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1.
Environ Sci Technol ; 58(19): 8501-8509, 2024 May 14.
Artículo en Inglés | MEDLINE | ID: mdl-38696244

RESUMEN

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.


Asunto(s)
Cromo , Hidróxidos , Hierro , Hidróxidos/química , Hierro/química , Cromo/química , Albúmina Sérica Bovina/química , Adsorción , Sustancias Húmicas , Agua/química , Precipitación Química , Alginatos/química
2.
J Vis Exp ; (206)2024 Apr 19.
Artículo en Inglés | MEDLINE | ID: mdl-38709074

RESUMEN

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.


Asunto(s)
Biocombustibles , Aceites de Plantas , Aceites de Plantas/química , Esterificación , Hidróxidos/química , Aceite de Oliva/química , Ondas Ultrasónicas , Compuestos de Potasio/química , Catálisis
3.
ACS Appl Mater Interfaces ; 16(19): 24295-24307, 2024 May 15.
Artículo en Inglés | MEDLINE | ID: mdl-38697643

RESUMEN

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.


Asunto(s)
Homeostasis , Inflamasomas , Proteína con Dominio Pirina 3 de la Familia NLR , Piroptosis , Piroptosis/efectos de los fármacos , Inflamasomas/metabolismo , Inflamasomas/efectos de los fármacos , Homeostasis/efectos de los fármacos , Proteína con Dominio Pirina 3 de la Familia NLR/metabolismo , Humanos , Ratones , Bortezomib/farmacología , Bortezomib/química , Liposomas/química , Animales , Lisosomas/metabolismo , Lisosomas/efectos de los fármacos , Hidróxidos/química , Hidróxidos/farmacología , Nanoestructuras/química , Nanopartículas/química
4.
J Pharm Biomed Anal ; 245: 116161, 2024 Aug 01.
Artículo en Inglés | MEDLINE | ID: mdl-38714135

RESUMEN

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.


Asunto(s)
Medicamentos Herbarios Chinos , Flavonoides , Hidróxidos , Extracción en Fase Sólida , Flavonoides/aislamiento & purificación , Flavonoides/análisis , Flavonoides/química , Extracción en Fase Sólida/métodos , Hidróxidos/química , Medicamentos Herbarios Chinos/química , Adsorción , Nanopartículas de Magnetita/química , Estructuras Metalorgánicas/química , Espectroscopía Infrarroja por Transformada de Fourier/métodos
5.
J Agric Food Chem ; 72(20): 11381-11391, 2024 May 22.
Artículo en Inglés | MEDLINE | ID: mdl-38728113

RESUMEN

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.


Asunto(s)
Larva , Interferencia de ARN , ARN Bicatenario , Animales , Larva/crecimiento & desarrollo , Larva/genética , ARN Bicatenario/genética , ARN Bicatenario/metabolismo , Hidróxidos/química , Hidróxidos/metabolismo , ATPasas de Translocación de Protón Vacuolares/genética , ATPasas de Translocación de Protón Vacuolares/metabolismo , ATPasas de Translocación de Protón Vacuolares/química , Arachis/genética , Arachis/química , Arachis/crecimiento & desarrollo , Arachis/metabolismo , Control Biológico de Vectores , Escarabajos/genética , Escarabajos/crecimiento & desarrollo , Tecnología Química Verde , Agentes de Control Biológico/química , Agentes de Control Biológico/metabolismo , Nanopartículas/química
6.
J Nanobiotechnology ; 22(1): 268, 2024 May 19.
Artículo en Inglés | MEDLINE | ID: mdl-38764056

RESUMEN

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.


Asunto(s)
Frío , Cucumis sativus , Hierro , Plantones , Cucumis sativus/crecimiento & desarrollo , Cucumis sativus/metabolismo , Cucumis sativus/efectos de los fármacos , Plantones/crecimiento & desarrollo , Plantones/metabolismo , Plantones/efectos de los fármacos , Hierro/metabolismo , Raíces de Plantas/metabolismo , Raíces de Plantas/crecimiento & desarrollo , Germinación/efectos de los fármacos , Hidróxidos/farmacología , Hidróxidos/metabolismo , Fertilizantes , Regulación de la Expresión Génica de las Plantas/efectos de los fármacos , Nanopartículas/química , Estrés Fisiológico , Magnesio/metabolismo
7.
Int J Nanomedicine ; 19: 4181-4197, 2024.
Artículo en Inglés | MEDLINE | ID: mdl-38766656

RESUMEN

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.


