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1.
Angew Chem Int Ed Engl ; : e202402669, 2024 Apr 18.
Artigo em Inglês | MEDLINE | ID: mdl-38637296

RESUMO

Singlet oxygen (1O2) is an essential reactive species responsible for selective oxidation of organic matter, especially in Fenton-like processes. However, due to the great limitations in synthesizing catalysts with well-defined active sites, the controllable production and practical application of 1O2 remain challenging. Herein, guided by theoretical simulations, a series of boron nitride-based single-atom catalysts (BvBN/M, M = Co, Fe, Cu, Ni and Mn) were synthesized to regulate 1O2 generation by activating peroxymonosulfate (PMS). All the fabricated BvBN/M catalysts with explicit M-N3 sites promoted the self-decomposition of the two PMS molecules to generate 1O2 with high selectivity, where BvBN/Co possessed moderate adsorption energy and d-band center exhibited superior catalytic activity. As an outcome, the BvBN/Co-PMS system coupled with membrane filtration technology could continuously transform aromatic alcohols to aldehydes with nearly 100% selectivity and conversion rate under mild conditions, suggesting the potential of this novel catalytic system for green organic synthesis.

2.
Cell Biosci ; 14(1): 55, 2024 Apr 27.
Artigo em Inglês | MEDLINE | ID: mdl-38678262

RESUMO

BACKGROUND: Alzheimer's disease (AD) is the most prevalent neurodegenerative disease with limited disease-modifying treatments. Drug repositioning strategy has now emerged as a promising approach for anti-AD drug discovery. Using 5×FAD mice and Aß-treated neurons in culture, we tested the efficacy of Y-2, a compounded drug containing the antioxidant Edaravone (Eda), a pyrazolone and (+)-Borneol, an anti-inflammatory diterpenoid from cinnamon, approved for use in amyotrophic lateral sclerosis patients. RESULTS: We examined effects of Y-2 versus Eda alone by i.p. administered in 8-week-old 5×FAD mice (females) for 4 months by comparing cognitive function, Aß pathologies, neuronal necroptosis and neuroinflammation. Using primary neurons and astrocytes, as well as neuronal and astrocytic cell lines, we elucidated the molecular mechanisms of Y-2 by examining neuronal injury, astrocyte-mediated inflammation and necroptosis. Here, we find that Y-2 improves cognitive function in AD mice. Histopathological data show that Y-2, better than Eda alone, markedly ameliorates Aß pathologies including Aß burden, astrogliosis/microgliosis, and Tau phosphorylation. In addition, Y-2 reduces Aß-induced neuronal injury including neurite damage, mitochondrial impairment, reactive oxygen species production and NAD+ depletion. Notably, Y-2 inhibits astrocyte-mediated neuroinflammation and attenuates TNF-α-triggered neuronal necroptosis in cell cultures and AD mice. RNA-seq further demonstrates that Y-2, compared to Eda, indeed upregulates anti-inflammation pathways in astrocytes. CONCLUSIONS: Our findings infer that Y-2, better than Eda alone, mitigates AD pathology and may provide a potential drug candidate for AD treatment.

3.
Chemosphere ; 354: 141737, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38499078

RESUMO

Extracting heavy metal ions from wastewater has significant implications for both environmental remediation and resource preservation. However, the conventional adsorbents still suffer from incomplete ion removal and low utilization efficiency of the recovered metals. Herein, we present an extraction and reutilization method assisted by porous boron nitride (p-BN) containing high-density N atoms for metal recovery with simultaneous catalyst formation. The p-BN exhibits stable and efficient metal adsorption performance, particularly for ultra-trace-level water purification. The distribution coefficients towards Pb2+, Cd2+, Co2+ and Fe3+ can exceed 106 mL g-1 and the residual concentrations that reduced from 1 mg L-1 to 0.8-1.3 µg L-1 are much lower than the acceptable limits in drinking water standards of World Health Organization. Meanwhile, the used p-BN after Co ion adsorption can be directly adopted as a high-efficiency catalyst for activating peroxymonosulfate (PMS) in organic pollutant degradation without additional post-treatment, avoiding the secondary metal pollution and the problems of neglected manpower and energy consumption. Moreover, a flow-through multistage utilization system assisted by p-BN/polyvinylidene fluoride (PVDF) membrane is constructed for achieving both metal ion separation and reutilization in the removal of organic pollutants, providing a new avenue for sustainable wastewater remediation.


