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1.
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
2.
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
3.
J Pharm Biomed Anal ; 245: 116161, 2024 Aug 01.
Article in English | MEDLINE | ID: mdl-38714135

ABSTRACT

In this study, Fe3O4@ZnCr-layered double hydroxide/zeolitic imidazolate frameworks-8 (MLDH/ZIF-8) magnetically functionalized composites were synthesized by co-precipitation and in situ growth based on the advantages of LDHs and ZIF-8 using Fe3O4 nanoparticles as a magnetic substrate to obtain adsorbents with excellent performance. Moreover, the composite was used for the efficient enrichment of flavonoids in Chinese herbal medicines. The internal structures and surface properties were characterized by SEM, Fourier transform infrared spectroscopy, X-ray diffraction and so on. MLDH/ZIF-8 exhibited a large specific surface area and good paramagnetic properties. The MLDH/ZIF-8 magnetic composite was used as a magnetic solid-phase extraction (MSPE) adsorbent, and a MLDH/ZIF-8 MSPE-pressurized capillary electrochromatography coupling method was developed for the separation and detection of flavonoids (luteolin, kaempferol and apigenin) in a sample of the Chinese herb Ohwia caudata (Thunberg) H. Ohashi. The relevant parameters affecting the extraction efficiency were optimized to determine the ideal conditions for MSPE. 5 mg of adsorbent in sample solution at pH 6, vortex extraction for 5 min, elution with 1.5 mL of ethyl acetate for 15 min. The method showed good linearity in the concentration range of 3-50 µg mL-1 with correlation coefficients of 0.9934-0.9981, and displayed a relatively LODs of 0.07-0.09 µg mL-1. The spiked recoveries of all analytes ranged from 84.5% to 122.0% with RSDs (n=3) between 4.5% and 7.7%. This method is straightforward and efficient, with promising potential in the separation and analysis of active ingredients in various Chinese herbal medicines.


Subject(s)
Drugs, Chinese Herbal , Flavonoids , Hydroxides , Solid Phase Extraction , Flavonoids/isolation & purification , Flavonoids/analysis , Flavonoids/chemistry , Solid Phase Extraction/methods , Hydroxides/chemistry , Drugs, Chinese Herbal/chemistry , Adsorption , Magnetite Nanoparticles/chemistry , Metal-Organic Frameworks/chemistry , Spectroscopy, Fourier Transform Infrared/methods
4.
Int J Nanomedicine ; 19: 4181-4197, 2024.
Article in English | MEDLINE | ID: mdl-38766656

ABSTRACT

Purpose: The committed differentiation fate regulation has been a difficult problem in the fields of stem cell research, evidence showed that nanomaterials could promote the differentiation of stem cells into specific cell types. Layered double hydroxide (LDH) nanoparticles possess the regulation function of stem cell fate, while the underlying mechanism needs to be investigated. In this study, the process of embryonic stem cells (ESCs) differentiate to neural progenitor cells (NPCs) by magnesium aluminum LDH (MgAl-LDH) was investigated. Methods: MgAl-LDH with diameters of 30, 50, and 100 nm were synthesized and characterized, and their effects on the cytotoxicity and differentiation of NPCs were detected in vitro. Dot blot and MeRIP-qPCR were performed to detect the level of m6A RNA methylation in nanoparticles-treated cells. Results: Our work displayed that LDH nanoparticles of three different sizes were biocompatible with NPCs, and the addition of MgAl-LDH could significantly promote the process of ESCs differentiate to NPCs. 100 nm LDH has a stronger effect on promoting NPCs differentiation compared to 30 nm and 50 nm LDH. In addition, dot blot results indicated that the enhanced NPCs differentiation by MgAl-LDH was closely related to m6A RNA methylation process, and the major modification enzyme in LDH controlled NPCs differentiation may be the m6A RNA methyltransferase METTL3. The upregulated METTL3 by LDH increased the m6A level of Sox1 mRNA, enhancing its stability. Conclusion: This work reveals that MgAl-LDH nanoparticles can regulate the differentiation of ESCs into NPCs by increasing m6A RNA methylation modification of Sox1.


