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1.
Arq. bras. oftalmol ; 88(1): e2023, 2025. graf
Artículo en Inglés | LILACS-Express | LILACS | ID: biblio-1568848

RESUMEN

ABSTRACT Purpose: The epithelial-mesenchymal transition of human lens epithelial cells plays a role in posterior capsule opacification, a fibrotic process that leads to a common type of cataract. Hyaluronic acid has been implicated in this fibrosis. Studies have investigated the role of transforming growth factor (TGF)-β2 in epithelial-mesenchymal transition. However, the role of TGF-β2 in hyaluronic acid-mediated fibrosis of lens epithelial cell remains unknown. We here examined the role of TGF-β2 in the hyaluronic acid-mediated epithelial-mesenchymal transition of lens epithelial cells. Methods: Cultured human lens epithelial cells (HLEB3) were infected with CD44-siRNA by using the Lipofectamine 3000 transfection reagent. The CCK-8 kit was used to measure cell viability, and the scratch assay was used to determine cell migration. Cell oxidative stress was analyzed in a dichloro-dihydro-fluorescein diacetate assay and by using a flow cytometer. The TGF-β2 level in HLEB3 cells was examined through immunohistochemical staining. The TGF-β2 protein level was determined through western blotting. mRNA expression levels were determined through quantitative real-time polymerase chain reaction. Results: Treatment with hyaluronic acid (1.0 μM, 24 h) increased the epithelial-mesenchymal transition of HLEB3 cells. The increase in TGF-β2 levels corresponded to an increase in CD44 levels in the culture medium. However, blocking the CD44 function significantly reduced the TGF-β2-mediated epithelial-mesenchymal transition response of HLEB3 cells. Conclusions: Our study showed that both CD44 and TGF-β2 are critical contributors to the hyaluronic acid-mediated epithelial-mesenchymal transition of lens epithelial cells, and that TGF-β2 in epithelial-mesenchymal transition is regulated by CD44. These results suggest that CD44 could be used as a target for preventing hyaluronic acid-induced posterior capsule opacification. Our findings suggest that CD44/TGF-β2 is crucial for the hyaluronic acid-induced epithelial-mesenchymal transition of lens epithelial cells.

2.
Arq. bras. oftalmol ; 88(1): e2023, 2025. graf
Artículo en Inglés | LILACS-Express | LILACS | ID: biblio-1568849

RESUMEN

ABSTRACT Unvaccinated identical twins developed bilateral anterior uveitis soon after the onset of coronavirus disease 2019 symptoms. During follow-up, both patients developed choroiditis, and one twine developed posterior scleritis and serous retinal detachment. Prompt treatment with oral prednisone ameliorated the lesions, and no recurrence was observed at the 18-month follow-up. Choroiditis may rarely be associated with severe acute respiratory syndrome coronavirus 2 infection, and it responds well to corticosteroid therapy. Although the exact mechanism is unknown, we hypothesize that the virus may act as an immunological trigger for choroiditis.

3.
J Environ Sci (China) ; 148: 1-12, 2025 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-39095148

RESUMEN

In present work, blue carbon dots (b-CDs) were derived from ammonium citrate and guanidine hydrochloride, and red carbon dots (r-CDs) were stemmed from malonate, ethylenediamine and meso­tetra (4-carboxyphenyl) porphin based on facile hydrothermal method. Eco-friendly ratiometric fluorescence probe was innovatively constructed to effectively measure Hg2+ utilizing b-CDs and r-CDs. The developed probe displayed two typical emission peaks at 450 nm from b-CDs and 650 nm from r-CDs under the excitation at 360 nm. Mercury ion has strong quenching effect on the fluorescence intensity at 450 nm due to the electron transfer process and the fluorescence change at 450 nm was used as the response signal, whereas the fluorescence intensity at 650 nm kept unchangeable which resulted from the chemical inertness between Hg2+ and r-CDs, serving as the reference signal in the sensing system. Under optimal circumstances, this probe exhibited an excellent linearity between the fluorescence response values of ΔF450/F650 and Hg2+ concentrations over range of 0.01-10 µmol/L, and the limit of detection was down to 5.3 nmol/L. Furthermore, this probe was successfully employed for sensing Hg2+ in practical environmental water samples with satisfied recoveries of 98.5%-105.0%. The constructed ratiometric fluorescent probe provided a rapid, environmental-friendly, reliable, and efficient platform for measuring trace Hg2+ in environmental field.