Assuntos
Compostos de Boro , Poluentes Ambientais , Metais Pesados , Poluentes Químicos da Água , Águas Residuárias , Porosidade , Poluentes Químicos da Água/análise , Metais Pesados/análise , Adsorção , Íons
4.
Nat Commun ; 14(1): 7841, 2023 Nov 29.
Artigo em Inglês | MEDLINE | ID: mdl-38030639

RESUMO

The development of heterogenous catalysts based on the synthesis of 2D carbon-supported metal nanocatalysts with high metal loading and dispersion is important. However, such practices remain challenging to develop. Here, we report a self-polymerization confinement strategy to fabricate a series of ultrafine metal embedded N-doped carbon nanosheets (M@N-C) with loadings of up to 30 wt%. Systematic investigation confirms that abundant catechol groups for anchoring metal ions and entangled polymer networks with the stable coordinate environment are essential for realizing high-loading M@N-C catalysts. As a demonstration, Fe@N-C exhibits the dual high-efficiency performance in Fenton reaction with both impressive catalytic activity (0.818 min-1) and H2O2 utilization efficiency (84.1%) using sulfamethoxazole as the probe, which has not yet been achieved simultaneously. Theoretical calculations reveal that the abundant Fe nanocrystals increase the electron density of the N-doped carbon frameworks, thereby facilitating the continuous generation of long-lasting surface-bound •OH through lowering the energy barrier for H2O2 activation. This facile and universal strategy paves the way for the fabrication of diverse high-loading heterogeneous catalysts for broad applications.

5.
Cell Biosci ; 13(1): 128, 2023 Jul 10.
Artigo em Inglês | MEDLINE | ID: mdl-37430358

RESUMO

BACKGROUND: Ectodysplasin-A (EDA), a skin-specific TNF ligand, interacts with its membrane receptor EDAR to trigger EDA signaling in skin appendage formation. Gene mutations in EDA signaling cause Anhidrotic/Hypohidrotic Ectodermal Dysplasia (A/HED), which affects the formation of skin appendages including hair, teeth, and several exocrine glands. RESULTS: We report that EDA triggers the translocation of its receptor EDAR from a cytosolic compartment into the plasma membrane. We use protein affinity purification to show that upon EDA stimulation EDAR associates with SNAP23-STX6-VAMP1/2/3 vesicle trafficking complexes. We find that EDA-dependent PKA activation is critical for the association. Notably, either of two HED-linked EDAR mutations, T346M and R420W, prevents EDA-induced EDAR translocation; and both EDA-induced PKA activation and SNAP23 are required for Meibomian gland (MG) growth in a skin appendage model. CONCLUSIONS: Overall, in a novel regulatory mechanism, EDA increases plasma membrane translocation of its own receptor EDAR, augmenting EDA-EDAR signaling in skin appendage formation. Our findings also provide PKA and SNAP23 as potential targets for the intervention of HED.

6.
Molecules ; 28(6)2023 Mar 21.
Artigo em Inglês | MEDLINE | ID: mdl-36985806

RESUMO

Plastic electrodes are desirable for the rapid development of flexible organic electronics. In this article, a plastic electrode has been prepared by employing traditional conducting polymer poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) and plastic substrate polyethersulfone (PES). The completed electrode (Denote as HC-PEDOT:PSS) treated by 80% concentrated sulfuric acid (H2SO4) possesses a high electrical conductivity of over 2673 S/cm and a high transmittance of over 90% at 550 nm. The high conductivity is attributed to the regular arrangement of PEDOT molecules, which has been proved by the X-ray diffraction characterization. Temperature-dependent conductivity measurement reveals that the HC-PEDOT:PSS possesses both semiconducting and metallic properties. The binding force and effects between the PEDOT and PEI are investigated in detail. All plastic solar cells with a classical device structure of PES/HC-PEDOT:PSS/PEI/P3HT:ICBA/EG-PEDOT:PSS show a PCE of 4.05%. The ITO-free device with a structure of Glass/HC-PEDOT:PSS/Al4083/PM6:Y6/PDINO/Ag delivers an open-circuit voltage (VOC) of 0.81 V, short-circuit current (JSC ) of 23.5 mA/cm2, fill factor (FF) of 0.67 and a moderate power conversion efficiency (PCE) of 12.8%. The above results demonstrate the HC-PEDOT:PSS electrode is a promising candidate for all-plastic solar cells and ITO-free organic solar cells.

