methods , Hydroxides/chemistry , Metal Nanoparticles/chemistry , Biosensing Techniques/methods , Gold/chemistry , Luminescent Measurements/methods , Limit of Detection
4.
J Environ Manage ; 362: 121338, 2024 Jun.
Article in English | MEDLINE | ID: mdl-38823296

ABSTRACT

A series of Fe3O4@CuCr-LDH hybrids decorated with different amount of ZIF-8 (FLZ, 10-40 wt%) was prepared using simple methods and characterized with different techniques. The activity of the synthesized nanocomposites was investigated in the sonocatalytic degradation of tetracycline (TC) antibiotic from wastewater. When the content of ZIF-8 in the nanocomposite structure was 20 wt%, the FLZ-20 sonocatalyst exhibited the high performance in the sonocatalytic removal of TC. At optimum conditions (0.7 g/L catalyst dosage, pH of 7, 50 mg/L initial concentration of antibiotic, and 15 min sonication time) of the sonocatalytic removal of TC approached to 91.4% under ultrasonic irradiation (USI) using FLZ-20. This efficiency was much higher than those of obtained results by Fe3O4@CuCr-LDH and pristine ZIF-8. The formed ●OH and ●O2- exhibited the major roles in the sonocatalytic TC degradation process. The excellent performance of FLZ-20 can be attributed to the heterojunctions created between composite components, which could improve the electron transfer ability and effectively separate e-/h+ pairs. In addition, FLZ-20 showed the superior reusability and stability during three successive recycling. Moreover, the facile magnetically separation of the sonocatalyst from the aqueous solution was another outstanding feature, which prevents the formation of secondary pollutants. It can be concluded that the fabrication of heterojunctions is an efficient procedure to promote the sonocatalytic acting of the catalyst.


Subject(s)
Tetracycline , Tetracycline/chemistry , Catalysis , Hydroxides/chemistry , Wastewater/chemistry , Nanocomposites/chemistry , Water Pollutants, Chemical/chemistry
5.
J Nanobiotechnology ; 22(1): 317, 2024 Jun 08.
Article in English | MEDLINE | ID: mdl-38849886

ABSTRACT

Sonodynamic therapy (SDT), a promising strategy for cancer treatment with the ability for deep tissue penetration, has received widespread attention in recent years. Sonosensitizers with intrinsic characteristics for tumor-specific curative effects, tumor microenvironment (TME) regulation and tumor diagnosis are in high demand. Herein, amorphous CoBiMn-layered double hydroxide (a-CoBiMn-LDH) nanoparticles are presented as multifunctional sonosensitizers to trigger reactive oxygen species (ROS) generation for ultrasound (US) imaging-guided SDT. Hydrothermal-synthesized CoBiMn-LDH nanoparticles are etched via a simple acid treatment to obtain a-CoBiMn-LDH nanoparticles with abundant defects. The a-CoBiMn-LDH nanoparticles give greater ROS generation upon US irradiation, reaching levels ~ 3.3 times and ~ 8.2 times those of the crystalline CoBiMn-LDH nanoparticles and commercial TiO2 sonosensitizer, respectively. This excellent US-triggered ROS generation performance can be attributed to the defect-induced narrow band gap and promoted electrons and holes (e-/h+) separation. More importantly, the presence of Mn4+ enables the a-CoBiMn-LDH nanoparticles to regulate the TME by decomposing H2O2 into O2 for hypoxia relief and US imaging, and consuming glutathione (GSH) for protection against ROS clearance. Biological mechanism analysis shows that a-CoBiMn-LDH nanoparticles modified with polyethylene glycol can serve as a multifunctional sonosensitizer to effectively kill cancer cells in vitro and eliminate tumors in vivo under US irradiation by activating p53, apoptosis, and oxidative phosphorylation-related signaling pathways.