Asunto(s)
Carbono , Colorantes Fluorescentes , Mercurio , Puntos Cuánticos , Contaminantes Químicos del Agua , Mercurio/análisis , Carbono/química , Colorantes Fluorescentes/química , Contaminantes Químicos del Agua/análisis , Puntos Cuánticos/química , Monitoreo del Ambiente/métodos , Espectrometría de Fluorescencia/métodos , Límite de Detección , Fluorescencia
4.
J Environ Sci (China) ; 148: 116-125, 2025 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-39095150

RESUMEN

Perfluoroalkyl substances (PFASs) are typical persistent organic pollutants, and their removal is urgently required but challenging. Photocatalysis has shown potential in PFASs degradation due to the redox capabilities of photoinduced charge carriers in photocatalysts. Herein, hexagonal ZnIn2S4 (ZIS) nanosheets were synthesized by a one-pot oil bath method and were well characterized by a series of techniques. In the degradation of sodium p-perfluorous nonenoxybenzenesulfonate (OBS), one kind of representative PFASs, the as-synthesized ZIS showed activity superior to P25 TiO2 under both simulated sunlight and visible-light irradiation. The good photocatalytic performance was attributed to the enhanced light absorption and facilitated charge separation. The pH conditions were found crucial in the photocatalytic process by influencing the OBS adsorption on the ZIS surface. Photogenerated e- and h+ were the main active species involved in OBS degradation in the ZIS system. This work confirmed the feasibility and could provide mechanistic insights into the degradation and defluorination of PFASs by visible-light photocatalysis.


Asunto(s)
Fluorocarburos , Luz , Fotólisis , Fluorocarburos/química , Nanoestructuras/química , Catálisis , Contaminantes Químicos del Agua/química , Zinc/química , Indio/química , Modelos Químicos
5.
J Environ Sci (China) ; 148: 174-187, 2025 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-39095155

RESUMEN

Cost-effective CO2 adsorbents are gaining increasing attention as viable solutions for mitigating climate change. In this study, composites were synthesized by electrochemically combining the post-gasification residue of Macadamia nut shell with copper benzene-1,3,5-tricarboxylate (CuBTC). Among the different composites synthesized, the ratio of 1:1 between biochar and CuBTC (B 1:1) demonstrated the highest CO2 adsorption capacity. Under controlled laboratory conditions (0°C, 1 bar, without the influence of ambient moisture or CO2 diffusion limitations), B 1:1 achieved a CO2 adsorption capacity of 9.8 mmol/g, while under industrial-like conditions (25°C, 1 bar, taking into account the impact of ambient moisture and CO2 diffusion limitations within a bed of adsorbent), it reached 6.2 mmol/g. These values surpassed those reported for various advanced CO2 adsorbents investigated in previous studies. The superior performance of the B 1:1 composite can be attributed to the optimization of the number of active sites, porosity, and the preservation of the full physical and chemical surface properties of both parent materials. Furthermore, the composite exhibited a notable CO2/N2 selectivity and improved stability under moisture conditions. These favorable characteristics make B 1:1 a promising candidate for industrial applications.