7.
ChemSusChem ; 16(6): e202202208, 2023 Mar 22.
Artigo em Inglês | MEDLINE | ID: mdl-36527278

RESUMO

Herein, a novel conducting polymer complex PEDOT:CF3 SO2(x) PSS(1-x) [denoted as S-PEDOT:CF3 SO2(x) PSS(1-x) , where PEDOT is poly(3,4-ethylenedioxythiophene) and PSS is poly(styrene sulfonate)], is fabricated with the assistance of zinc di[bis(trifluoromenthylsulfonyl) imide][Zn(TFSI)2 ] (CFE). The introduction of CF3 SO2 - group is expected to bring better stability of PEDOT:CF3 SO2 than PEDOT:PSS due to its strong Coulomb force. Electrochemical measurement shows that a high specific capacitance of 194 F cm-3 was achieved from the novel complex S-PEDOT:CF3 SO2(x) PSS(1-x) , the highest value reported so far. An all-solid-state supercapacitor assembly with a structure of S-PEDOT:CF3 SO2(x) PSS(1-x) /H2 SO4 :polyvinyl alcohol (PVA)/S-PEDOT:CF3 SO2(x) PSS(1-x) shows a record specific capacitance of 70.9 F cm-3 and a maximum energy density of 6.02 mWh cm-3 at a power density of 397 mW cm-3 . This supercapacitor device demonstrates excellent electrochemical stability with a capacitance retention rate of 98 % after 10 000 cycles and extreme air stability of 96 % capacitance retention rate after 10 000 cycles, even if the device is exposed to air over 2880 h, much better than that of PEDOT:PSS based supercapacitors. Excellent capacitance can be achieved from PEDOT:CF3 SO2(x) PSS(1-x) electrode under electrolyte-free conditions. This work provides a novel method for high performance stable supercapacitors and may pave the way for the commercialization of PEDOT based supercapacitors.

8.
Environ Sci Pollut Res Int ; 30(1): 1386-1398, 2023 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-35917064

RESUMO

Wastewater containing organic pollutants with high toxicity and poor biodegradability poses a considerable threat to human health and the ecosystem. Although adsorption and advanced oxidation processes (AOPs) are currently the most widely used technologies for wastewater treatment, limitations of these two independent processes make the treatment effect unsatisfactory. Herein, a system of integrating adsorption and subsequent in situ AOPs is established by a 3D carbon aerogel embedded with Fe-doped carbonitrides (Fe-NC/CAG). The SEM and BET analysis demonstrate that Fe-NC/CAG possesses porous structures with a specific surface area of 518.7 m2/g. The XRD result indicates the formation of Fe0 and Fe3O4 in Fe-NC/CAG. The impacts of operational parameters such as Fe-NC/CAG dosage, pollutants concentration, temperature, initial pH, and inorganic ions on the adsorption efficiency are investigated. The adsorption kinetics is predominantly based on the pseudo-second-order model. After adsorbing organic pollutants, the Fe-NC/CAG is immersed in peroxymonosulfate (PMS) solution. The adsorbed pollutants are in situ degraded by PMS-based AOPs, leading to the regeneration of Fe-NC/CAG. At optimum conditions, the integrating process established by Fe-NC/CAG achieves over 90% removal of antibiotics, phenolics, and dyes as well as keeps stable performance even after 6 cycles. This integrating adsorption and AOPs system is expected to open up a rich field for wastewater treatment.