Subject(s)
Hydroxides , Nanoparticles , Reactive Oxygen Species , Tumor Microenvironment , Ultrasonic Therapy , Tumor Microenvironment/drug effects , Animals , Reactive Oxygen Species/metabolism , Humans , Ultrasonic Therapy/methods , Hydroxides/chemistry , Hydroxides/pharmacology , Mice , Nanoparticles/chemistry , Cell Line, Tumor , Cobalt/chemistry , Ultrasonography/methods , Mice, Inbred BALB C , Neoplasms/therapy , Neoplasms/diagnostic imaging , Apoptosis/drug effects , Female , Mice, Nude
6.
Langmuir ; 40(25): 12939-12953, 2024 Jun 25.
Article in English | MEDLINE | ID: mdl-38861462

ABSTRACT

In this study, magnetic inulin/Mg-Zn-Al layered double hydroxide (MILDH) was synthesized for the adsorption of ciprofloxacin. The application of various analytical techniques confirmed the successful formation of MILDH. For the optimization of controllable factors, Taguchi design was applied and optimum values were obtained as equilibrium time─100 min, adsorbent dose─20 mg, and ciprofloxacin concentration─30 mg/L. The highest capacity of the material was recorded as 196.19 mg/g at 298 K. Langmuir model (R2 = 0.9669-0.9832) fitted best as compared to the Freundlich model (R2 = 0.9588-0.9657), concluded the monolayer adsorption of ciprofloxacin on MILDH. Statistical physics model M 2 was found to fit best to measured data (R2 = 0.9982-0.9989), indicating that the binding of ciprofloxacin took place on two types of receptor sites (n1 and n2). The multidocking mechanism with horizontal position was suggested on the first receptor site (n1 < 1), while multimolecular adsorption of ciprofloxacin lying vertically on the second receptor site (n2 > 1) at all temperatures. The adsorption energies (E1 = 22.79-27.20 kJ/mol; E2 = 18.00-19.46 kJ/mol) illustrated that the adsorption of ciprofloxacin onto MILDH occurred through physical forces. Best fitting of the fractal-like pseudo-first-order kinetic model (R2 = 0.9982-0.9992) indicated that the adsorption of ciprofloxacin happened on the MILDH surface having different energies. X-ray photoelectron spectroscopy analysis further confirmed the adsorption mechanism of ciprofloxacin onto MILDH.


Subject(s)
Ciprofloxacin , Inulin , Zinc , Ciprofloxacin/chemistry , Adsorption , Inulin/chemistry , Zinc/chemistry , Hydroxides/chemistry , Magnesium/chemistry , Aluminum/chemistry , Kinetics , Surface Properties
7.
Nature ; 630(8017): 654-659, 2024 Jun.
Article in English | MEDLINE | ID: mdl-38839965

ABSTRACT

Emissions reduction and greenhouse gas removal from the atmosphere are both necessary to achieve net-zero emissions and limit climate change1. There is thus a need for improved sorbents for the capture of carbon dioxide from the atmosphere, a process known as direct air capture. In particular, low-cost materials that can be regenerated at low temperatures would overcome the limitations of current technologies. In this work, we introduce a new class of designer sorbent materials known as 'charged-sorbents'. These materials are prepared through a battery-like charging process that accumulates ions in the pores of low-cost activated carbons, with the inserted ions then serving as sites for carbon dioxide adsorption. We use our charging process to accumulate reactive hydroxide ions in the pores of a carbon electrode, and find that the resulting sorbent material can rapidly capture carbon dioxide from ambient air by means of (bi)carbonate formation. Unlike traditional bulk carbonates, charged-sorbent regeneration can be achieved at low temperatures (90-100 °C) and the sorbent's conductive nature permits direct Joule heating regeneration2,3 using renewable electricity. Given their highly tailorable pore environments and low cost, we anticipate that charged-sorbents will find numerous potential applications in chemical separations, catalysis and beyond.