Asunto(s)
Dióxido de Carbono , Estructuras Metalorgánicas , Dióxido de Carbono/química , Adsorción , Estructuras Metalorgánicas/química , Contaminantes Atmosféricos/química , Carbón Orgánico/química
6.
J Environ Sci (China) ; 148: 399-408, 2025 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-39095175

RESUMEN

A mixed oxidant of chlorine dioxide (ClO2) and NaClO was often used in water treatment. A novel UVA-LED (365 nm)-activated mixed ClO2/NaClO process was proposed for the degradation of micropollutants in this study. Carbamazepine (CBZ) was selected as the target pollutant. Compared with the UVA365/ClO2 process, the UVA365/ClO2/NaClO process can improve the degradation of CBZ, with the rate constant increasing from 2.11×10-4 sec-1 to 2.74×10-4 sec-1. In addition, the consumption of oxidants in the UVA365/ClO2/NaClO process (73.67%) can also be lower than that of UVA365/NaClO (86.42%). When the NaClO ratio increased, both the degradation efficiency of CBZ and the consumption of oxidants can increase in the UVA365/ClO2/NaClO process. The solution pH can affect the contribution of NaClO in the total oxidant ratio. When the pH range of 6.0-8.0, the combination process can generate more active species to promote the degradation of CBZ. The change of active species with oxidant molar ratio was investigated in the UVA365/ClO2/NaClO process. When ClO2 acted as the main oxidant, HO• and Cl• were the main active species, while when NaClO was the main oxidant, ClO• played a role in the system. Both chloride ion (Cl-), bicarbonate ion (HCO3-), and nitrate ion (NO3-) can promote the reaction system. As the concentration of NaClO in the reaction solution increased, the generation of chlorates will decrease. The UVA365/ClO2/NaClO process can effectively control the formation of volatile disinfection by-products (DBPs), and with the increase of ClO2 dosage, the formation of DBPs can also decrease.


Asunto(s)
Carbamazepina , Compuestos de Cloro , Óxidos , Rayos Ultravioleta , Contaminantes Químicos del Agua , Purificación del Agua , Carbamazepina/química , Contaminantes Químicos del Agua/química , Compuestos de Cloro/química , Purificación del Agua/métodos , Óxidos/química , Cinética , Hipoclorito de Sodio/química , Modelos Químicos
7.
J Environ Sci (China) ; 148: 476-488, 2025 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-39095182

RESUMEN

In this study, non-thermal plasma (NTP) was employed to modify the Cu/TiO2 adsorbent to efficiently purify H2S in low-temperature and micro-oxygen environments. The effects of Cu loading amounts and atmospheres of NTP treatment on the adsorption-oxidation performance of the adsorbents were investigated. The NTP modification successfully boosted the H2S removal capacity to varying degrees, and the optimized adsorbent treated by air plasma (Cu/TiO2-Air) attained the best H2S breakthrough capacity of 113.29 mg H2S/gadsorbent, which was almost 5 times higher than that of the adsorbent without NTP modification. Further studies demonstrated that the superior performance of Cu/TiO2-Air was attributed to increased mesoporous volume, more exposure of active sites (CuO) and functional groups (amino groups and hydroxyl groups), enhanced Ti-O-Cu interaction, and the favorable ratio of active oxygen species. Additionally, the X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) results indicated the main reason for the deactivation was the consumption of the active components (CuO) and the agglomeration of reaction products (CuS and SO42-) occupying the active sites on the surface and the inner pores of the adsorbents.


Asunto(s)
Cobre , Sulfuro de Hidrógeno , Oxidación-Reducción , Titanio , Titanio/química , Adsorción , Cobre/química , Sulfuro de Hidrógeno/química , Contaminantes Atmosféricos/química , Gases em Plasma/química , Modelos Químicos
8.
J Environ Sci (China) ; 148: 489-501, 2025 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-39095183