Assuntos
Poluentes Ambientais , Poluentes Químicos da Água , Humanos , Carbono , Águas Residuárias , Adsorção , Ecossistema , Poluentes Ambientais/análise , Poluentes Químicos da Água/análise
9.
ACS Omega ; 8(51): 49372-49382, 2023 Dec 26.
Artigo em Inglês | MEDLINE | ID: mdl-38162746

RESUMO

This study aimed to prepare open-cell foams using a blend of long-chain branched polypropylene and polyolefin elastomer (LCBPP/POE) for the production of reusable oil absorbents. The supercritical CO2 foaming process was conducted using a two-step batch rapid depressurization method. This unique two-step foaming approach significantly expanded the temperature and pressure windows, resulting in more uniform cells with smaller sizes, ultimately leading to higher expansion ratios and an increased open cell content. The foaming process was optimized by adjusting parameters, such as the LCBPP/POE ratio, foaming temperature, and foaming pressure, reaching a maximum open cell content of 97.6% and a maximum expansion ratio of 48. The influence of polypropylene (PP) crystallization was investigated with the aid of scanning electron microscopy and differential scanning calorimetry. Furthermore, the hydrophobic and lipophilic characteristics of the LCBPP/POE open-cell foam were determined via contact angle measurements and oil/water separation tests. Oil absorption tests revealed that the blended LCBPP/POE foam has a higher oil absorption capacity than that of the pure LCBPP foam. The cyclic oil absorption tests demonstrated the outstanding ductility and recoverability of the LCBPP/POE open-cell foam in comparison to those of the pure LCBPP foam. Over 10 cycles, the LCBPP/POE foam maintained a substantial adsorption capacity, retaining 99.3% of its initial oil absorption capacity. With its notable features, including a high open cell content, excellent hydrophobic and lipophilic characteristics, superior oil absorption capacity, impressive cyclic oil absorption performance, and robust reusability, LCBPP/POE open-cell foams exhibit significant promise as potential oil adsorbents for use in oil spill cleanup applications.

10.
Cell Biosci ; 12(1): 180, 2022 Nov 04.
Artigo em Inglês | MEDLINE | ID: mdl-36333711

RESUMO

BACKGROUND: Neurite dystrophy is a pathologic hallmark of Alzheimer's disease (AD). However, drug discovery targeting neurite protection in AD remains largely unexplored. METHODS: Aß-induced neurite and mitochondrial damage assays were used to evaluate Aß toxicity and the neuroprotective efficacy of a natural compound salidroside (SAL). The 5×FAD transgenic mouse model of AD was used to study the neuroprotective function of SAL. To verify the direct target of SAL, we used surface plasmon resonance and cellular thermal shift assays to analyze the drug-protein interaction. RESULTS: SAL ameliorates Aß-mediated neurite damage in cell culture. We further reveal that SAL represses mitochondrial damage in neurites by promoting mitophagy and maintaining mitochondrial homeostasis, dependent on an NAD-dependent deacetylase SIRT3. In AD mice, SAL protects neurite morphology, mitigates Aß pathology, and improves cognitive function, which are all SIRT3-dependent. Notably, SAL directly binds to transcription factor NRF2, inhibits its degradation by blocking its interaction with KEAP1 ubiquitin ligase, and then advances NRF2-mediated SIRT3 transcription. CONCLUSIONS: Overall, we demonstrate that SAL, a potential anti-aging drug candidate, attenuates AD pathology by targeting NRF2/SIRT3 pathway for mitochondrial and neurite protection. Drug discovery strategies focusing on SAL may thus provide promising therapeutics for AD.

11.
Int J Mol Sci ; 23(16)2022 Aug 10.
Artigo em Inglês | MEDLINE | ID: mdl-36012178

RESUMO

Ectodysplasin A (EDA) signaling is initially identified as morphogenic signaling regulating the formation of skin appendages including teeth, hair follicles, exocrine glands in mammals, feathers in birds and scales in fish. Gene mutation in EDA signaling causes hypohidrotic ectodermal dysplasia (HED), a congenital hereditary disease with malformation of skin appendages. Interestingly, emerging evidence suggests that EDA and its receptors can modulate the proliferation, apoptosis, differentiation and migration of cancer cells, and thus may regulate tumorigenesis and cancer progression. More recently, as a newly discovered hepatocyte factor, EDA pathway has been demonstrated to be involved in the pathogenesis of nonalcoholic fatty liver disease (NAFLD) and type II diabetes by regulating glucose and lipid metabolism. In this review, we summarize the function of EDA signaling from skin appendage development to multiple other diseases, and discuss the clinical application of recombinant EDA protein as well as other potential targets for disease intervention.


