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2.
Sci Total Environ ; 923: 171476, 2024 May 01.
Artículo en Inglés | MEDLINE | ID: mdl-38458471

RESUMEN

DOM (dissolved organic matter) play a crucial role in lakes' geochemical and carbon cycles. Eutrophication evolution would influence nutrient status of waters and investigating the DOM variation helps a better understanding of bioremediation on environmental behavior of DOM in eutrophic lakes. In our study, the contents, compositions and characteristics of systematic DOM&SOM (sediment organic matter) were greatly influenced by seasonal changes. But the effective bioremediations obviously reduced the DOM concentration and thus mitigated the eutrophication outbreak risks in water bodies due to the increased MBC (microbial biomass carbon), microbial activity and metabolism. In early summer, the overall DOM in each treatment were readily low levels and derived from both autochthonous and exogenous origins, dominated by fulvic acid-like. In midsummer, the DOM contents and characteristics in each treatment increased significantly as phytoplankton activity improved, and the majority of DOM were humic acid-like and mainly of biological origin. The greatest differences of enzymes, MBC, microbial metabolism and DOM&SOM removal among different treatments were observed in summer months. In autumn, the systematic DOM&SOM slightly reduced due to the deceased microbial activity, in which the microbial humic acids were main component and derived from endogenous sources. Additionally, the gradually decreased SOM with cultivated time in each treatment was a result of microbiological conversion of SOM into DOM. For various treatments, BE, BE.A, BE.C and BE.E increased the MBC, enzymatic and microbial activities due to the application of biochar-supported EMs. Among these, BE and BE.A, especially BE.A with oxygen supplement, achieved the most desirable effect on reducing systematic DOM&SOM levels and increasing enzymatic and microbial activities. The group of EM also reduced the levels of DOM&SOM as improved degradation of EMs for DOM. However, BC, BE.C and BE.E finally did not achieved the desirable effect on reducing DOM&SOM due to the suppression of microbial activities, respectively, from high dose of biochar, weakening of dominant species and additional introduction of EMs in low liveness.


Asunto(s)
Materia Orgánica Disuelta , Lagos , Lagos/química , Estaciones del Año , Carbón Orgánico , Sustancias Húmicas/análisis
3.
J Am Chem Soc ; 146(10): 6466-6470, 2024 Mar 13.
Artículo en Inglés | MEDLINE | ID: mdl-38428040

RESUMEN

N-heterocyclic carbenes (NHCs) have been extensively studied to modulate the reactivity of molecular catalysts, colloids, and their supported analogues, being isolated sites, clusters, or nanoparticles. While the interaction of NHCs on metal surfaces has been discussed in great detail, showing specific coordination chemistry depending on the type of NHC ligands, much less is known when the metal is dispersed on oxide supports, as in heterogeneous catalysts. Herein, we study the interaction of NHC ligands with Au surface sites dispersed on silica, a nonreducible oxide support. We identify the easy formation of bis-NHC ligated Au(I) surface sites parallel to what is found on metallic Au surfaces. These species display a specific 13C NMR spectroscopic signature that clearly distinguishes them from the mono-NHC Au(I) surface sites or supported imidazoliums. We find that bis-ligated surface species are not unique to supported Au(I) species and are found for the corresponding Ag(I) and Cu(I) species, as well as for the isolobal surface silanols. Furthermore, the interaction of NHC ligand with silica-supported Au nanoparticles also yields bis-NHC ligated Au(I) surface sites, indicating that metal atoms can also be easily extracted from nanoparticles, further illustrating the dynamics of these systems and the overall favorable formation of such bis-ligated species across a range of systems, besides what has been found on crystalline metal facets.

4.
Chem Sci ; 15(8): 3028-3032, 2024 Feb 22.
Artículo en Inglés | MEDLINE | ID: mdl-38404381

RESUMEN

Molecular-level understanding of the acid/base properties of heterogeneous catalysts requires the development of selective spectroscopic probes to establish structure-activity relationships. In this work we show that substituting the surface protons in oxide supports by isolobal N-heterocyclic carbene (NHC) Ag cations and measuring their 109Ag nuclear magnetic resonance (NMR) signatures enables to probe the speciation and to evaluate the corresponding Brønsted acidity of the substituted OH surface sites. Specifically, a series of silver N-heterocyclic carbene (NHC) Ag(i) complexes of general formula [(NHC)AgX] are synthesized and characterized, showing that the 109Ag NMR chemical shift of the series correlates with the Brønsted acidity of the conjugate acid of X- (i.e., HX), thus establishing an acidity scale based on 109Ag NMR chemical shift. The methodology is then used to evaluate the Brønsted acidity of the OH sites of representative oxide materials using Dynamic Nuclear Polarization (DNP-)enhanced solid-state NMR spectroscopy.