Subject(s)
Cell Differentiation , Nanoparticles , Neural Stem Cells , Cell Differentiation/drug effects , Animals , Neural Stem Cells/drug effects , Neural Stem Cells/cytology , Neural Stem Cells/metabolism , Mice , Nanoparticles/chemistry , Methylation/drug effects , Hydroxides/chemistry , Hydroxides/pharmacology , Methyltransferases/metabolism , Methyltransferases/genetics , Particle Size , Embryonic Stem Cells/drug effects , Embryonic Stem Cells/cytology , Adenosine/pharmacology , Adenosine/chemistry , Adenosine/analogs & derivatives , Aluminum Hydroxide/chemistry , Aluminum Hydroxide/pharmacology , Magnesium Hydroxide/chemistry , Magnesium Hydroxide/pharmacology
5.
Int J Nanomedicine ; 19: 4199-4215, 2024.
Article in English | MEDLINE | ID: mdl-38766657

ABSTRACT

Background: Breast cancer is the most common cancer in women and one of the leading causes of cancer death worldwide. Ferroptosis, a promising mechanism of killing cancer cells, has become a research hotspot in cancer therapy. Simvastatin (SIM), as a potential new anti-breast cancer drug, has been shown to cause ferroptosis of cancer cells and inhibit breast cancer metastasis and recurrence. The purpose of this study is to develop a novel strategy boosting ferroptotic cascade for synergistic cancer therapy. Methods: In this paper, iron base form of layered double hydroxide supported simvastatin (LDHs-SIM) was synthesized by hydrothermal co-precipitation method. The characterization of LDHs-SIM were assessed by various analytical techniques, including ultraviolet-visible (UV-vis) spectroscopy, X-ray diffraction (XRD), Fourier transform infrared (FTIR) spectroscopy, and transmission electron microscopy (TEM). Biological activity, ferroptosis mechanism and biocompatibility were analyzed through in vivo and in vitro analysis, so as to evaluate its therapeutic effect on breast cancer. Results: The constructed LDHs-SIM nanosystem can not only release SIM through mevalonate (MVA) pathway, inhibit the expression of glutathione peroxidase 4 (GPX4), inhibit the expression of SLC7A11 and reduce the synthesis efficiency of GSH, but also promote the accumulation of Fe2+ in cells through the release of Fe3+, and increase the intracellular ROS content. In addition, LDHs-SIM nanosystem can induce apoptosis of breast cancer cells to a certain extent, and achieve the synergistic effect of apoptosis and ferroptosis. Conclusion: In the present study, we demonstrated that nanoparticles of layered double hydroxides (LDHs) loaded with simvastatin were more effective than a free drug at inhibiting breast cancer cell growth, In addition, superior anticancer therapeutic effects were achieved with little systemic toxicity, indicating that LDHs-SIM could serve as a safe and high-performance platform for ferroptosis-apoptosis combined anticancer therapy.


Subject(s)
Apoptosis , Breast Neoplasms , Ferroptosis , Hydroxides , Simvastatin , Ferroptosis/drug effects , Female , Humans , Breast Neoplasms/drug therapy , Breast Neoplasms/pathology , Breast Neoplasms/metabolism , Hydroxides/chemistry , Hydroxides/pharmacology , Simvastatin/pharmacology , Simvastatin/chemistry , Simvastatin/administration & dosage , Apoptosis/drug effects , Animals , Cell Line, Tumor , Nanoparticles/chemistry , Drug Synergism , Mice , Antineoplastic Agents/pharmacology , Antineoplastic Agents/chemistry , Mice, Nude , Mice, Inbred BALB C , MCF-7 Cells , Phospholipid Hydroperoxide Glutathione Peroxidase/metabolism
6.
J Vis Exp ; (206)2024 Apr 19.
Article in English | MEDLINE | ID: mdl-38709074

ABSTRACT

Utilizing vegetable oil as a sustainable feedstock, this study presents an innovative approach to ultrasonic-assisted transesterification for biodiesel synthesis. This alkaline-catalyzed procedure harnesses ultrasound as a potent energy input, facilitating the rapid conversion of extra virgin olive oil into biodiesel. In this demonstration, the reaction is run in an ultrasonic bath under ambient conditions for 15 min, requiring a 1:6 molar ratio of extra virgin olive oil to methanol and a minimum amount of KOH as the catalyst. The physiochemical properties of biodiesel are also reported. Emphasizing the remarkable advantages of ultrasonic-assisted transesterification, this method demonstrates notable reductions in reaction and separation times, achieving near-perfect purity (~100%), high yields, and negligible waste generation. Importantly, these benefits are achieved within a framework that prioritizes safety and environmental sustainability. These compelling findings underscore the effectiveness of this approach in converting vegetable oil into biodiesel, positioning it as a viable option for both research and practical applications.