Subject(s)
Carbon Dioxide , Carbon Dioxide/analysis , Carbon Dioxide/chemistry , Carbon Dioxide/isolation & purification , Adsorption , Electrodes , Hydroxides/chemistry , Atmosphere/chemistry , Carbonates/chemistry , Air , Temperature , Charcoal/chemistry , Porosity , Carbon/chemistry
8.
J Chromatogr A ; 1729: 465035, 2024 Aug 16.
Article in English | MEDLINE | ID: mdl-38851029

ABSTRACT

This work presents the development, synthesis, and application of a layered double hydroxide (LDH) coupled to magnetic particles for the removal of antibiotics as tetracyclines (TC´s): tetracycline (TC), chlortetracycline (CT), oxytetracycline (OT), and doxycycline (DT) from milk samples. The LDH synthesis conditions, reaction time (30-90 min), molar ratios Mg2+/Al3+ (7:1-1:7), interlayer anion (NO3-, Cl-, CO32-, and dodecyl sulphate (DS-)) were evaluated. Under synthesis conditions (reaction time of 30 min, Mg2+/Al3+ molar ratio of 7:1, and DS- as interlayer anion), the LDH was coupled in a magnetic solid phase microextraction (MSPµE) methodology. At the optimal extraction conditions (pH 6, 5 min of contact time, 10 mg of adsorbent), a removal percentage of 99.0 % was obtained for each tetracycline. FTIR, TGA, SEM, and adsorption isotherms were employed to characterize the optimal adsorbent. Each experiment was corroborated by large-volume sample stacking capillary electrophoresis (LVSS-CE). The adsorbent was applied directly to positive milk samples (previously tested) for TC´s removal.


Subject(s)
Hydroxides , Milk , Tetracyclines , Milk/chemistry , Animals , Tetracyclines/isolation & purification , Tetracyclines/analysis , Tetracyclines/chemistry , Hydroxides/chemistry , Adsorption , Solid Phase Microextraction/methods , Anti-Bacterial Agents/isolation & purification , Anti-Bacterial Agents/chemistry , Anti-Bacterial Agents/analysis , Silicon Dioxide/chemistry
9.
Article in English | MEDLINE | ID: mdl-38851151

ABSTRACT

In this study, a magnetic three-dimensional nano-composite based on Rubber-Fe3O4@Ni-Co Layered double hydroxide derived from ZIF-67 template was synthesized by a hydrothermal method. The proposed nano-composite was used as a sorbent for the enrichment of trace amounts of anti-cancer drugs (dasatinib and erlotinib hydrochloride) from plasma samples followed by determination using high-performance liquid chromatographic analysis (HPLC-UV). The synthesized nano-sorbent was characterized by X-ray diffraction, field emission scanning electron microscopy, Fourier transform infrared spectroscopy, vibrating-sample magnetometer, Brunauer-Emmett-Teller surface analysis, Barrett-Joyner-Halenda pore size analysis and energy dispersive X-ray spectroscopy. Under optimal experimental conditions, factors affecting on extraction efficiency such as pH, ionic strength, extraction temperature and time, desorption solvent and time, the limit of detection (LODs) and the limit of quantification (LOQs) were obtained as 0.6, 2 µg/L for both of dasatinib and erlotinib, respectively. Also, linear range of the method were 2-500 and 2-1000 µg/L for dasatinib and erlotinib, respectively. Relative standard deviations (RSD%) for the repeatability of extraction on sorbent to sorbent were obtained as 3.59, 1.97 %, and one sorbent reusability were investigated and relative standard deviation values were obtained 5.35, 3.30 % for dasatinib and erlotinib, respectively.


Subject(s)
Antineoplastic Agents , Erlotinib Hydrochloride , Limit of Detection , Rubber , Rubber/chemistry , Antineoplastic Agents/blood , Antineoplastic Agents/chemistry , Chromatography, High Pressure Liquid/methods , Reproducibility of Results , Humans , Erlotinib Hydrochloride/blood , Erlotinib Hydrochloride/chemistry , Linear Models , Dasatinib/blood , Dasatinib/chemistry , Hydroxides/chemistry , Imidazoles/chemistry , Imidazoles/blood , Adsorption , Solid Phase Extraction/methods , Cobalt/chemistry , Cobalt/blood , Nanostructures/chemistry , Zeolites
10.
Environ Sci Technol ; 58(24): 10696-10705, 2024 Jun 18.
Article in English | MEDLINE | ID: mdl-38845125