5.
Sci Total Environ ; 916: 170101, 2024 Mar 15.
Artículo en Inglés | MEDLINE | ID: mdl-38242474

RESUMEN

The presence of residual antibiotics in the environment is a prominent issue. Photodegradation behavior is an important way of antibiotics reduction, which is closely related to dissolved organic matter (DOM) in water. The review provides an overview of the latest advancements in the field. Classification, characterization of DOM, and the dominant mechanisms for antibiotic photodegradation were discussed. Furthermore, it summarized and compared the effects of DOM on different antibiotics photodegradation. Moreover, the review comprehensively considered the factors influencing the photodegradation of antibiotics in the aquatic environment, including the characteristics of light, temperature, dosage of DOM, concentration of antibiotics, solution pH, and the presence of coexisting ions. Finally, potential directions were proposed for the development of predictive models for the photodegradation of antibiotics. Based on the review of existing literature, this paper also considered several pathways for the future study of antibiotic photodegradation. This study allows for a better understanding of the DOM's environmental role and provides important new insights into the photochemical fate of antibiotics in the aquatic environment.


Asunto(s)
Antibacterianos , Contaminantes Químicos del Agua , Materia Orgánica Disuelta , Fotólisis , Contaminantes Químicos del Agua/química , Agua/química
6.
J Hazard Mater ; 465: 133098, 2024 Mar 05.
Artículo en Inglés | MEDLINE | ID: mdl-38064949

RESUMEN

In mineral-rich areas, eutrophic lakes are at risk of HMs pollution. However, few papers focused on the repair of HMs in eutrophic environment. Our study analyzed multiple forms of HMs, pore structure and microbial responses in the water-sediment system of eutrophic lake treated with biochar, Effective Microorganisms (EMs) or/and microplastics (MPs). As biochar provided an ideal carrier for EMs, the remediation of biochar-supported EMs (BE) achieved the greatest repairment that improved the bacterial indexes and greatly decreased the most HMs in various forms across the water-sediment system, and it also reduced metal mobility, bioavailability and ecological risk. The addition of aged MPs (MP) stimulated the microbial activity and significantly reduced the HMs levels in different forms due to the adsorption of biofilms/EPS adhered on MPs, but it increased metals mobility and ecological risks. The strong adsorption and high mobility of aged MPs would increase enrichment of HMs and cause serious ecological hazards. The incorporation of BE and MP (MBE) also greatly reduced the HMs in full forms, which was primarily ascribed to the adsorption of superfluous biofilms/EPS, but it distinctly depressed the microbial activity. The single addition of biochar and EMs resulted in the inability of HMs to be adsorbed due to the preferentially adsorption of dissolved nutrients and the absence of effective carrier, respectively. In the remediation cases, the remarkable removal of HMs was principally accomplished by the adsorption of HMs with molecular weight below 100 kDa, especially 3 kDa ∼100 kDa, which had higher specific surfaces and abundant active matters, resulting in higher adsorption onto biofilms/EPS.


Asunto(s)
Carbón Orgánico , Metales Pesados , Microplásticos , Plásticos , Lagos , Metales Pesados/análisis , Agua
7.
Angew Chem Int Ed Engl ; 62(50): e202312713, 2023 Dec 11.
Artículo en Inglés | MEDLINE | ID: mdl-37869935