RESUMEN

The chemistry of sulfur cycle contributes significantly to the atmospheric nucleation process, which is the first step of new particle formation (NPF). In the present study, cycloaddition reaction mechanism of sulfur trioxide (SO3) to hydrogen sulfide (H2S) which is a typical air pollutant and toxic gas detrimental to the environment were comprehensively investigate through theoretical calculations and Atmospheric Cluster Dynamic Code simulations. Gas-phase stability and nucleation potential of the product thiosulfuric acid (H2S2O3, TSA) were further analyzed to evaluate its atmospheric impact. Without any catalysts, the H2S + SO3 reaction is infeasible with a barrier of 24.2 kcal/mol. Atmospheric nucleation precursors formic acid (FA), sulfuric acid (SA), and water (H2O) could effectively lower the reaction barriers as catalysts, even to a barrierless reaction with the efficiency of cis-SA > trans-FA > trans-SA > H2O. Subsequently, the gas-phase stability of TSA was investigated. A hydrolysis reaction barrier of up to 61.4 kcal/mol alone with an endothermic isomerization reaction barrier of 5.1 kcal/mol under the catalytic effect of SA demonstrates the sufficient stability of TSA. Furthermore, topological and kinetic analysis were conducted to determine the nucleation potential of TSA. Atmospheric clusters formed by TSA and atmospheric nucleation precursors (SA, ammonia NH3, and dimethylamine DMA) were thermodynamically stable. Moreover, the gradually decreasing evaporation coefficients for TSA-base clusters, particularly for TSA-DMA, suggests that TSA may participate in NPF where the concentration of base molecules are relatively higher. The present new reaction mechanism may contributes to a better understanding of atmospheric sulfur cycle and NPF.


Asunto(s)
Contaminantes Atmosféricos , Sulfuro de Hidrógeno , Modelos Químicos , Sulfuro de Hidrógeno/química , Contaminantes Atmosféricos/química , Reacción de Cicloadición , Atmósfera/química , Óxidos de Azufre/química , Cinética , Azufre/química
9.
J Environ Sci (China) ; 148: 57-68, 2025 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-39095190

RESUMEN

The expandable graphite (EG) modified TiO2 nanocomposites were prepared by the high shear method using the TiO2 nanoparticles (NPs) and EG as precursors, in which the amount of EG doped in TiO2 was 10 wt.%. Followed by the impregnation method, adjusting the pH of the solution to 10, and using the electrostatic adsorption to achieve spatial confinement, the Pt elements were mainly distributed on the exposed TiO2, thus generating the Pt/10EG-TiO2-10 catalyst. The best CO oxidation activity with the excellent resistance to H2O and SO2 was obtained over the Pt/10EG-TiO2-10 catalyst: CO conversion after 36 hr of the reaction was ca. 85% under the harsh condition of 10 vol.% H2O and 100 ppm SO2 at a high gaseous hourly space velocity (GHSV) of 400,000 hr-1. Physicochemical properties of the catalysts were characterized by various techniques. The results showed that the electrostatic adsorption, which riveted the Pt elements mainly on the exposed TiO2 of the support surface, reduced the dispersion of Pt NPs on EG and achieved the effective dispersion of Pt NPs, hence significantly improving CO oxidation activity over the Pt/10EG-TiO2-10 catalyst. The 10 wt.% EG doped in TiO2 caused the TiO2 support to form a more hydrophobic surface, which reduced the adsorption of H2O and SO2 on the catalyst, greatly inhibited deposition of the TiOSO4 and formation of the PtSO4 species as well as suppressed the oxidation of SO2, thus resulting in an improvement in the resistance to H2O and SO2 of the Pt/10EG-TiO2-10 catalyst.


Asunto(s)
Grafito , Oxidación-Reducción , Platino (Metal) , Dióxido de Azufre , Titanio , Titanio/química , Grafito/química , Dióxido de Azufre/química , Platino (Metal)/química , Catálisis , Monóxido de Carbono/química , Agua/química , Contaminantes Atmosféricos/química , Modelos Químicos
10.
J Environ Sci (China) ; 148: 650-664, 2025 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-39095197