ABSTRACT

Because ozone (O3) is a significant air pollutant, advanced O3 elimination technologies, particularly those under high-humidity conditions, have become an essential research focus. In this study, a nickel-iron layered double hydroxide (NiFe-LDH) was modified via intercalation with octanoate to develop an effective hydrophobic catalyst (NiFe-OAa-LDH) for O3 decomposition. The NiFe-OAa-LDH catalyst sustained its O3 decomposition rate of >98% for 48 h under conditions of 90% relative humidity, 840 L/(g·h) space velocity, and 100 ppm inlet O3 concentration. Moreover, it maintained a decomposition rate of 90% even when tested at a higher airflow rate of 2500 L/(g·h). Based on the changes induced by the Ni-OII to Ni-OIII bonds in NiFe-OAa-LDH during O3 treatment, catalytic O3 decomposition was proposed to occur in two stages. The first stage involved the reaction between the hydroxyl groups and O3, leading to the breakage of the O-H bonds, formation of NiOOH, and structural changes in the catalyst. This transformation resulted in the formation of abundant and stable hydrogen vacancies. According to density functional theory calculations, O3 can be effectively decomposed at the hydrogen vacancies with a low energy barrier during the second stage. This study provides new insights into O3 decomposition.


Subject(s)
Hydroxides , Ozone , Hydroxides/chemistry , Ozone/chemistry , Nickel/chemistry , Catalysis , Air Pollutants/chemistry
11.
Chemosphere ; 361: 142554, 2024 Aug.
Article in English | MEDLINE | ID: mdl-38851502

ABSTRACT

Increasing multidrug-resistant pathogenic microbial around the world become a global problem, making it imperative to develop effective methods for bacterial inactivation in wastewater. In this study, we propose a multifunctional photoelectrochemical (PEC) system to successfully disinfect microbial cells and degrade orange (II) dyes. CoOx NP were synthesized by spin-coating onto hydrothermally synthesized TiO2 nanorod arrays followed by electrodeposited NiFe-LDH to develop the NiFe-LDH/CoOx NP-TiO2 NRs. Interestingly, spin-coated CoOx NP-TiO2 NRs exhibited a 1.5-fold enhancement in photocurrent (1.384 mA/cm2) than pristine TiO2 NRs (0.92 mA/cm2). A NiFe-layered double hydroxide (LDH) cocatalysts layer further exhibits the maximum photocurrent density of 1.64 mA/cm2 with IPCE of 84.5% at 1.0 VAg/AgCl at 380 nm. Furthermore, NiFe-LDH/CoOx-TiO2 NR photoanodes were effectually employed for photoelectrochemical bacteria disinfection and organic pollutant removals. With NiFe-LDH/CoOx-TiO2 NR, 99% (120 min) bacterial inactivation and 99% (60 min) orange II dye decomposition efficiency was achieved. Superoxide radicals (-O2•), hydroxyl radicals (HO•), and holes (h+) played a critical role in the PEC degradation systems. Due to the synergy between NiFe-LDH cocatalyst and CoOx interlayer, surface water oxidation reactions were accelerated over NiFe-LDH/CoOx NP-TiO2 NRs. The charge transport process in NiFe-LDH/CoOx NP-TiO2 NRs photoanode-based PEC system was proposed in detail.


Subject(s)
Electrodes , Titanium , Wastewater , Titanium/chemistry , Wastewater/chemistry , Catalysis , Electrochemical Techniques/methods , Water Pollutants, Chemical/chemistry , Hydroxides/chemistry , Waste Disposal, Fluid/methods , Photochemical Processes , Nanotubes/chemistry , Coloring Agents/chemistry , Azo Compounds/chemistry , Water Purification/methods , Disinfection/methods
12.
Environ Sci Technol ; 58(23): 10378-10387, 2024 Jun 11.
Article in English | MEDLINE | ID: mdl-38805367