RESUMEN

Converting colloidal nanocrystals (NCs) into devices for various applications is facilitated by designing and controlling their surface properties. One key strategy for tailoring surface properties is thus to choose tailored surface ligands. In that context, amines have been universally used, with the goal to improve NCs synthesis, processing and performances. However, understanding the nature of surface sites in amine-capped NCs remains challenging, due to the complex surface compositions as well as surface ligands dynamic. Here, we investigate both surface sites and amine ligation in CdSe NCs by combining advanced NMR spectroscopy and computational modelling. Notably, dynamic nuclear polarization (DNP) enhanced 113 Cd and 77 Se 1D NMR helps to identify both bulk and surface sites of NCs, while 113 Cd 2D NMR spectroscopy enables to resolve amines terminated sites on both Se-rich and nonpolar surfaces. In addition to directly bonding to surface sites, amines are shown to also interact through hydrogen-bonding with absorbed water as revealed by 15 N NMR, augmented with computations. The characterization methodology developed for this work provides unique molecular-level insight into the surface sites of a range of amine-capped CdSe NCs, and paves the way to identify structure-function relationships and rational approaches towards colloidal NCs with tailored properties.

8.
Sci Rep ; 13(1): 14820, 2023 Sep 08.
Artículo en Inglés | MEDLINE | ID: mdl-37684297

RESUMEN

Carbon doping in GaN-on-Silicon (Si) epitaxial layers is an essential way to reduce leakage current and improve breakdown voltage. However, complicated occupy forms caused by carbon lead to hard analysis leakage/breakdown mechanisms of GaN-on-Si epitaxial layers. In this paper, we demonstrate the space charge distribution and intensity in GaN-on-Si epitaxial layers from 0 to 448 V by simulation. Depending on further monitoring of the trapped charge density of CN and CGa in carbon-doped GaN at 0.1 µm, 0.2 µm, 1.8 µm and 1.9 µm from unintentionally doped GaN/carbon-doped GaN interface, we discuss the relationship between space charge and plateau, breakdown at CN concentrations from 6 × 1016 cm-3 to 6 × 1018 cm-3. The results show that CN in different positions of carbon-doped GaN exhibits significantly different capture and release behaviors. By utilizing the capture and release behavior differences of CN at different positions in carbon-doped GaN, the blocking effect of space charge at unintentionally doped GaN/carbon-doped GaN interface on electron conduction was demonstrated. The study would help to understand the behavior of CN and CGa in GaN-on-Si epitaxial layers and more accurate control of CN and CGa concentration at different positions in carbon-doped GaN to improve GaN-on-Si device performance.

9.
ACS Appl Mater Interfaces ; 15(28): 34272-34289, 2023 Jul 19.
Artículo en Inglés | MEDLINE | ID: mdl-37415272

RESUMEN

Dye/salt separation in textile wastewater is of great importance. Membrane filtration technology is an environmentally friendly and effective approach to solve this issue. In this study, a thin-film composite membrane with a tannic acid (TA)-modified carboxylic multiwalled carbon nanotube (MWCNT) interlayer (M-TA) was prepared by interfacial polymerization with amino-functionalized graphene quantum dots (NGQDs) acting as aqueous monomers. The addition of the M-TA interlayer favored the formation of a thinner, more hydrophilic, and smoother selective skin layer for the composite membrane. The pure water permeability of the M-TA-NGQDs membrane was ∼9.32 L m-2 h-1 bar-1, which was higher than that of the NGQDs membrane without the interlayer. Meanwhile, the M-TA-NGQDs membrane presented better methyl orange (MO) rejection (97.79%) than the NGQDs membrane (87.51%). The optimal M-TA-NGQDs membrane exhibited excellent dye rejection (Congo red (CR): 99.61%; brilliant green (BG): 96.04%) and low salt rejection (NaCl < 15%). Noticeably, the M-TA-NGQDs membrane displayed effective selective separation performance (CR and BG > 99%) for dye/NaCl mixed solutions even at a high NaCl concentration of 50,000 mg/L. Furthermore, the M-TA-NGQDs membrane presented high water permeability recovery ratio values (91.02-98.20%). Importantly, the M-TA-NGQDs membrane showed excellent chemical stability (acid/alkali resistance). Generally, the fabricated M-TA-NGQDs membrane exhibited a great prospect for applications in dye wastewater treatment and water recycling, especially for the effective selective separation of dye/salt mixtures for high-salinity textile dyeing wastewater.