Asunto(s)
Diferenciación Celular , Nanopartículas , Células-Madre Neurales , Diferenciación Celular/efectos de los fármacos , Animales , Células-Madre Neurales/efectos de los fármacos , Células-Madre Neurales/citología , Células-Madre Neurales/metabolismo , Ratones , Nanopartículas/química , Metilación/efectos de los fármacos , Hidróxidos/química , Hidróxidos/farmacología , Metiltransferasas/metabolismo , Metiltransferasas/genética , Tamaño de la Partícula , Células Madre Embrionarias/efectos de los fármacos , Células Madre Embrionarias/citología , Adenosina/farmacología , Adenosina/química , Adenosina/análogos & derivados , Hidróxido de Aluminio/química , Hidróxido de Aluminio/farmacología , Hidróxido de Magnesio/química , Hidróxido de Magnesio/farmacología
8.
Int J Nanomedicine ; 19: 4199-4215, 2024.
Artículo en Inglés | MEDLINE | ID: mdl-38766657

RESUMEN

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.


Asunto(s)
Apoptosis , Neoplasias de la Mama , Ferroptosis , Hidróxidos , Simvastatina , Ferroptosis/efectos de los fármacos , Femenino , Humanos , Neoplasias de la Mama/tratamiento farmacológico , Neoplasias de la Mama/patología , Neoplasias de la Mama/metabolismo , Hidróxidos/química , Hidróxidos/farmacología , Simvastatina/farmacología , Simvastatina/química , Simvastatina/administración & dosificación , Apoptosis/efectos de los fármacos , Animales , Línea Celular Tumoral , Nanopartículas/química , Sinergismo Farmacológico , Ratones , Antineoplásicos/farmacología , Antineoplásicos/química , Ratones Desnudos , Ratones Endogámicos BALB C , Células MCF-7 , Fosfolípido Hidroperóxido Glutatión Peroxidasa/metabolismo
9.
ACS Nano ; 18(15): 10495-10508, 2024 Apr 16.
Artículo en Inglés | MEDLINE | ID: mdl-38556991

RESUMEN

Sonodynamic therapy (SDT) has promising application prospects in tumor therapy. However, SDT does not eradicate metastatic tumors. Herein, Cu-substituted ZnAl ternary layered double hydroxide nanosheets (ZCA NSs) were developed as both sonosensitizers and copper nanocarriers for synergistic SDT/cuproptosis cancer therapy. An optimized electronic structure more conducive to the sonodynamic process was obtained from ZCA NSs via the Jahn-Teller effect induced by the introduction of Cu2+, and the synthesized ZCA NSs regulated the intricate tumor microenvironment (TME) by depleting endogenous glutathione (GSH) to amplify oxidative stress for further enhanced SDT performance. Furthermore, cuproptosis was evoked by intracellular overload of Cu2+ and amplified by SDT, leading to irreversible proteotoxicity. In vitro results showed that such synergetic SDT/cuproptosis triggered immunogenic cell death (ICD) and promoted the maturation of dendritic cells (DCs). Furthermore, the as-synthesized ZCA NS-mediated SDT/cuproptosis thoroughly eradicated the in vivo solid tumors and simultaneously elicited antitumor immunity to suppress lung and liver metastasis. Overall, this work established a nanoplatform for synergistic SDT/cuproptosis with a satisfactory antitumor immunity.


Asunto(s)
Neoplasias Hepáticas , Neoplasias , Terapia por Ultrasonido , Humanos , Cobre , Electrónica , Glutatión , Hidróxidos , Neoplasias Hepáticas/tratamiento farmacológico , Inmunidad , Línea Celular Tumoral , Neoplasias/tratamiento farmacológico , Microambiente Tumoral
10.
Chemosphere ; 358: 142094, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38648984

RESUMEN

Designing of an effectual heterostructure photocatalyst for catalytic organic pollutant exclusion has been the subject of rigorous research intended to resolve the related environmental aggravation. Fabricating p-n junctions is an effective strategy to promote electron-hole separation of semiconductor photocatalysts as well as enhance the organic toxin degradation performance. In this study, a series of n-type NiAlFe-layered triple hydroxide (LTH) loaded with various ratios of p-type MoS2 was synthesized for forming a heterostructure LTH/MoS2 (LMs) by an in situ hydrothermal strategy. The photocatalysts were characterized by XRD, SEM&EDX, TEM, FT-IR, XPS, as well as UV-vis DRS. The photoactivity of photocatalysts was tested by the degradation of Indigo Carmine (IC) dye. The optimized catalyst (LM1) degrades 100% of indigo dye in high alkaline pH under UV light for 100 min. Besides, the degradation rate of LM1 is 15 times higher than that of pristine NiAlFe-LTH. The enhanced photoactivity is attributed to the synergistic effect between NiAlFe-LTH and MoS2 as well as the p-n junction formation.