ABSTRACT

Room temperature catalytic oxidation (RTCO) using non-noble metals has emerged as a highly promising technique for removal of formaldehyde (HCHO) under ambient conditions; however, non-noble catalysts still face the challenges related to poor water resistance and low stability under harsh conditions. In this study, we synthesized a series of layered double hydroxides (LDHs) incorporating various dual metals (MgAl, ZnAl, NiAl, NiFe, and NiTi) for formaldehyde oxidation at ambient temperature. Among the synthesized catalysts, the NiTi-LDH catalyst showed an HCHO removal efficiency and CO2 yield close to 100.0%, and exceptional water resistance and chemical stability on running 1300 min. The abundant hydroxyl groups in LDHs directly bonded with HCHO, leading to the production of CO2 and H2O, thus inhibiting the formation of CO, even in the absence of O2 and H2O. The coexistence of O2 effectively reduced the reaction barrier for H2O molecule dissociation, facilitating the formation of hydroxyl groups and their subsequent backfill on the catalyst surface. The mechanisms underlying the involvement and regeneration of hydroxyl groups in room temperature oxidation of formaldehyde were elucidated with the combined in situ DRIFTS, HCHO-TPD-MS, and DFT calculations. This work not only demonstrates the potential of LDH catalysts in environmental applications but also advances the understanding of the fundamental processes involved in room temperature oxidation of formaldehyde.


Subject(s)
Formaldehyde , Hydroxides , Oxidation-Reduction , Temperature , Formaldehyde/chemistry , Hydroxides/chemistry , Catalysis
13.
Int J Biol Macromol ; 269(Pt 1): 132122, 2024 Jun.
Article in English | MEDLINE | ID: mdl-38718992

ABSTRACT

In the treatment of bowel diseases such as ulcerative colitis through oral administration, an effective drug delivery system targeting the colon is crucial for enhancing efficacy and minimizing side effects of therapeutic agents. This study focuses on the development of a novel nanocomposite hydrogel bead comprising a synergistic blend of biological macromolecules, namely sodium alginate (ALG) and hyaluronic acid (HA), reinforced with layered double hydroxide nanoparticles (LDHs) for the oral delivery of dual therapeutics. The synthesized hydrogel bead exhibits significantly enhanced gel strength and controllable release of methylprednisolone (MP) and curcumin (CUR), serving as an anti-inflammatory drug and a mucosal healing agent, compared to native ALG or ALG/HA hydrogel beads without LDHs. The physicochemical properties of the synthesized LDHs and hydrogel beads were characterized using various techniques, including scanning electron microscopy, zeta potential measurement, transmission electron microscopy, X-ray diffraction, and energy-dispersive X-ray spectroscopy. In vitro release studies of MP and CUR under simulated gastrointestinal tract (GIT) conditions demonstrate the superior controlled release property of the nanocomposite hydrogel bead, particularly in minimizing premature drug release in the upper GIT environment while sustaining release of over 82 % of drugs in the colonic environment. Thus, the modularly engineered carrier designed for oral colon targeting holds promise as a potential candidate for the treatment of ulcerative colitis.


Subject(s)
Alginates , Drug Liberation , Hyaluronic Acid , Hydrogels , Nanoparticles , Alginates/chemistry , Hyaluronic Acid/chemistry , Hydrogels/chemistry , Nanoparticles/chemistry , Administration, Oral , Drug Carriers/chemistry , Humans , Hydroxides/chemistry , Curcumin/chemistry , Curcumin/administration & dosage , Curcumin/pharmacology , Methylprednisolone/chemistry , Methylprednisolone/administration & dosage , Drug Delivery Systems , Colitis, Ulcerative/drug therapy
14.
Inorg Chem ; 63(23): 10691-10704, 2024 Jun 10.
Article in English | MEDLINE | ID: mdl-38805682

ABSTRACT

As the main challenge of dental healthcare, oral infectious diseases are highly associated with the colonization of pathogenic microbes. However, current antibacterial treatments in the field of stomatology still lack a facile, safe, and universal approach. Herein, we report the controllable synthesis of copper aluminum-layered double hydroxides (CuAl-LDHs) with high Fenton-like catalytic activity, which can be utilized in the treatment of oral infectious diseases with negligible side effects. Our strategy can efficiently avoid the unwanted doping of other divalent metal ions in the synthesis of Cu-contained LDHs and result in the formation of binary CuAl-LDHs with high crystallinity and purity. Evidenced by experimental and theoretical results, CuAl-LDHs exhibit excellent catalytic ability toward the ·OH generation in the presence of H2O2 and hold strong affinity toward bacteria, endowing them with great catalytic sterilization against both Gram-positive and Gram-negative bacteria. As expected, these CuAl-LDHs provide outstanding treatments for mucosal infection and periodontitis by promoting wound healing and remodeling of the periodontal microenvironment. Moreover, toxicity investigation demonstrates the overall safety. Accordingly, the current study not only provides a convenient and economic strategy for treating oral infectious diseases but also extends the development of novel LDH-based Fenton or Fenton-like antibacterial reagents for further biomedical applications.