RESUMEN

China is the most important steel producer in the world, and its steel industry is one of the most carbon-intensive industries in China. Consequently, research on carbon emissions from the steel industry is crucial for China to achieve carbon neutrality and meet its sustainable global development goals. We constructed a carbon dioxide (CO2) emission model for China's iron and steel industry from a life cycle perspective, conducted an empirical analysis based on data from 2019, and calculated the CO2 emissions of the industry throughout its life cycle. Key emission reduction factors were identified using sensitivity analysis. The results demonstrated that the CO2 emission intensity of the steel industry was 2.33 ton CO2/ton, and the production and manufacturing stages were the main sources of CO2 emissions, accounting for 89.84% of the total steel life-cycle emissions. Notably, fossil fuel combustion had the highest sensitivity to steel CO2 emissions, with a sensitivity coefficient of 0.68, reducing the amount of fossil fuel combustion by 20% and carbon emissions by 13.60%. The sensitivities of power structure optimization and scrap consumption were similar, while that of the transportation structure adjustment was the lowest, with a sensitivity coefficient of less than 0.1. Given the current strategic goals of peak carbon and carbon neutrality, it is in the best interest of the Chinese government to actively promote energy-saving and low-carbon technologies, increase the ratio of scrap steel to steelmaking, and build a new power system.


Asunto(s)
Dióxido de Carbono , Huella de Carbono , Acero , China , Dióxido de Carbono/análisis , Contaminantes Atmosféricos/análisis , Metalurgia , Monitoreo del Ambiente , Industrias , Contaminación del Aire/estadística & datos numéricos , Contaminación del Aire/prevención & control
11.
Methods Mol Biol ; 2854: 153-170, 2025.
Artículo en Inglés | MEDLINE | ID: mdl-39192127

RESUMEN

cGAS is a key cytosolic dsDNA receptor that senses viral infection and elicits interferon production through the cGAS-cGAMP-STING axis. cGAS is activated by dsDNA from viral and bacterial origins as well as dsDNA leaked from damaged mitochondria and nucleus. Eventually, cGAS activation launches the cell into an antiviral state to restrict the replication of both DNA and RNA viruses. Throughout the long co-evolution, viruses devise many strategies to evade cGAS detection or suppress cGAS activation. We recently reported that the Dengue virus protease NS2B3 proteolytically cleaves human cGAS in its N-terminal region, effectively reducing cGAS binding to DNA and consequent production of the second messenger cGAMP. Several other RNA viruses likely adopt the cleavage strategy. Here, we describe a protocol for the purification of recombinant human cGAS and Dengue NS2B3 protease, as well as the in vitro cleavage assay.


Asunto(s)
Virus del Dengue , Nucleotidiltransferasas , Proteínas no Estructurales Virales , Humanos , Proteínas no Estructurales Virales/metabolismo , Nucleotidiltransferasas/metabolismo , Nucleotidiltransferasas/antagonistas & inhibidores , Proteolisis , Proteínas Recombinantes/metabolismo , Proteínas Recombinantes/genética , Proteínas Recombinantes/aislamiento & purificación , Nucleótidos Cíclicos/metabolismo , Dengue/virología , Dengue/metabolismo
12.
Methods Mol Biol ; 2854: 265-282, 2025.
Artículo en Inglés | MEDLINE | ID: mdl-39192136

RESUMEN

Protein kinase R (PKR), a key double-stranded RNA (dsRNA)-activated sensor, is pivotal for cellular responses to diverse stimuli. This protocol delineates a comprehensive methodological framework employing single luciferase assays, yeast assays, immunoblot assays, and quantitative PCR (qPCR) to discern and validate PKR activities and their downstream impacts on NF-κB-activating signaling pathways. These methodologies furnish a systematic approach to unraveling the role of PKR as a dsRNA sensor and effector in antiviral innate immunity, enabling in-depth analyses of dsRNA sensor activities.


Asunto(s)
Inmunidad Innata , ARN Bicatenario , eIF-2 Quinasa , eIF-2 Quinasa/metabolismo , eIF-2 Quinasa/genética , ARN Bicatenario/inmunología , ARN Bicatenario/genética , Humanos , FN-kappa B/metabolismo , Transducción de Señal , Animales
13.
J Environ Sci (China) ; 149: 177-187, 2025 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-39181632