Subject(s)
Biofuels , Plant Oils , Plant Oils/chemistry , Esterification , Hydroxides/chemistry , Olive Oil/chemistry , Ultrasonic Waves , Potassium Compounds/chemistry , Catalysis
7.
ACS Appl Mater Interfaces ; 16(19): 24295-24307, 2024 May 15.
Article in English | MEDLINE | ID: mdl-38697643

ABSTRACT

Pyroptosis has garnered increasing attention because of its ability to trigger robust antitumor immunity. Pyroptosis is initiated by the activation of inflammasomes, which are regulated by various organelles. The collaboration among organelles offers several protective mechanisms to prevent activation of the inflammasome, thereby limiting the induction of efficient pyroptosis. Herein, a multiorganelle homeostasis disruptor (denoted BLL) is constructed by encapsulating liposomes and bortezomib (BTZ) within a layered double hydroxide (LDH) nanocage to continuously activate inflammasomes for inducing efficient pyroptosis. In lysosomes, the negatively charged liposomes are released to recruit the NLRP3 inflammasomes through electrostatic interactions. ER stress is induced by BTZ to enhance the activation of the NLRP3 inflammasome. Meanwhile, the BLL nanocage exhibited H+-scavenging ability due to the weak alkalinity of LDH, thus disrupting the homeostasis of the lysosome and alleviating the degradation of the NLRP3 inflammasome by lysosomal-associated autophagy. Our results suggest that the BLL nanocage induces homeostatic imbalance in various organelles and efficient pyroptosis. We hope this work can provide new insights into the design of an efficient pyroptosis inducer by disrupting the homeostatic balance of multiple organelles and promote the development of novel antineoplastic platforms.


Subject(s)
Homeostasis , Inflammasomes , NLR Family, Pyrin Domain-Containing 3 Protein , Pyroptosis , Pyroptosis/drug effects , Inflammasomes/metabolism , Inflammasomes/drug effects , Homeostasis/drug effects , NLR Family, Pyrin Domain-Containing 3 Protein/metabolism , Humans , Mice , Bortezomib/pharmacology , Bortezomib/chemistry , Liposomes/chemistry , Animals , Lysosomes/metabolism , Lysosomes/drug effects , Hydroxides/chemistry , Hydroxides/pharmacology , Nanostructures/chemistry , Nanoparticles/chemistry
8.
Int J Biol Macromol ; 269(Pt 1): 132047, 2024 Jun.
Article in English | MEDLINE | ID: mdl-38702008

ABSTRACT

In our study, we developed a novel nanobiocomposite using graphene oxide (GO), casein (Cas), ZnAl layered double hydroxide (LDH), sodium alginate (Alg), and Fe3O4 magnetic nanoparticles. To synthesize the GO, we used a modified Hummer's method and then covalently functionalized its surface with Cas protein. The functionalized GO was combined with as-synthesized ZnAl LDH, and the composite was conjugated with alginate hydrogel through the gelation process. Finally, we magnetized the nanobiocomposite using in-situ magnetization. The nanobiocomposite was comprehensively characterized using FT-IR, FE-SEM, EDX, and XRD. Its biological potential was assessed through cell viability, hemolysis, and anti-biofilm assays, as well as its application in hyperthermia. The MTT assay showed high cell viability percentages for Hu02 cells after 24, 48, and 72 h of incubation. The nanobiocomposite had a hemolytic effect lower than 3.84 %, and the measured bacterial growth inhibition percentages of E. coli and S. aureus bacteria in the presence of the nanobiocomposite were 52.18 % and 55.72 %, respectively. At a concentration of 1 mg.mL-1 and a frequency of 400 kHz, the nanocomposite exhibits a remarkable specific absorption rate (SAR) of 67.04 W.g-1, showcasing its promising prospects in hyperthermia applications.