Subject(s)
Aluminum , Anti-Bacterial Agents , Copper , Hydrogen Peroxide , Copper/chemistry , Copper/pharmacology , Catalysis , Anti-Bacterial Agents/pharmacology , Anti-Bacterial Agents/chemistry , Anti-Bacterial Agents/chemical synthesis , Hydrogen Peroxide/chemistry , Hydrogen Peroxide/pharmacology , Aluminum/chemistry , Aluminum/pharmacology , Hydroxides/chemistry , Hydroxides/pharmacology , Microbial Sensitivity Tests , Animals , Iron/chemistry , Iron/pharmacology , Oral Health , Mice , Humans , Gram-Negative Bacteria/drug effects
15.
J Agric Food Chem ; 72(20): 11381-11391, 2024 May 22.
Article in English | MEDLINE | ID: mdl-38728113

ABSTRACT

RNA interference (RNAi)-based biopesticides offer an attractive avenue for pest control. Previous studies revealed high RNAi sensitivity in Holotrichia parallela larvae, showcasing its potential for grub control. In this study, we aimed to develop an environmentally friendly RNAi method for H. parallela larvae. The double-stranded RNA (dsRNA) of the V-ATPase-a gene (HpVAA) was loaded onto layered double hydroxide (LDH). The dsRNA/LDH nanocomplex exhibited increased environmental stability, and we investigated the absorption rate and permeability of dsRNA-nanoparticle complexes and explored the RNAi controlling effect. Silencing the HpVAA gene was found to darken the epidermis of H. parallela larvae, with growth cessation or death or mortality, disrupting the epidermis and midgut structure. Quantitative reverse transcription-polymerase chain reaction and confocal microscopy confirmed the effective absorption of the dsRNA/LDH nanocomplex by peanut plants, with distribution in roots, stems, and leaves. Nanomaterial-mediated RNAi silenced the target genes, leading to the death of pests. Therefore, these findings indicate the successful application of the nanomaterial-mediated RNAi system for underground pests, thus establishing a theoretical foundation for developing a green, safe, and efficient pest control strategy.


Subject(s)
Larva , RNA Interference , RNA, Double-Stranded , Animals , Larva/growth & development , Larva/genetics , RNA, Double-Stranded/genetics , RNA, Double-Stranded/metabolism , Hydroxides/chemistry , Hydroxides/metabolism , Vacuolar Proton-Translocating ATPases/genetics , Vacuolar Proton-Translocating ATPases/metabolism , Vacuolar Proton-Translocating ATPases/chemistry , Arachis/genetics , Arachis/chemistry , Arachis/growth & development , Arachis/metabolism , Pest Control, Biological , Coleoptera/genetics , Coleoptera/growth & development , Green Chemistry Technology , Biological Control Agents/chemistry , Biological Control Agents/metabolism , Nanoparticles/chemistry
16.
Water Res ; 258: 121744, 2024 Jul 01.
Article in English | MEDLINE | ID: mdl-38754301

ABSTRACT

Replacing petroleum-based plastics with biodegradable polymers is a major challenge for modern society especially for food packaging applications. To date, poly(lactic acid) represents 25 % of the total biodegradable plastics and it is estimated that, in the future, it could become the main contributor to the biodegradable plastics industry. Anaerobic digestion is an interesting way for the poly(lactic acid) end of life, even if its biodegradability is limited in mesophilic conditions. The aims of this study were to identify the best pre-treatment for maximizing the methane yield, minimizing the anaerobic digestion duration and limiting residual plastic fragments in the digestate. A systematic comparison was carried out between thermal, chemical, and thermo-chemical pre-treatment. Pre-treatment with 4 M KOH for 48 h at 35°C was effective in improving the mesophilic anaerobic digestion of the poly(lactic acid). Such pre-treatment allows obtaining 90 % of the theoretical methane potential, in 24 - 30 days. Importantly, such pre-treatment completely solubilized the poly(lactic acid), leaving no solid residues in the digestate. In addition, using KOH permits to avoid the sodication of the soil due to the digestate application as fertilizer.