Asunto(s)
Colorantes , Carmin de Índigo , Molibdeno , Catálisis , Colorantes/química , Molibdeno/química , Carmin de Índigo/química , Disulfuros/química , Concentración de Iones de Hidrógeno , Luz , Contaminantes Químicos del Agua/química , Hidróxidos/química , Fotólisis , Rayos Ultravioleta
11.
J Nanobiotechnology ; 22(1): 144, 2024 Apr 02.
Artículo en Inglés | MEDLINE | ID: mdl-38566094

RESUMEN

Improving the efficiency of antiseizure medication entering the brain is the key to reducing its peripheral toxicity. A combination of intranasal administration and nanomedicine presents a practical approach for treating epileptic seizures via bypassing the blood-brain barrier. In this study, phenytoin (PHT) loaded layered double hydroxide nanoparticles (BSA-LDHs-PHT) were fabricated via a coprecipitation - hydrothermal method for epileptic seizure control. In this study, we expound on the preparation method and characterization of BSA-LDHs-PHT. In-vitro drug release experiment shows both rapid and continuous drug release from BSA-LDHs-PHT, which is crucial for acute seizure control and chronic epilepsy therapy. In-vivo biodistribution assays after intranasal administration indicate excellent brain targeting ability of BSA-LDHs. Compared to BSA-Cyanine5.5, BSA-LDHs-Cyanine5.5 were associated with a higher brain/peripheral ratio across all tested time points. Following intranasal delivery with small doses of BSA-LDHs-PHT, the latency of seizures in the pentylenetetrazole-induced mouse models was effectively improved. Collectively, the present study successfully designed and applied BSA-LDHs-PHT as a promising strategy for treating epileptic seizures with an enhanced therapeutic effect.


Asunto(s)
Epilepsia , Nanopartículas , Ratones , Animales , Fenitoína/farmacología , Fenitoína/uso terapéutico , Administración Intranasal , Distribución Tisular , Convulsiones/tratamiento farmacológico , Epilepsia/tratamiento farmacológico , Nanopartículas/uso terapéutico , Hidróxidos/uso terapéutico
12.
J Colloid Interface Sci ; 666: 512-528, 2024 Jul 15.
Artículo en Inglés | MEDLINE | ID: mdl-38613974

RESUMEN

Metronidazole (MNZ), a commonly used antibiotic, poses risks to water bodies and human health due to its potential carcinogenic, mutagenic, and genotoxic effects. In this study, mesoporous cobalt-manganese layered double hydroxides (CoxMny-LDH) with abundant oxygen vacancies (Ov) were successfully synthesized using the co-precipitation method and used to activate calcium sulfite (CaSO3) with slight soluble in water for MNZ degradation. The characterization results revealed that Co2Mn-LDH had higher specific areas and exhibited good crystallinity. Co2Mn-LDH/CaSO3 exhibited the best catalytic performance under optimal conditions, achieving a remarkable MNZ degradation efficiency of up to 98.1 % in only 8 min. Quenching experiments and electron paramagnetic resonance (EPR) tests showed that SO4•- and 1O2 played pivotal roles in the MNZ degradation process by activated CaSO3, while the redox cycles of Co2+/Co3+ and Mn3+/Mn4+ on the catalyst surface accelerated electron transfer, promoting radical generation. Three MNZ degradation routes were put forward based on the density functional theory (DFT) and liquid chromatography-mass spectrometer (LC-MS) analysis. Meanwhile, the toxicity analysis result demonstrated that the toxicity of intermediates post-catalytic reaction was decreased. Furthermore, the Co2Mn-LDH/CaSO3 system displayed excellent stability, reusability, and anti-interference capability, and achieved a comparably high removal efficiency across various organic pollutant water bodies. This study provides valuable insights into the development and optimization of effective heterogeneous catalysts for treating antibiotic-contaminated wastewater.