10.
J Am Chem Soc ; 145(23): 12928-12934, 2023 Jun 14.
Artículo en Inglés | MEDLINE | ID: mdl-37267262

RESUMEN

Selective oxidation of methane to methanol by dioxygen (O2) is an appealing route for upgrading abundant methane resource and represents one of the most challenging reactions in chemistry due to the overwhelmingly higher reactivity of the product (methanol) versus the reactant (methane). Here, we report that gold nanoparticles dispersed on mordenite efficiently catalyze the selective oxidation of methane to methanol by molecular oxygen in aqueous medium in the presence of carbon monoxide. The methanol productivity reaches 1300 µmol gcat-1 h-1 or 280 mmol gAu-1 h-1 with 75% selectivity at 150 °C, outperforming most catalysts reported under comparable conditions. Both hydroxyl radicals and hydroperoxide species participate in the activation and conversion of methane, while it is shown that the lower affinity of methanol on gold mainly accounts for higher methanol selectivity.

11.
J Colloid Interface Sci ; 641: 197-214, 2023 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-36933467

RESUMEN

For better sustainable resource recovery and elevating the separation efficiency of dye/salt mixture, it is essential to develop an appropriate nanofiltration membrane for the treatment of textile dyeing wastewater containing relatively smaller molecule dyes. In this work, a novel composite polyamide-polyester nanofiltration membrane was fabricated by tailoring amino functionalized quantum dots (NGQDs) and ß-cyclodextrin (CD). An in-situ interfacial polymerization occurred between the synthesized NGQDs-CD and trimesoyl chloride (TMC) on the modified multi-carbon nanotubes (MWCNTs) substrate. The incorporation of NGQDs significantly elevated the rejection (increased by âˆ¼ 45.08%) of the resultant membrane for small molecular dye (Methyl orange, MO) compared to the pristine CD membrane at low pressure (1.5 bar). The newly developed NGQDs-CD-MWCNTs membrane exhibited enhanced water permeability without compromising the dye rejection compared to the pure NGQDs membrane. The improved performance of the membrane was primarily attributed to the synergistic effect of functionalized NGQDs and the special hollow-bowl structure of CD. The optimal NGQDs-CD-MWCNTs-5 membrane expressed pure water permeability of 12.35 L m-2h-1 bar-1 at the pressure of 1.5 bar. Noteworthily, the NGQDs-CD-MWCNTs-5 membrane not only showed high rejection for the larger molecular dye of Congo Red (CR, 99.50%) but also for the smaller molecular dye of MO (96.01%) and Brilliant Green (BG, 95.60%) with the permeability of 8.81, 11.40, and 6.37 L m-2h-1 bar-1, respectively at low pressure (1.5 bar). The rejection of inorganic salts by the NGQDs-CD-MWCNTs-5 membrane was 17.20% for sodium chloride (NaCl), 14.30% for magnesium chloride (MgCl2), 24.63% for magnesium sulfate (MgSO4), and 54.58% for sodium sulfate (Na2SO4), respectively. The great rejection of dyes remained in the dye/salt binary mixed system (higher than 99% for BG and CR, <21% for NaCl). Importantly, the NGQDs-CD-MWCNTs-5 membrane exhibited favorable antifouling performance and potential good operation stability performance. Consequently, the fabricated NGQDs-CD-MWCNTs-5 membrane suggested a prospective application for the reuse of salts and water in textile wastewater treatment owing to the effective selective separation performance.

12.
Sci Adv ; 9(6): eade6975, 2023 Feb 10.
Artículo en Inglés | MEDLINE | ID: mdl-36763650

RESUMEN

Crystalline materials are often considered to have rigid periodic lattices, while soft materials are associated with flexibility and nonperiodicity. The continuous evolution of metal-organic frameworks (MOFs) has erased the boundaries between these two distinct conceptions. Flexibility, disorder, and defects have been found to be abundant in MOF materials with imperfect crystallinity, and their intricate interplay is poorly understood because of the limited strategies for characterizing disordered structures. Here, we apply advanced nuclear magnetic resonance spectroscopy to elucidate the mesoscale structures in a defective MOF with a semicrystalline lattice. We show that engineered defects can tune the degree of lattice flexibility by combining both ordered and disordered compartments. The one-dimensional alignment of correlated defects is the key for the reversible topological transition. The unique matrix is featured with both rigid framework of nanoporosity and flexible linkage of high swellability.