Subject(s)
Polyesters , Polyesters/chemistry , Anaerobiosis , Polymers/chemistry , Methane/metabolism , Lactic Acid/metabolism , Alkalies/chemistry , Hydroxides/chemistry , Potassium Compounds/chemistry , Biodegradation, Environmental , Temperature
17.
J Contam Hydrol ; 264: 104364, 2024 May.
Article in English | MEDLINE | ID: mdl-38749070

ABSTRACT

The increase in antibiotic residues poses a serious threat to ecological and aquatic environments, necessitating the development of cost-effective, convenient, and recyclable adsorbents. In our study, we used cellulose-based layered double hydroxide (LDH) as an efficient adsorbent and nanocarrier for both sulfamethoxazole (SMX) and cefixime (CFX) residues due to their biodegradability and biocompatibility. Chemical processes are measured according to green chemistry metrics to identify which features adhere to the principles. A GREEnness Assessment (ESA), Analytical GREEnness Preparation (AGREEprep), and Analytical Eco-Scale Assessments (ESA) were used to assess the suitability of the proposed analytical method. We extensively analyzed the synthesized CoFe LDH/cellulose before and after the adsorption processes using XRD, FTIR, and SEM. We investigated the factors affecting the adsorption process, such as pH, adsorbent dose, concentrations of SMX and CFX and time. We studied six nonlinear adsorption isotherm models at pH 5 using CoFe LDH, which showed maximum adsorption capacities (qmax) of 272.13 mg/g for SMX and 208.00 mg/g for CFX. Kinetic studies were also conducted. The 3-(4,5-dimethylthiazol-2-yl)-2,5-diphenyl-2H-tetrazolium bromide (MTT) assay was performed on Vero cells in direct contact with LDH nanocomposites to evaluate the cytotoxicity and side effects of cellulose-based CoFe LDH. The cellulose-based CoFe LDH nanocomposite demonstrated excellent cytocompatibility and less cytotoxic effects on the tested cell line. These results validate the potential use of these unique LDH-based cellulose cytocompatible biomaterials for water treatment applications. The cost of the prepared adsorbents was investigated.


Subject(s)
Cefixime , Cellulose , Sulfamethoxazole , Water Pollutants, Chemical , Cellulose/chemistry , Sulfamethoxazole/chemistry , Sulfamethoxazole/toxicity , Adsorption , Water Pollutants, Chemical/chemistry , Water Pollutants, Chemical/toxicity , Animals , Cefixime/chemistry , Anti-Bacterial Agents/chemistry , Anti-Bacterial Agents/toxicity , Vero Cells , Hydroxides/chemistry , Chlorocebus aethiops , Nanocomposites/chemistry , Nanocomposites/toxicity , Green Chemistry Technology/methods
18.
Chemosphere ; 359: 142228, 2024 Jul.
Article in English | MEDLINE | ID: mdl-38705407

ABSTRACT

Copper oxides are vital catalysts in facilitating the formation of polychlorinated thianthrenes/dibenzothiophenes (PCTA/DTs) through heterogeneous reactions in high-temperature industrial processes. Chlorothiophenols (CTPs) are the most crucial precursors for PCTA/DT formation. The initial step in this process is the metal-catalyzed production of chlorothiophenoxy radicals (CTPRs) from CTPs via dissociation reactions. This work combines density functional theory (DFT) calculations with ab initio molecular dynamics (AIMD) simulations to explore the formation mechanism of the adsorbed 2-CTPR from 2-CTP, with the assistance of CuO(111). Our study demonstrates that flat adsorption configurations of 2-CTP on the CuO(111) surface are more stable than vertical configurations. The CuO(111) surface acts as a strong catalyst, facilitating the dissociation of 2-CTP into the adsorbed 2-CTPR. Surface oxygen vacancies enhance the adsorption of 2-CTP on the CuO(111) surface, while moderately suppressing the dissociation of 2-CTP. More importantly, water molecules and surface hydroxyl groups actively promote the dissociation of 2-CTP. Specifically, water directly participates in the reaction through "water bridge", enabling a barrier-free process. This research provides molecular-level insights into the heterogeneous generation of dioxins with the catalysis of metal oxides in fly ash from static and dynamic aspects, providing novel approaches for reducing dioxin emissions and establishing dioxin control strategies.