Subject(s)
Alginates , Caseins , Graphite , Hydrogels , Hydroxides , Magnetite Nanoparticles , Graphite/chemistry , Graphite/pharmacology , Alginates/chemistry , Caseins/chemistry , Hydrogels/chemistry , Hydrogels/pharmacology , Hydroxides/chemistry , Magnetite Nanoparticles/chemistry , Humans , Nanocomposites/chemistry , Cell Survival/drug effects , Anti-Bacterial Agents/pharmacology , Anti-Bacterial Agents/chemistry , Escherichia coli/drug effects , Escherichia coli/growth & development , Hemolysis/drug effects , Staphylococcus aureus/drug effects , Zinc/chemistry , Zinc/pharmacology , Biofilms/drug effects
9.
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
10.
Food Chem ; 452: 139604, 2024 Sep 15.
Article in English | MEDLINE | ID: mdl-38749139

ABSTRACT

This study aims to repurpose waste grain from the Baijiu brewing process into activated carbon for mitigating risk factors in alcoholic beverages, enhancing quality and ensuring safety. For attaining the most effective activated carbon, tailored carbon synthesis conditions were identified for diverse alcoholic beverages, optimising strategies. For beverages with low flavour compound content, optimal conditions include 900 °C calcination, 16-hour activation and a 1:2 activation ratio. In contrast, for those with abundant flavour compounds, 800 °C calcination, 16-hour activation and a 1:1 activation ratio are recommended. Post-synthesis analyses, employing nitrogen physisorption-desorption isotherms, FT-IR and SEM, validated a significant BET surface area of 244.871 m2/g for the KOH-activated carbon. Critical to adsorption efficiency, calcination temperature showcased noteworthy micro-porosity (0.8-1 nm), selectively adsorbing higher alcohols (C3-C6) and acetaldehyde while minimising acid and ester adsorption. Sensory evaluations refined optimal parameters, ensuring efficient spent grain management and heightened beverage safety without compromising aroma.


Subject(s)
Alcoholic Beverages , Charcoal , Hydroxides , Potassium Compounds , Alcoholic Beverages/analysis , Charcoal/chemistry , Humans , Hydroxides/chemistry , Potassium Compounds/chemistry , Adsorption , Taste , Waste Products/analysis , Flavoring Agents/chemistry , Edible Grain/chemistry , Odorants/analysis , Risk Factors , Male , Female , Adult , Young Adult , Middle Aged
11.
J Chromatogr A ; 1727: 464988, 2024 Jul 19.
Article in English | MEDLINE | ID: mdl-38749348

ABSTRACT

In this research, a novel magnetic nanocomposite (Fe3O4@Zn/Al-LABSA-LDH/ZIF-8) was synthesized using Fe3O4 as the magnetic core, layered double hydroxide (LDH) with linear alkylbenzene sulfonic acid (LABSA) intercalation and zeolitic imidazolate framework-8 (ZIF-8) as the shell. Benefiting from the intercalation of LABSA into LDH combined with ZIF-8, the multiple interactions, including π-π stacking, hydrogen bonding, and electrostatic interactions, conferred high selectivity and good extraction capability to the material towards heterocyclic aromatic amines (HAAs). Fe3O4@Zn/Al-LABSA-LDH@ZIF-8 was used as an adsorbent for magnetic solid-phase extraction (MSPE) to enrich HAAs in thermally processed meat samples, followed by high-performance liquid chromatography-tandem mass spectrometry (HPLC-MS/MS) detection. The method exhibited a low detection limit (0.021-0.221 ng/g), good linearity (R2 ≥ 0.9999), high precision (RSD < 7.2 %), and satisfactory sample recovery (89.7 % -107.5 %). This research provides a promising approach for developing novel adsorbents in sample preparation and improving analytical performance.


Subject(s)
Amines , Limit of Detection , Nanocomposites , Solid Phase Extraction , Tandem Mass Spectrometry , Chromatography, High Pressure Liquid/methods , Tandem Mass Spectrometry/methods , Amines/analysis , Amines/chemistry , Nanocomposites/chemistry , Solid Phase Extraction/methods , Imidazoles/chemistry , Heterocyclic Compounds/analysis , Heterocyclic Compounds/chemistry , Hydroxides/chemistry , Zeolites/chemistry , Meat/analysis , Metal-Organic Frameworks/chemistry , Adsorption , Food Contamination/analysis , Liquid Chromatography-Mass Spectrometry
12.
J Nanobiotechnology ; 22(1): 268, 2024 May 19.
Article in English | MEDLINE | ID: mdl-38764056