Assuntos
Diabetes Mellitus Tipo 2 , Displasia Ectodérmica Anidrótica Tipo 1 , Animais , Diabetes Mellitus Tipo 2/metabolismo , Ectodisplasinas/genética , Ectodisplasinas/metabolismo , Mamíferos/metabolismo , Transdução de Sinais , Pele/metabolismo
12.
RSC Adv ; 12(31): 20062-20073, 2022 Jul 06.
Artigo em Inglês | MEDLINE | ID: mdl-35919620

RESUMO

Herein, we developed a low-cost fabrication route to prepare chemically grafted activated carbon fibers, which effectively removed Pb2+ from solution. Multiple characteristic results indicated that l-cyst-ACF had abundant nitrogen-containing and sulfur-containing functional groups. Based on the XPS and EDS analyses, the capture of Pb2+ was attributed to the abundant adsorption sites on the fiber surface. According to the analysis of the pseudo-second-order kinetic model and the Langmuir isotherm model, the adsorption process could be interpreted as monolayer adsorption and chemisorption, and the equilibrium adsorption capacity was determined to be 136.80 mg g-1 by fitting the pseudo-second-order kinetic model. The maximum adsorption capacity of l-cyst-ACF for Pb2+ was calculated to be 179.53 mg g-1 using the Langmuir model. In addition, the adsorption reaction was endothermic and spontaneous, as evidenced by the thermodynamic parameters. The outcomes of this study provide a low-cost and feasible strategy for the remediation of Pb2+ pollution in the environment.

13.
Chemosphere ; 306: 135501, 2022 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-35779678

RESUMO

Developing novel bifunctional materials to high efficiently degrade organic pollutants and eliminate hexavalent chromium (Cr (VI)) is significantly desired in the wastewater treatment field. The porous boron nitride (p-BN) was fabricated by a two-stage calcination strategy and was innovatively employed to support zero-valent iron (ZVI), achieving the bifunctional material (p-BN@ZVI) to degrade carbamazepine (CBZ) and eliminate Cr (VI). p-BN@ZVI could degrade more than 98% CBZ in 6 min with the high apparent first-order constant (kobs) of 0.536 min-1, almost 5 times higher than that of the ZVI/PMS system and outperformed most previous reported ZVI supported catalysts, which was mainly ascribed to the fact that the introduction of p-BN with high surface area (793.97 m2/g) improved the dispersion of ZVI and exposed more active sites. Quenching tests coupled with electron paramagnetic resonance (EPR) suggested that •OH was the major reactive oxygen species with a contribution of 71.6%. Notably, the p-BN@ZVI/PMS system expressed low activation energy of 8.23 kJ/mol and reached a 65.69% TOC degradation in 20 min even at 0 °C. p-BN@ZVI possessed remarkable storage stability and could still degrade 92.3% CBZ despite three-month storage. More interestingly, p-BN@ZVI was capable to eliminate 98.1% of 50 mg/L Cr (VI) within 5 min through adsorption and reduction, where nearly 80% Cr (VI) was transformed to Cr (III), and exhibited the maximum Cr (VI) elimination capacity of 349 mg/g. This study provides new insights into the efficient organic contaminants degradation and Cr (VI) elimination in the treatment of wastewater.