RESUMEN

In the context of peaking carbon dioxide emissions and carbon neutrality, development of feasible methods for converting CO2 into high value-added chemicals stands out as a hot subject. In this study, P[D+COO-][Br-][DBUH+], a series of novel heterogeneous dual-ionic poly(ionic liquid)s (PILs) were synthesized readily from 2-(dimethylamino) ethyl methacrylate (DMAEMA), bromo-substituted aliphatic acids, organic bases and divinylbenzene (DVB). The structures, compositions and morphologies were characterized or determined by nuclear magnetic resonance (NMR), thermal gravimetric analysis (TGA), infrared spectroscopy (IR), scanning electron microscopes (SEM), and Brunauer-Emmett-Teller analysis (BET), etc. Application of the P[D+COO-][Br-][DBUH+] series as catalysts in converting CO2 into cyclic carbonates showed that P[D+COO-][Br-][DBUH+]-2/1/0.6 was able to catalyze epiclorohydrin-CO2 cycloaddition the most efficiently. This afforded chloropropylene carbonate (CPC) in 98.4% yield with ≥ 99% selectivity in 24 hr under solvent- and additive-free conditions at atmospheric pressure. Reusability experiments showed that recycling of the catalyst 6 times only resulted in a slight decline in the catalytic performance. In addition, it could be used for the synthesis of a variety of differently substituted cyclic carbonates in good to excellent yields. Finally, key catalytic active sites were probed, and a reasonable mechanism was proposed accordingly. In summary, this work poses an efficient strategy for heterogenization of dual-ionic PILs and provides a mild and environmentally benign approach to the fixation and utilization of carbon dioxide.


Asunto(s)
Dióxido de Carbono , Carbonatos , Líquidos Iónicos , Líquidos Iónicos/química , Dióxido de Carbono/química , Carbonatos/química , Catálisis , Modelos Químicos
14.
J Environ Sci (China) ; 149: 234-241, 2025 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-39181638

RESUMEN

Reducing the cost of RuO2/TiO2 catalysts is still one of the urgent challenges in catalytic HCl oxidation. In the present work, a Ce-doped TiO2 supported RuO2 catalyst with a low Ru loading was developed, showing a high activity in the catalytic oxidation of HCl to Cl2. The results on some extensive characterizations of both Ce-doped TiO2 carriers and their supported RuO2 catalysts show that the doping of Ce into TiO2 can effectively change the lattice parameters of TiO2 to improve the dispersion of the active RuO2 species on the carrier, which facilitates the production of surface Ru species to expose more active sites for boosting the catalytic performance even under some harsh reaction conditions. This work provides some scientific basis and technical support for chlorine recycling.


Asunto(s)
Cerio , Ácido Clorhídrico , Oxidación-Reducción , Titanio , Titanio/química , Catálisis , Cerio/química , Ácido Clorhídrico/química , Compuestos de Rutenio/química , Cloruros/química , Modelos Químicos , Cloro/química
15.
J Environ Sci (China) ; 149: 330-341, 2025 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-39181646

RESUMEN

The emission of heavy-duty vehicles has raised great concerns worldwide. The complex working and loading conditions, which may differ a lot from PEMS tests, raised new challenges to the supervision and control of emissions, especially during real-world applications. On-board diagnostics (OBD) technology with data exchange enabled and strengthened the monitoring of emissions from a large number of heavy-duty diesel vehicles. This paper presents an analysis of the OBD data collected from more than 800 city and highway heavy-duty vehicles in China using remote OBD data terminals. Real-world NOx and CO2 emissions of China-6 heavy-duty vehicles have been examined. The results showed that city heavy-duty vehicles had higher NOx emission levels, which was mostly due to longer time of low SCR temperatures below 180°C. The application of novel methods based on 3B-MAW also found that heavy-duty diesel vehicles tended to have high NOx emissions at idle. Also, little difference had been found in work-based CO2 emissions, and this may be due to no major difference were found in occupancies of hot running.