ABSTRACT

The development of cost-effective and eco-friendly fertilizers is crucial for enhancing iron (Fe) uptake in crops and can help alleviate dietary Fe deficiencies, especially in populations with limited access to meat. This study focused on the application of MgFe-layered double hydroxide nanoparticles (MgFe-LDHs) as a potential solution. We successfully synthesized and characterized MgFe-LDHs and observed that 1-10 mg/L MgFe-LDHs improved cucumber seed germination and water uptake. Notably, the application of 10 mg/L MgFe-LDHs to roots significantly increased the seedling emergence rate and growth under low-temperature stress. The application of 10 mg/L MgFe-LDHs during sowing increased the root length, lateral root number, root fresh weight, aboveground fresh weight, and hypocotyl length under low-temperature stress. A comprehensive analysis integrating plant physiology, nutrition, and transcriptomics suggested that MgFe-LDHs improve cold tolerance by upregulating SA to stimulate CsFAD3 expression, elevating GA3 levels for enhanced nitrogen metabolism and protein synthesis, and reducing levels of ABA and JA to support seedling emergence rate and growth, along with increasing the expression and activity of peroxidase genes. SEM and FTIR further confirmed the adsorption of MgFe-LDHs onto the root hairs in the mature zone of the root apex. Remarkably, MgFe-LDHs application led to a 46% increase (p < 0.05) in the Fe content within cucumber seedlings, a phenomenon not observed with comparable iron salt solutions, suggesting that the nanocrystalline nature of MgFe-LDHs enhances their absorption efficiency in plants. Additionally, MgFe-LDHs significantly increased the nitrogen (N) content of the seedlings by 12% (p < 0.05), promoting nitrogen fixation in the cucumber seedlings. These results pave the way for the development and use of LDH-based Fe fertilizers.


Subject(s)
Cold Temperature , Cucumis sativus , Iron , Seedlings , Cucumis sativus/growth & development , Cucumis sativus/metabolism , Cucumis sativus/drug effects , Seedlings/growth & development , Seedlings/metabolism , Seedlings/drug effects , Iron/metabolism , Plant Roots/metabolism , Plant Roots/growth & development , Germination/drug effects , Hydroxides/pharmacology , Hydroxides/metabolism , Fertilizers , Gene Expression Regulation, Plant/drug effects , Nanoparticles/chemistry , Stress, Physiological , Magnesium/metabolism
13.
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
14.
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
15.
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
16.
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
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.
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
19.
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
20.
Environ Sci Technol ; 58(19): 8501-8509, 2024 May 14.
Article in English | MEDLINE | ID: mdl-38696244

ABSTRACT

Iron/chromium hydroxide coprecipitation controls the fate and transport of toxic chromium (Cr) in many natural and engineered systems. Organic coatings on soil and engineered surfaces are ubiquitous; however, mechanistic controls of these organic coatings over Fe/Cr hydroxide coprecipitation are poorly understood. Here, Fe/Cr hydroxide coprecipitation was conducted on model organic coatings of humic acid (HA), sodium alginate (SA), and bovine serum albumin (BSA). The organics bonded with SiO2 through ligand exchange with carboxyl (-COOH), and the adsorbed amounts and pKa values of -COOH controlled surface charges of coatings. The adsorbed organic films also had different complexation capacities with Fe/Cr ions and Fe/Cr hydroxide particles, resulting in significant differences in both the amount (on HA > SA(-COOH) ≫ BSA(-NH2)) and composition (Cr/Fe molar ratio: on BSA(-NH2) ≫ HA > SA(-COOH)) of heterogeneous precipitates. Negatively charged -COOH attracted more Fe ions and oligomers of hydrolyzed Fe/Cr species and subsequently promoted heterogeneous precipitation of Fe/Cr hydroxide nanoparticles. Organic coatings containing -NH2 were positively charged at acidic pH because of the high pKa value of the functional group, limiting cation adsorption and formation of coprecipitates. Meanwhile, the higher local pH near the -NH2 coatings promoted the formation of Cr(OH)3. This study advances fundamental understanding of heterogeneous Fe/Cr hydroxide coprecipitation on organics, which is essential for successful Cr remediation and removal in both natural and engineered settings, as well as the synthesis of Cr-doped iron (oxy)hydroxides for material applications.


Subject(s)
Chromium , Hydroxides , Iron , Hydroxides/chemistry , Iron/chemistry , Chromium/chemistry , Serum Albumin, Bovine/chemistry , Adsorption , Humic Substances , Water/chemistry , Chemical Precipitation , Alginates/chemistry
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