Assuntos
Poluentes Químicos da Água , Purificação da Água , Adsorção , Compostos de Boro , Cromo/análise , Ferro/química , Porosidade , Poluentes Químicos da Água/química
14.
J Environ Manage ; 311: 114859, 2022 Mar 08.
Artigo em Inglês | MEDLINE | ID: mdl-35276558

RESUMO

Developing highly efficient and stable catalysts for peroxymonosulfate (PMS) based advanced oxidation processes (AOPs) are crucial in the field of environmental remediation. In this work, a facile encapsulated-precursor pyrolysis strategy was reported to prepare a competent PMS-activation catalyst, in which uniformly distributed Fe3O4 nanoparticles were firmly anchored on porous boron nitride (BN) nanosheets by N-doped carbon shell (NC layer). Taking advantage of strong metal-support interaction, the as-synthesized catalyst (BFA-500) could efficiently activate PMS to achieve 100% removal of 4-chlorophenol (4-CP) in 6 min, and the corresponding turnover frequency (TOF) value was 1-2 orders of magnitude higher than that of the benchmark homogeneous (Fe2+) and nanoparticle (Fe0 and Fe3O4) catalysts. Moreover, the well protected encapsulated structure of BFA-500 ensured the remarkable stability that could effectively resist the interference of complex water environment, including initial pH value, various inorganic ions and actual water, and its catalytic activity remained almost unchanged in 5 use-regeneration cycles. More importantly, the generation of O2•- and 1O2 radicals for the 4-CP removal in BFA-500/PMS system was ascribed to Fe3O4 boosted C-N sites containing pyridinic N, where electrons transferred from the embedded Fe3O4 nanoparticles to C-N sites to secure the PMS dissociation into reactive radicals. Overall, this work provided a promising way to design desired PMS-activation catalyst toward wastewater purification.

15.
Chemosphere ; 294: 133704, 2022 May.
Artigo em Inglês | MEDLINE | ID: mdl-35066083

RESUMO

Developing Fe-based catalysts with high-effective and environmentally friendly features in Fenton-like system for treating wastewater is still a challenge. Novel nitrogen-doped carbon nanosheets with Fe0/Fe3C nano-particles (Fe@NCS-900) were prepared through a simple solvent-free strategy by pyrolyzing the mixture of 2,6-diaminopyridine and ferric chloride hexahydrate under 900 °C. The Fe@NCS-900 possessed almost 100% removal efficiency and 66.5% mineralization rate for the degradation of CBZ in 10 min. Moreover, the Fe@NCS-900 exhibited an apparent first-order constant as high as 0.8809 min-1, which is 22 and 29 times higher than that of the commercial Fe0 and traditional Fenton system, respectively, which could be attribute to the high graphitization degree and rich nitrogen content. Besides, the results of the radical quenching experiments, electron paramagnetic resonance (EPR) and the probe experiments demonstrated that a large number of high valent iron species (Fe (IV)) besides singlet oxygen (1O2) and superoxide radicals (O2•-) existed and contributed to the CBZ degradation. More interestingly, the addition of coexisting anion SO42- in the reaction system could significantly boost the concentration of •OH and SO4•- by 28.3 times and 9.7 times, respectively, resulting in the increase of the apparent first-order constant by 5.9 times (5.1733 min-1), which was entirely different from previous reports that SO42- had no effect on the catalytic activity or even displayed slightly inhibitory effect. In addition, the catalyst exhibited broad pH adaptability in the pH range of 2-9. The intermediate products of CBZ degradation were investigated by liquid chromatography mass spectrometry (LC-MS) and the degradation pathway was proposed. This paper provides new insights for developing a promising Fe-based nitrogen-doped catalyst for practical wastewater treatment.


Assuntos
Carbono , Nanopartículas , Antibacterianos , Nitrogênio , Peróxidos/química , Sulfatos
16.
Environ Res ; 207: 112212, 2022 05 01.
Artigo em Inglês | MEDLINE | ID: mdl-34662578