Asunto(s)
Contaminantes Atmosféricos , Dióxido de Carbono , Monitoreo del Ambiente , Óxidos de Nitrógeno , Emisiones de Vehículos , Emisiones de Vehículos/análisis , China , Contaminantes Atmosféricos/análisis , Dióxido de Carbono/análisis , Monitoreo del Ambiente/métodos , Óxidos de Nitrógeno/análisis , Ciudades , Contaminación del Aire/estadística & datos numéricos , Contaminación del Aire/análisis , Gasolina/análisis
16.
J Environ Sci (China) ; 149: 35-45, 2025 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-39181648

RESUMEN

Post-etching method using dilute acid solutions is an effective technology to modulate the surface compositions of metal-oxide catalysts. Here the α-MnO2 catalyst treated with 0.1 mol/L nitric acid exhibits higher ozone decomposition activity at high relative humidity than the counterpart treated with acetic acid. Besides the increases in surface area and lattice dislocation, the improved activity can be due to relatively higher Mn valence on the surface and newly-formed Brønsted acid sites adjacent to oxygen vacancies. The remnant nitro species deposited on the catalyst by nitric acid treatment is ideal hydrophobic groups at ambient conditions. The decomposition route is also proposed based on the DRIFTS and DFT calculations: ozone is facile to adsorb on the oxygen vacancy, and the protonic H of Brønsted acid sites bonds to the terminal oxygen of ozone to accelerate its cleavage to O2, reducing the reaction energy barrier of O2 desorption.


Asunto(s)
Humedad , Compuestos de Manganeso , Óxidos , Ozono , Ozono/química , Óxidos/química , Compuestos de Manganeso/química , Catálisis , Modelos Químicos
17.
J Environ Sci (China) ; 149: 374-385, 2025 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-39181650

RESUMEN

Electrocatalytic reduction of nitrate to ammonia has been considered a promising and sustainable pathway for pollutant treatment and ammonia has significant potential as a clean energy. Therefore, the method has received much attention. In this work, Cu/Fe 2D bimetallic metal-organic frameworks were synthesized by a facile method applied as cathode materials without high-temperature carbonization. Bimetallic centers (Cu, Fe) with enhanced intrinsic activity demonstrated higher removal efficiency. Meanwhile, the 2D nanosheet reduced the mass transfer barrier between the catalyst and nitrate and increased the reaction kinetics. Therefore, the catalysts with a 2D structure showed much better removal efficiency than other structures (3D MOFs and Bulk MOFs). Under optimal conditions, Cu/Fe-2D MOF exhibited high nitrate removal efficiency (87.8%) and ammonium selectivity (89.3%) simultaneously. The ammonium yielded up to significantly 907.2 µg/(hr·mgcat) (7793.8 µg/(hr·mgmetal)) with Faradaic efficiency of 62.8% at an initial 100 mg N/L. The catalyst was proved to have good stability and was recycled 15 times with excellent effect. DFT simulations confirm the reduced Gibbs free energy of Cu/Fe-2D MOF. This study demonstrates the promising application of Cu/Fe-2D MOF in nitrate reduction to ammonia and provides new insights for the design of efficient electrode materials.


Asunto(s)
Amoníaco , Cobre , Hierro , Estructuras Metalorgánicas , Nitratos , Contaminantes Químicos del Agua , Amoníaco/química , Cobre/química , Nitratos/química , Estructuras Metalorgánicas/química , Hierro/química , Contaminantes Químicos del Agua/química , Catálisis , Modelos Químicos , Oxidación-Reducción , Cinética
18.
J Environ Sci (China) ; 149: 512-523, 2025 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-39181663

RESUMEN

Oxygen activation leading to the generation of reactive oxygen species (ROS) is essential for photocatalytic environmental remediation. The limited efficiency of O2 adsorption and reductive activation significantly limits the production of ROS when employing C3N4 for the degradation of emerging pollutants. Doping with metal single atoms may lead to unsatisfactory efficiency, due to the recombination of photogenerated electron-hole pairs. Here, Mn and S single atoms were introduced into C3N4, resulting in the excellent photocatalytic performances. Mn/S-C3N4 achieved 100% removal of bisphenol A, with a rate constant 11 times that of pristine C3N4. According to the experimental results and theoretical simulations, S-atoms restrict holes, facilitating the photo-generated carriers' separation. Single-atom Mn acts as the O2 adsorption site, enhancing the adsorption and activation of O2, resulting the generation of ROS. This study presents a novel approach for developing highly effective photocatalysts that follows a new mechanism to eliminate organic pollutants from water.