13.
Anal Chem ; 95(2): 792-801, 2023 01 17.
Artículo en Inglés | MEDLINE | ID: mdl-36520837

RESUMEN

Ligand exchange is fundamentally related to the surface chemistry of nanoparticles in solution and is also an essential procedure for their synthesis and solution processing. The solution of ligand-bearing nanoparticles can be regarded as a dynamic equilibrium of bound and free ligands depending on the concentration and temperature. The direct experimental calibration of the ligand exchange dynamics relies on the in situ and real-time quantification of bound and free ligands. However, existing analytical strategies are often with limited applicability considering the requirement of special functional groups or the indirect detection of photoluminescence or reaction heat. In this work, we explore diffusion-based methods of solution-state nuclear magnetic resonance (NMR) as a general strategy to probe ligand exchange. Using comprehensive numerical simulations, we show that diffusion NMR with designable time sequences can effectively distinguish bound and free ligands and measure the exchange rate constants from 0.5 to 200 s-1 under typical instrumental settings. These methods are demonstrated experimentally on colloidal CdSe nanocrystal systems with carboxylate or amine ligands whose exchange rates were previously undetectable. The kinetic rate constants, activation energies, and thermodynamic parameters of ligand exchange have been obtained under variable temperature conditions. We expect the diffusion NMR strategies to be generally applicable for calibrating the exchange of organic ligands on various nanoparticle systems.


Asunto(s)
Nanopartículas , Ligandos , Nanopartículas/química , Espectroscopía de Resonancia Magnética , Termodinámica , Temperatura
14.
Chemosphere ; 308(Pt 3): 136427, 2022 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-36122753

RESUMEN

Pyrite and engineering carbon materials have received increasing attention for their catalytic potential in Fenton reactions due to their extensive sources and low cost. However, effects of carbon materials on the degradation of pollutants by pyrite-catalyzed heterogeneous Fenton oxidation have not been fully understood. In this study, the performance of pyrite-catalyzed heterogeneous Fenton system on the degradation of ciprofloxacin (CIP) was investigated in the presence of activated carbon (AC), biochar (BC), and carbon nanotubes (CNTs). Synchronous and asynchronous experiments (adsorption and catalysis) were conducted to elucidate the roles of the carbon materials in pyrite-catalyzed Fenton reactions. The results demonstrated that all the three carbon materials accelerated the pyrite-catalyzed Fenton oxidation of CIP. Under the experimental conditions, the reaction rates, which were obtained by fitting the synchronous experimental results with the pseudo-first-order kinetic model, of pyrite/AC, pyrite/BC and pyrite/CNTs with H2O2 for the removal of CIP were 8.28, 3.40 and 3.37 times faster than that of pyrite alone. Adsorption experiments and characterization analysis showed that AC had a higher adsorption capacity than BC and CNTs for CIP, which enabled it to distinguish itself in assisting the pyrite-catalyzed Fenton oxidation. In the presence of the carbon materials, the adsorption effect should not be neglected when studying the catalytic performance of pyrite. Free radical quenching experiments and electron spin-resonance spectroscopy (ESR) were used to detect and identify free radical species in the reactions. The results showed that hydroxyl radicals (•OH) contributed significantly to the degradation of CIP. The addition of carbon materials promoted the production of •OH, which favored the degradation of CIP. The results of this study suggested that the synergistic effect of oxidation and adsorption promoted the removal of CIP in pyrite/carbon materials/H2O2 systems, and coupling pyrite and carbon materials shows great potential in treating antibiotic wastewater.


Asunto(s)
Nanotubos de Carbono , Contaminantes Químicos del Agua , Antibacterianos , Catálisis , Carbón Orgánico/química , Ciprofloxacina/química , Peróxido de Hidrógeno/química , Hierro , Oxidación-Reducción , Sulfuros , Aguas Residuales , Contaminantes Químicos del Agua/química
15.
Nanotechnology ; 33(49)2022 Sep 19.
Artículo en Inglés | MEDLINE | ID: mdl-36044817