Asunto(s)
Cobalto , Hidróxidos , Manganeso , Metronidazol , Cobalto/química , Metronidazol/química , Hidróxidos/química , Manganeso/química , Porosidad , Propiedades de Superficie , Sulfitos/química , Catálisis , Tamaño de la Partícula , Teoría Funcional de la Densidad , Contaminantes Químicos del Agua/química
13.
Biosens Bioelectron ; 256: 116275, 2024 Jul 15.
Artículo en Inglés | MEDLINE | ID: mdl-38603839

RESUMEN

Constructing relatively inexpensive nanomaterials to simulate the catalytic performance of laccase is of great significance in recent years. Although research on improving laccase-like activity by regulating ligands of copper (amino acids or small organic molecules, etc.) have achieved remarkable success. There are few reports on improving laccase-like activity by adjusting the composition of metal Cu. Here, we used perovskite hydroxide AB(OH)6 as a model to evaluate the relationship between Cu based alloys and their laccase-like activity. We found that when the Cu/Mn alloy ratio of the perovskite hydroxide A point is greater than 1, the laccase-like activity of the binary alloy perovskite hydroxide is higher than that of the corresponding single Cu. Based on the measurements of XPS and ICP-MS, we deduced that the improvements of laccase-like activity mainly attribute to the ratio of Cu+/Cu2+and the content of Cu. Moreover, two types of substrates (toxic pollutants and catechol neurotransmitters) were used to successfully demonstrated such nanozymes' excellent environmental protecting function and biosensing property. This work will provide a novel approach for the construction and application of laccase-like nanozymes in the future.


Asunto(s)
Técnicas Biosensibles , Cobre , Lacasa , Óxidos , Titanio , Lacasa/química , Lacasa/metabolismo , Técnicas Biosensibles/métodos , Cobre/química , Titanio/química , Óxidos/química , Hidróxidos/química , Compuestos de Calcio/química , Restauración y Remediación Ambiental/métodos , Catecoles/análisis , Catecoles/química , Materiales Biomiméticos/química , Catálisis
14.
Int J Mol Sci ; 25(8)2024 Apr 19.
Artículo en Inglés | MEDLINE | ID: mdl-38674090

RESUMEN

Cinnamic acid (CA) was successfully incorporated into Zn-Al layered double hydroxide (LDH) through coprecipitation. The CA moiety was stabilized in the interlayer space through not only electrostatic interaction but also intermolecular π-π interaction. It was noteworthy that the CA arrangement was fairly independent of the charge density of LDH, showing the important role of the layer-CA and CA-CA interactions in molecular stabilization. Computer simulations using the Monte Carlo method as well as analytical approaches including infrared, UV-vis spectroscopy, and differential scanning calorimetry showed the existence of intermolecular interaction. In order to reinforce molecular stabilization, a neutral derivative of CA, cinnamaldehyde (CAD), was additionally incorporated into LDH. It was clearly shown that CAD played a role as a π-π interaction mediator to enhance the stabilization of CA. The time-dependent release of CA from LDH was first governed by the layer charge density of LDH; however, the existence of CAD provided additional stabilization to the CA arrangement to slow down the release kinetics.


Asunto(s)
Acroleína/análogos & derivados , Cinamatos , Preparaciones de Acción Retardada , Hidróxidos , Cinamatos/química , Hidróxidos/química , Preparaciones de Acción Retardada/química , Acroleína/química , Cinética , Método de Montecarlo , Rastreo Diferencial de Calorimetría
15.
Environ Sci Pollut Res Int ; 31(20): 29132-29147, 2024 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-38568311

RESUMEN

Layered double hydroxides (LDH) hold great promise as phosphate adsorbents; however, the conventional binary LDH exhibits low adsorption rate and adsorption capacity. In this study, Mg and La were chosen as binary metals in the synthesis of Mg-La LDH to enhance phosphate efficient adsorption. Different molar ratios of Mg to La (2:1, 3:1, and 4:1) were investigated to further enhance P adsorption. The best performing Mg-La LDH, with Mg to La ratio is 4:1 (LDH-4), presented a larger adsorption capacity and faster adsorption rate than other Mg-La LDH. The maximum adsorption capacity (87.23 mg/g) and the rapid adsorption rate in the initial 25 min of LDH-4 (70 mg/(g·h)) were at least 1.6 times and 1.8 times higher than the others. The kinetics, isotherms, the effect of initial pH and co-existing anions, and the adsorption-desorption cycle experiment were studied. The batch experiment results proved that the chemisorption progress occurred on the single-layered LDH surface and the optimized LDH exhibited strong anti-interference capability. Furthermore, the structural characteristics and adsorption mechanism were further investigated by SEM, BET, FTIR, XRD, and XPS. The characterization results showed that the different metal ratios could lead to changes in the metal hydroxide layer and the main ions inside. At lower Mg/La ratios, distortion occurred in the hydroxide layer, resulting in lower crystallinity and lower performance. The characterization results also proved that the main mechanisms of phosphate adsorption are electrostatic adsorption, ion exchange, and inner-sphere complexation. The results emphasized that the Mg-La LDH was efficient in phosphate removal and could be successfully used for this purpose.