Asunto(s)
Oxígeno , Contaminantes Químicos del Agua , Contaminantes Químicos del Agua/química , Oxígeno/química , Catálisis , Manganeso/química , Compuestos de Bencidrilo/química , Nitrilos/química , Adsorción , Especies Reactivas de Oxígeno , Restauración y Remediación Ambiental/métodos , Fenoles/química
19.
J Environ Sci (China) ; 149: 574-584, 2025 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-39181669

RESUMEN

The formation of oligomeric hydrogen peroxide triggered by Criegee intermediate maybe contributes significantly to the formation and growth of secondary organic aerosol (SOA). However, to date, the reactivity of C2 Criegee intermediates (CH3CHOO) in areas contaminated with acidic gas remains poorly understood. Herein, high-level quantum chemical calculations and Born-Oppenheimer molecular dynamics (BOMD) simulations are used to explore the reaction of CH3CHOO and H2SO4 both in the gas phase and at the air-water interface. In the gas phase, the addition reaction of CH3CHOO with H2SO4 to generate CH3HC(OOH)OSO3H (HPES) is near-barrierless, regardless of the presence of water molecules. BOMD simulations show that the reaction at the air-water interface is even faster than that in the gas phase. Further calculations reveal that the HPES has a tendency to aggregate with sulfuric acids, ammonias, and water molecules to form stable clusters, meanwhile the oligomerization reaction of CH3CHOO with HPES in the gas phase is both thermochemically and kinetically favored. Also, it is noted that the interfacial HPES- ion can attract H2SO4, NH3, (COOH)2 and HNO3 for particle formation from the gas phase to the water surface. Thus, the results of this work not only elucidate the high atmospheric reactivity of C2 Criegee intermediates in polluted regions, but also deepen our understanding of the formation process of atmospheric SOA induced by Criegee intermediates.


Asunto(s)
Ácidos Sulfúricos , Ácidos Sulfúricos/química , Aerosoles , Modelos Químicos , Contaminantes Atmosféricos/química , Simulación de Dinámica Molecular , Atmósfera/química
20.
J Environ Sci (China) ; 149: 535-550, 2025 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-39181665

RESUMEN

Li6ZnO4 was chemically modified by nickel addition, in order to develop different compositions of the solid solution Li6Zn1-xNixO4. These materials were evaluated bifunctionally; analyzing their CO2 capture performances, as well as on their catalytic properties for H2 production via dry reforming of methane (DRM). The crystal structures of Li6Zn1-xNixO4 solid solution samples were determined through X-ray diffraction, which confirmed the integration of nickel ions up to a concentration around 20 mol%, meanwhile beyond this value, a secondary phase was detected. These results were supported by XPS and TEM analyses. Then, dynamic and isothermal thermogravimetric analyses of CO2 capture revealed that Li6Zn1-xNixO4 solid solution samples exhibited good CO2 chemisorption efficiencies, similarly to the pristine Li6ZnO4 chemisorption trends observed. Moreover, a kinetic analysis of CO2 isothermal chemisorptions, using the Avrami-Erofeev model, evidenced an increment of the constant rates as a function of the Ni content. Since Ni2+ ions incorporation did not reduce the CO2 capture efficiency and kinetics, the catalytic properties of these materials were evaluated in the DRM process. Results demonstrated that nickel ions favored hydrogen (H2) production over the pristine Li6ZnO4 phase, despite a second H2 production reaction was determined, methane decomposition. Thereby, Li6Zn1-xNixO4 ceramics can be employed as bifunctional materials.


Asunto(s)
Dióxido de Carbono , Hidrógeno , Metano , Hidrógeno/química , Metano/química , Dióxido de Carbono/química , Níquel/química , Catálisis , Modelos Químicos
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