RESUMEN

Carbon impurity as point defects makes key impact on the leakage in GaN-on-Si structures. GaN-based epitaxial layers with different point defects by changing carbon-doped concentration were used to investigate the point defects behavior. It was found that leakage mechanisms correspond with space-charge-limited current models at low voltages, and after 1st kink, electron injection from silicon to GaN and PF conduction play a key role in the leakage of both point defects case with low carbon and high carbon doped. In addition, high carbon in GaN-on-Si epitaxial layers obtained lower leakage and larger breakdown voltage. The slope of logJ-Vhas two kinks and effective energy barrierEahas two peaks, 0.4247 eV at about 300 V and 0.3485 eV at about 900 V, respectively, which is related to accepted states and donor states related with carbon impurity. While the slope of logJ-Vhas one kink and effective energy barrierEahas one peak, 0.4794 eV at about 400 V of low carbon in GaN-on-Si epitaxial layers, indicating only field-induced accepted ionized makes impact on leakage. The comparative results of more donor trap density in high carbon indicate point defects related with carbon impurity play a key role in the kinks of logJ-Vslope.

16.
Nat Commun ; 13(1): 5112, 2022 Aug 30.
Artículo en Inglés | MEDLINE | ID: mdl-36042242

RESUMEN

The defects in metal-organic frameworks (MOFs) can dramatically alter their pore structure and chemical properties. However, it has been a great challenge to characterize the molecular structure of defects, especially when the defects are distributed irregularly in the lattice. In this work, we applied a characterization strategy based on solid-state nuclear magnetic resonance (NMR) to assess the chemistry of defects. This strategy takes advantage of the coordination-sensitive phosphorus probe molecules, e.g., trimethylphosphine (TMP) and trimethylphosphine oxide (TMPO), that can distinguish the subtle differences in the acidity of defects. A variety of local chemical environments have been identified in defective and ideal MOF lattices. The geometric dimension of defects can also be evaluated by using the homologs of probe molecules with different sizes. In addition, our method provides a reliable way to quantify the density of defect sites, which comes together with the molecular details of local pore environments. The comprehensive solid-state NMR strategy can be of great value for a better understanding of MOF structures and for guiding the design of MOFs with desired catalytic or adsorption properties.

17.
ACS Appl Mater Interfaces ; 14(34): 38990-39003, 2022 Aug 31.
Artículo en Inglés | MEDLINE | ID: mdl-35976131

RESUMEN

Thin-film nanocomposite (TFN) membranes with efficient molecular separation and organic solvent resistance are active in demand in wastewater treatment and resource reclamation, meeting the goal of emission peaks and carbon neutrality. In this work, a simple and rational design strategy has been employed to construct a sandwich-structured membrane for removing fluoroquinolone antibiotics and recycling organic solvents. The sandwich-structured membrane is composed of a porous substrate, a hydrophilic tannic acid-polyethyleneimine (TA-PEI) interlayer, and a polyamide (PA) selective layer decorated with metal-organic framework (PA-MOF). Results manifest that the hydrophilic TA-PEI interlayer played a bridging and gutter effect to achieve effective control in amide storage, amine diffusion, and nanomaterial downward leakage at the immiscible interface. The PA-MOF selective layer has been changed to a loosely crumpled surface, endowing functionalities on the sandwich-structured membrane that included limited pores, strengthened electronegativity, and stronger hydrophilicity. Thus, an enhanced water flux of 87.23 ± 7.43 LMH was achieved by the TFN-2 membrane (0.04 mg·mL-1 UiO-66-NH2), which is more than five times that of the thin-film composite membrane (17.46 ± 3.88 LMH). The rejection against norfloxacin, ciprofloxacin, and levofloxacin is 92.94 ± 1.60%, 94.62 ± 1.29%, and 96.92 ± 1.05%, respectively, effectively breaking through the "trade-off" effect between membrane permeability and rejection efficiency. Further antifouling results showed that the sandwich-structured membrane had lower flux decay ratios (3.36∼7.07%) and higher flux recovery ratios (93.40∼98.40%), as well as superior long-term stability after 30 days of filtration. Moreover, organic solvent resistance testing confirms that the sandwich-structured membrane maintained stable solvent flux and better recovery rates in ethanol, acetone, isopropanol, and N,N-dimethylformamide. Detailed nanofiltration mechanism studies revealed that these outstanding performances are based on the joint effect of the TA-PEI interlayer and PA-MOF selective layer, proposing a new perspective to break through the bottleneck of nanofiltration application in a complex environment.