Subject(s)
Copper , Density Functional Theory , Copper/chemistry , Adsorption , Catalysis , Water/chemistry , Molecular Dynamics Simulation , Hydroxides/chemistry , Surface Properties , Sulfhydryl Compounds/chemistry
19.
Chemosphere ; 359: 142283, 2024 Jul.
Article in English | MEDLINE | ID: mdl-38734251

ABSTRACT

Polyvinyl chloride (PVC), known for its chemical stability and flame-retardant qualities, has many uses in various fields, such as pipes, electric wires, and cable insulation. Research has established its potential recovery as a fluidic fuel through pyrolysis, but the use of PVC pyrolysis oil, which is tainted by chlorine, is constrained by its low heat value and harmful environmental effects. This study engineered a layered double hydroxide (LDH) to tackle these challenges. The LDH facilitated dechlorination during PVC pyrolysis and bolstered thermal stability via cross-linking. During pyrolysis with LDH, PVC was transformed into carbon-rich precursors to sorbents. Chemical activation of these residues using KOH created sorbents with a specific surface area of 1495.4 m2 g⁻1, rendering them hydrophilic. These resulting sorbents displayed impressive adsorption capabilities, removing up to 486.79 mg g⁻1 of methylene blue and exhibiting the simultaneous removal of cations and anions.


Subject(s)
Coloring Agents , Hydroxides , Polyvinyl Chloride , Polyvinyl Chloride/chemistry , Hydroxides/chemistry , Adsorption , Coloring Agents/chemistry , Coloring Agents/isolation & purification , Potassium Compounds/chemistry , Water Pollutants, Chemical/chemistry , Methylene Blue/chemistry , Pyrolysis
20.
Chemosphere ; 359: 142318, 2024 Jul.
Article in English | MEDLINE | ID: mdl-38735495

ABSTRACT

The effective removal of micropollutants by water treatment technologies remains a significant challenge. Herein, we develop a CoFe layered double hydroxide (CoFeLDH) catalytic membrane for peroxymonosulfate (PMS) activation to achieve efficient micropollutant removal with improved mass transfer rate and reaction kinetics. This study found that the CoFeLDH membrane/PMS system achieved an impressive above 98% degradation of the probe chemical ranitidine at 0.1 mM of PMS including five more micropollutants (Sulfamethoxazole, Ciprofloxacin, Carbamazepine, Acetaminophen and Bisphenol A) at satisfactory level (above 80%). Moreover, significant improvements in water flux and antifouling properties were observed, marking the membrane as a specific advancement in the removal of membrane fouling in water purification technology. The membrane demonstrated consistent degradation efficiency for several micropollutants and across a range of pH (4-9) as well as different anionic environments, thereby showing it suitability for scale-up application. The key role of reactive species such as SO4•-, and O2• - radicals in the degradation process was elucidated. This is followed by the confirmation of the occurrence of redox cycling between Co and Fe, and the presence of CoOH+ that promotes PMS activation. Over the ten cycles, the membrane could be operated with a flux recovery of up to 99.8% and maintained efficient performance over 24 h continuous operation. Finally, the efficiency in degrading micropollutants, coupled with reduced metal leaching, makes the CoFeLDH membrane as a promising technology for application in water treatment.


Subject(s)
Hydroxides , Membranes, Artificial , Water Pollutants, Chemical , Water Purification , Water Purification/methods , Water Pollutants, Chemical/chemistry , Hydroxides/chemistry , Phenols/chemistry , Peroxides/chemistry , Benzhydryl Compounds/chemistry , Carbamazepine/chemistry , Ranitidine/chemistry , Acetaminophen/chemistry , Sulfamethoxazole/chemistry , Ciprofloxacin/chemistry , Catalysis , Cobalt/chemistry , Oxidation-Reduction
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