Asunto(s)
Hidróxidos , Magnesio , Fosfatos , Adsorción , Hidróxidos/química , Fosfatos/química , Magnesio/química , Cinética , Lantano/química , Contaminantes Químicos del Agua/química , Concentración de Iones de Hidrógeno
16.
Chemosphere ; 356: 141916, 2024 May.
Artículo en Inglés | MEDLINE | ID: mdl-38583536

RESUMEN

This study presents an assessment of inorganic and organic modification of biochar on physicochemical properties, dissolved organic carbon (DOC) release, sorption efficiency towards enrofloxacin (E) and silver nanoparticles (Ag-NPs), as well as an evaluation of addition of prepared materials on hydro-physical properties and adsorption capacity of montmorillonite (M). The biochar was derived from wheat straw at 650 °C. An inorganic modification was performed using ammonia hydroxide, whereas an organic modification, using citric acid. The ammonia hydroxide and citric acid changed the biochar nature and surface chemistry by introducing amino and ester groups. The lowest DOC release was from ammonia-biochar (BCN) and the highest, from citric acid-biochar (BCC). The adsorption data were better described by pseudo-II order equation and Marczewski-Jaroniec isotherm. Results showed that BCN exhibited the highest efficiency in adsorption of E and Ag-NPs. It also improved the adsorptive abilities and saturated hydraulic conductivity of M. This provides the chemically modified biochars have an excellent potential to improve pollution removal from aqueous media and hydro-physical/sorption properties of soil sorption complex. They can be used with advantageous in environmental applications.


Asunto(s)
Carbón Orgánico , Ácido Cítrico , Nanopartículas del Metal , Triticum , Triticum/química , Carbón Orgánico/química , Ácido Cítrico/química , Adsorción , Nanopartículas del Metal/química , Bentonita/química , Plata/química , Enrofloxacina/química , Hidróxidos/química , Amoníaco/química
17.
Environ Sci Pollut Res Int ; 31(20): 30196-30211, 2024 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-38600374

RESUMEN

This study innovatively added biochar to optimize regulation in the neutralization process of simulated acid mine drainage (AMD) and recovered a new type of matrix layered double hydroxides (MLDH), which can be used to remove copper (Cu(II)) and cadmium (Cd(II)) from wastewater. A series of batch experiments show that MLDH with strong selective removal ability of Cu(II) and Cd(II) can be successfully obtained by adding biochar (BC) at pH = 5 end in the neutralization process. Kinetic and isotherm modeling studies indicated that the removal of Cu(II) and Cd(II) by the MLDH was a chemical multilayer adsorption process. The removal mechanism of Cu(II) and Cd(II) was further analyzed through related characterization analysis with contribution rate calculation: the removal rates of Cu(II) and Cd(II) by ion exchange were 42.7% and 26%, while that by precipitation were 34.5% and 49.9%, respectively. This study can provide a theoretical reference and experimental basis for the recovery and utilization of valuable by-products in AMD and the treatment of heavy metal wastewater.


Asunto(s)
Cadmio , Cobre , Hidróxidos , Minería , Aguas Residuales , Contaminantes Químicos del Agua , Cobre/química , Cadmio/química , Aguas Residuales/química , Contaminantes Químicos del Agua/química , Hidróxidos/química , Adsorción , Carbón Orgánico/química , Cinética , Eliminación de Residuos Líquidos/métodos
18.
Environ Sci Technol ; 58(19): 8597-8606, 2024 May 14.
Artículo en Inglés | MEDLINE | ID: mdl-38687950

RESUMEN

NiFe layered double hydroxides (NiFe-LDH) exhibited an outstanding performance and promising application potential for removing ozone. However, the effect of interlayer anions on ozone removal remains ambiguous. Here, a series of NiFe-LDH with different interlayer anions (F-, Cl-, Br-, NO3-, CO32-, and SO42-) were prepared to investigate the effect of the interlayer anion on ozone removal for the first time. It was found that the interlayer anions are a key factor affecting the water resistance of the NiFe-LDH catalyst under moist conditions. NiFe-LDH-CO32- exhibited the best water resistance, which was much better than that of NiFe-LDH containing other interlayer anions. The in situ DIRFTS demonstrates that the carbonates in the interlayer of NiFe-LDH-CO32- will undergo coordination changes through the interaction with water molecules under moist conditions, exposing new metal sites. As a result, the newly exposed metal sites could activate water molecules into hydroxyl groups that act as active sites for catalyzing ozone decomposition. This work provides a new insight into the interlayer anions of LDH, which is important for the design and development of LDH catalysts with excellent ozone removal properties.


Asunto(s)
Aniones , Hidróxidos , Ozono , Ozono/química , Hidróxidos/química , Catálisis , Aniones/química
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