RESUMO

Developing filtering materials with high permeation flux and contaminant removal rate is of great importance for oily wastewater remediation. Herein, a robust three-dimensional (3D) activated carbon fibers (ACFs) based composite with uniformly grown layered double hydroxide (LDH) on the surface was successfully constructed through a feasible hydrothermal strategy. The LDH with a high surface energy and vertically aligned structure could provide superhydrophilicity to ACFs. Systematic investigation confirmed that the 3D material could overcome the size mismatch between the ACFs macropores and tiny emulsified droplets through the combination of size-sieving filtration on the surface and oil droplet coalescence in the fiber network. This process efficiently separated the intractable surfactant-stabilized oil-in-water emulsions with high permeation flux (up to 4.16 × 106 L m-2 h-1 bar-1). Notably, the LDH also had well-dispersed catalytic active sites, which could initiate advanced oxidation processes (AOPs) to efficiently eliminate various types of water-soluble organic pollutants (e.g., pharmaceuticals, phenolic compounds and organic dyes). The resulting modified ACFs exhibited exceptional removal rates for both oil and organic pollutants in the complex sewage during the continuous filtration process. These versatile abilities integrated with the facile preparation method reported herein provide outstanding prospects for the large-scale treatment of oily wastewater.


Assuntos
Carvão Vegetal , Águas Residuárias , Fibra de Carbono , Óleos/química , Esgotos
17.
Chemosphere ; 286(Pt 1): 131640, 2022 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-34315085

RESUMO

The morphology and specific surface area of layered double hydroxide (LDH) are of great significance for optimizing the application of LDH in sewage treatment. Herein, we present a study of the relation between the catalytic property and the morphology of LDH via activating peroxymonosulfate (PMS) for degradation of organic pollutants. The results demonstrated that LDH nanoscrolls possessed a superior performance for methylene blue (MB) degradation, which achieved almost 100% removal in 40 min and the calculated apparent rate constant was about 2.1, 4.5 and 11.5 times higher than that of LDH nanosheets, Co2+ and Co3O4, respectively. According to the results of X-ray photoelectrons spectroscopy (XPS) and electron paramagnetic resonance (EPR), 1O2 was confirmed to play a dominant role in the MB degradation, where the redox cycle of Co3+/Co2+ provided the impetus for the reaction. Moreover, the pH and ion tolerance abilities of LDH nanoscrolls in PMS activating process were determined as well. Remarkably, CO32- and H2PO4- could even promote the generation of •OH and 1O2 to facilitate the progress of reaction. Overall, these findings in the study may provide more opportunities in the preparation of high-efficiency catalysts and give insight into the accelerated degradation of refractory contaminants with surrounding anions.


Assuntos
Hidróxidos , Peróxidos , Catálise , Oxirredução
18.
Environ Technol ; 43(18): 2796-2808, 2022 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-33719927

RESUMO

Developing high-performance adsorbent for hexavalent chromium (Cr(VI)) elimination presents an enticing prospect in environmental remediation. Herein, three-dimensional flowerlike nanospheres composed of molybdenum disulphide and polypyrrole (MoS2@PPy) were successfully prepared via a one-pot hydrothermal and subsequent carbothermal reduction process for the removal of Cr(VI). The effects of pH, adsorbent dosage, co-existing ions, initial Cr(VI) concentration and temperature were investigated systematically by batch experiments. Benefiting from the incorporation of MoS2, the obtained MoS2@PPy composites showed a dramatic increase of specific surface area (149.82 m2·g-1) and adsorption capacity (230.97 mg·g-1) when compared with the pure PPy nanoparticles. Based on the thermodynamics study and X-ray photoelectron spectroscopy analyses, the removal process of Cr(VI) was proved to be exothermic and spontaneous, and accessible under-coordinated Mo(IV) and pyrrolic N groups coupled with redox reactions were conducive to the efficient removal of Cr(VI). Attractively, the MoS2@PPy acted as the electron donor could also activate peroxymonosulphate for the efficient degradation of organic contaminants. These results suggested that the MoS2@PPy was promising in Cr(VI) elimination and other kinds of organic pollutants removal in wastewater.