Asunto(s)
Antibacterianos , Membranas Artificiales , Filtración/métodos , Estructuras Metalorgánicas , Nylons/química , Ácidos Ftálicos , Solventes
18.
Environ Sci Pollut Res Int ; 29(40): 60953-60967, 2022 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-35435545

RESUMEN

Gold (Au) nanoparticles supported on certain platforms display highly efficient activity on nitroaromatics reduction. In this study, steam-activated carbon black (SCB) was used as a platform to fabricate Au/SCB composites via a green and simple method for 4-nitrophenol (4-NP) reduction. The obtained Au/SCB composites exhibit efficient catalytic performance in reduction of 4-NP (rate constant kapp = 2.1925 min-1). The effects of SCB activated under different steam temperature, Au loading amount, pH, and reaction temperature and NaBH4 concentration were studied. The structural advantages of SCB as a platform were analyzed by various characterizations. Especially, the result of N2 adsorption-desorption method showed that steam activating process could bring higher surface area (from 185.9689 to 249.0053 m2/g), larger pore volume (from 0.073268 to 0.165246 cm3/g), and more micropore for SCB when compared with initial CB, demonstrating the suitable of SCB for Au NP anchoring, thus promoting the catalytic activity. This work contributes to the fabrication of other supported metal nanoparticle catalysts for preparing different functional nanocomposites for different applications.


Asunto(s)
Oro , Nanopartículas del Metal , Catálisis , Carbón Orgánico , Oro/química , Nanopartículas del Metal/química , Nitrofenoles/química , Hollín , Vapor
19.
J Hazard Mater ; 433: 128801, 2022 07 05.
Artículo en Inglés | MEDLINE | ID: mdl-35405589

RESUMEN

The ability of microplastics (MPs) to interact with environmental pollutants is of great concern. Riverine sediments, as sinks for multi-pollutants, have been rarely studied for MPs risk evaluation. Meanwhile, MPs generated from biodegradable plastics are questioning the safety of the promising materials. In this study, we investigated the effects of typical non-degradable polyethylene (PE) and biodegradable polylactic acid (PLA) MPs on sediment enzymes, arsenic (As) fractionation, and microbial community structures in As-contaminated riverine sediments. The results indicated that the presence of MPs (1% and 3%, w/w) led As transformed into more labile and bioavailable fractions in riverine sediments, especially under higher As and MPs levels. Analysis on microbial activities and community structures confirmed the strong potential of MPs in inhibiting microbial activities and shifting bacterial community succession patterns through enrichment of certain microbiota. Moreover, biodegradable PLA MPs presented stronger alterations in arsenic fractionation and microbial community structures than PE MPs did, which might be jointly attributed to adsorption behaviors, microbial alterations, and potential PLA degradation behaviors. The study indicated that MPs contamination increased As mobility and bioavailability, and shifted microbial communities in riverine sediments. Moreover, biodegradable MPs might lead to stronger microbial alterations and increases in As bioavailability, acting as a threat to ecological safety, which needed further exploration.


Asunto(s)
Arsénico , Microbiota , Contaminantes Químicos del Agua , Arsénico/análisis , Arsénico/toxicidad , Microplásticos/toxicidad , Plásticos , Poliésteres , Polietileno , Contaminantes Químicos del Agua/análisis , Contaminantes Químicos del Agua/toxicidad
20.
Natl Sci Rev ; 9(2): nwab138, 2022 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-35233287

RESUMEN

High-quality colloidal nanocrystals are commonly synthesized in hydrocarbon solvents with alkanoates as the most common organic ligand. Water molecules with an approximately equal number of surface alkanoate ligands are identified at the inorganic-organic interface for all types of colloidal nanocrystals studied, and investigated quantitatively using CdSe nanocrystals as the model system. Carboxylate ligands are coordinated to the surface metal ions and the first monolayer of water molecules is found to bond to the carboxylate groups of alkanoate ligands through hydrogen bonds. Additional monolayer(s) of water molecules can further be adsorbed through hydrogen bonds to the first monolayer of water molecules. The nearly ideal environment for hydrogen bonding at the inorganic-organic interface of alkanoate-coated nanocrystals helps to rapidly and stably enrich the interface-bonded water molecules, most of which are difficult to remove through vacuum treatment, thermal annealing and chemical drying. The water-enriched structure of the inorganic-organic interface of high-quality colloidal nanocrystals must be taken into account in order to understand the synthesis, processing and properties of these novel materials.

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