Assuntos
Nanocompostos , Poluentes Químicos da Água , Adsorção , Cromo/química , Dissulfetos , Concentração de Íons de Hidrogênio , Cinética , Molibdênio/análise , Nanocompostos/química , Polímeros/química , Pirróis/análise , Pirróis/química , Poluentes Químicos da Água/química
19.
Theranostics ; 11(19): 9452-9469, 2021.
Artigo em Inglês | MEDLINE | ID: mdl-34646380

RESUMO

Background: Neuronal death is a major hallmark of Alzheimer's disease (AD). Necroptosis, as a programmed necrotic process, is activated in AD. However, what signals and factors initiate necroptosis in AD is largely unknown. Methods: We examined the expression levels of critical molecules in necroptotic signaling pathway by immunohistochemistry (IHC) staining and immunoblotting using brain tissues from AD patients and AD mouse models of APP/PS1 and 5×FAD. We performed brain stereotaxic injection with recombinant TNF-α, anti-TNFR1 neutralizing antibody or AAV-mediated gene expression and knockdown in APP/PS1 mice. For in vitro studies, we used TNF-α combined with zVAD-fmk and Smac mimetic to establish neuronal necroptosis models and utilized pharmacological or molecular biological approaches to study the signaling pathways. Results: We find that activated neuronal necroptosis is dependent on upstream TNF-α/TNFR1 signaling in both neuronal cell cultures and AD mouse models. Upon TNF-α stimulation, accumulated p62 recruits RIPK1 and induces its self-oligomerization, and activates downstream RIPK1/RIPK3/MLKL cascade, leading to neuronal necroptosis. Ectopic accumulation of p62 is caused by impaired autophagy flux, which is mediated by UVRAG downregulation during the TNF-α-promoted necroptosis. Notably, UVRAG overexpression inhibits neuronal necroptosis in cell and mouse models of AD. Conclusions: We identify a finely controlled regulation of neuronal necroptosis in AD by coordinated TNF-α signaling, RIPK1/3 activity and autophagy machinery. Strategies that could fine-tune necroptosis and autophagy may bring in promising therapeutics for AD.


Assuntos
Doença de Alzheimer/fisiopatologia , Fator de Necrose Tumoral alfa/metabolismo , Proteínas Supressoras de Tumor/fisiologia , Doença de Alzheimer/metabolismo , Animais , Apoptose/efeitos dos fármacos , Proteínas Reguladoras de Apoptose/metabolismo , Autofagia/efeitos dos fármacos , Encéfalo/patologia , Morte Celular/efeitos dos fármacos , Modelos Animais de Doenças , Expressão Gênica , Humanos , Camundongos , Necroptose/fisiologia , Necrose/metabolismo , Neurônios/metabolismo , Proteínas de Ligação a RNA/metabolismo , Proteína Serina-Treonina Quinases de Interação com Receptores/metabolismo , Transdução de Sinais/efeitos dos fármacos , Transcriptoma/genética , Proteínas Supressoras de Tumor/metabolismo
20.
Chemosphere ; 280: 130911, 2021 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-34162124

RESUMO

Developing single-atom Fenton-like catalysts with the maximum utilization of active sites present an attractive potential in environmental remediation. Herein, the single-atom Fe and N co-doped hollow carbon microsphere loaded g-C3N4 catalyst (HFeNC-g-C3N4) was prepared by an innovative cascade anchoring strategy using polystyrene as the hard template, iron phthalocyanine, polydopamine and urea as the Fe, N and C precursor, in which the in-situ generated g-C3N4 could not only effectively anchor Fe atom to create the well-dispersed Fe-Nx active sites, but also accelerate the electron transfer in peroxymonosulfate (PMS) activation. Taking advantages of such sequential protecting strategy, the as-synthesized HFeNC-g-C3N4 catalyst with single-atom Fe-Nx active sites, verified by XRD, XPS and HAADF-STEM, could work as an efficient Fenton-like catalyst for PMS activation, which achieved almost 100% removal of 4-chlorophenol (4-CP) in 5 min with the turnover frequency calculated to be 34.6 times higher than that of the homogeneous Fe2+ catalyst. The mechanism of O2•- dominated radical combined with nonradical 1O2 pathway was confirmed by quenching experiments and ESR analysis, which might be interrelated to the improvement of pH adaptability and interference immunity of HFeNC-g-C3N4/PMS system. Overall, the present findings provided an innovation strategy for the synthesis of excellent single-atom Fe based catalyst in wastewater purification.


Assuntos
Carbono , Ferro , Microesferas , Nitrogênio , Peróxidos
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