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1.
Mar Pollut Bull ; 205: 116602, 2024 Jun 30.
Artigo em Inglês | MEDLINE | ID: mdl-38950512

RESUMO

The potential effect of hydrological conditions on distribution and loadings of Hg species was investigated in the microtidal Hyeongsan River Estuary (HRE). Dissolved Hg (DHg) and dissolved methylmercury (DMeHg) from the creek receiving industrial wastes were effectively settled to sediment during the post-typhoon period, while persistent input from the Hg-contaminated creek without settling was observed during the dry periods. The event-based mean approach was applied to explore the hydrological effects on the annual flux of Hg. The largest inputs of DHg and particulate Hg (PHg) were found in the Hg-contaminated creek, and DHg input was higher in the dry than wet periods whereas PHg input was higher in the wet than dry periods. In sediment, Hg and MeHg concentrations decreased after the typhoon, attributed to erosion of surface sediments. Overall, the HRE serves as an effective sink of Hg that reduces the degree of Hg contamination in coastal water.

2.
Chemosphere ; 359: 142344, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38754484

RESUMO

Burning incenses and scented candles may provide harmful chemicals. Although many studies have evaluated volatile organic chemicals emitted by their use and related health risks, extension of our understanding for guiding appropriate use under various use conditions is necessary. In this study, emission characteristics of commercial incenses and scented candles were evaluated in a laboratory chamber using real-time measurement and the time-weighted average exposure concentrations of monoaromatic compounds and monoterpenes were assessed using passive samplers while volunteers living in a studio apartment use them. After burning incense, the average levels of benzene increased from 1.4 to 100 µg m-3. The presence of a wood core in commercial incense products was the main cause of high benzene emission by burning them although the increase in benzene was also influenced by factors such as the brand of the products, the number of incense sticks burned, the duration of each burning session, and ventilation period. Electrical warming of scented candles increased the levels of monoterpenes by factors of 16-30 on average. Considering the emission characteristics found in this study, exposure to benzene and monoterpenes could be mitigated by cautious use of those products in residential areas.


Assuntos
Poluentes Atmosféricos , Poluição do Ar em Ambientes Fechados , Benzeno , Monitoramento Ambiental , Compostos Orgânicos Voláteis , Compostos Orgânicos Voláteis/análise , Poluição do Ar em Ambientes Fechados/análise , Poluição do Ar em Ambientes Fechados/estatística & dados numéricos , Monitoramento Ambiental/métodos , Benzeno/análise , Poluentes Atmosféricos/análise , Habitação , Humanos , Monoterpenos/análise , Odorantes/análise
3.
Chem Sci ; 15(15): 5604-5611, 2024 Apr 17.
Artigo em Inglês | MEDLINE | ID: mdl-38638221

RESUMO

Highly organized π-aggregate architectures can strongly affect electronic couplings, leading to important photophysical behaviors. With the escalating interest in two-dimensional (2D) materials attributed to their exceptional electronic and optical characteristics, there is growing anticipation that 2D radial-π-stacks built upon radial π-conjugation nanorings, incorporating intra- and inter-ring electronic couplings within the confines of a 2D plane, will exhibit superior topological attributes and distinct properties. Despite their immense potential, the design and synthesis of 2D π-stacks have proven to be a formidable challenge due to the insufficient π-π interactions necessary for stable stacking. In this study, we present the successful preparation of single-layer 2D radial-π-stacks in a solution. Pillar-shaped radially π-conjugated [4]cyclo-naphthodithiophene diimide ([4]C-NDTIs) molecules were tetragonally arranged via in-plane intermolecular π-π interactions. These 2D π-stacks have a unique topology that differs from that of conventional 1D π-stacks and exhibit notable properties, such as acting as a 2D template capable of absorbing C60 guest molecules and facilitating the formation of 2D radial-π-stacks comprising [4]C-NDTI-C60 complexes, rapid exciton delocalization across the 2D plane, and efficient excitation energy funneling towards a trap.

4.
J Am Chem Soc ; 146(15): 10833-10846, 2024 Apr 17.
Artigo em Inglês | MEDLINE | ID: mdl-38578848

RESUMO

Multiexciton in singlet exciton fission represents a critical quantum state with significant implications for both solar cell applications and quantum information science. Two distinct fields of interest explore contrasting phenomena associated with the geminate triplet pair: one focusing on the persistence of long-lived correlation and the other emphasizing efficient decorrelation. Despite the pivotal nature of multiexciton processes, a comprehensive understanding of their dependence on the structural and spin properties of materials is currently lacking in experimental realizations. To address this gap in knowledge, molecular engineering was employed to modify the TIPS-tetracene structures, enabling an investigation of the structure-property relationships in spin-related multiexciton processes. In lieu of the time-resolved electron paramagnetic resonance technique, two time-resolved magneto-optical spectroscopies were implemented for quantitative analysis of spin-dependent multiexciton dynamics. The utilization of absorption and fluorescence signals as complementary optical readouts, in the presence of a magnetic field, provided crucial insights into geminate triplet pair dynamics. These insights encompassed the duration of multiexciton correlation and the involvement of the spin state in multiexciton decorrelation. Furthermore, simulations based on our kinetic models suggested a role for quintet dilution in multiexciton dynamics, surpassing the singlet dilution principle established by the Merrifield model. The integration of intricate model structures and time-resolved magneto-optical spectroscopies served to explicitly elucidate the interplay between structural and spin properties in multiexciton processes. This comprehensive approach not only contributes to the fundamental understanding of these processes but also aligns with and reinforces previous experimental studies of solid states and theoretical assessments.

5.
J Hazard Mater ; 470: 134167, 2024 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-38598880

RESUMO

This study investigated the leaching of phthalate and non-phthalate plasticizers from polyvinyl chloride microplastics (MPs) into sediment and their degradation over a 30-d period via abiotic and biotic processes. The results showed that 3579% of plasticizers were released into the sediment from the MPs and > 99.9% degradation was achieved. Although a significantly higher degradation was found in plasticizer-added microcosms under biotic processes (overall, 94%), there was a noticeable abiotic loss (72%), suggesting that abiotic processes also play a role in plasticizer degradation. Interestingly, when compared with the initial sediment-water partitioning for plasticizers, the partition constants for low-molecular-weight compounds decreased in both microcosms, whereas those for high-molecular-weight compounds increased after abiotic degradation. Furthermore, changes in the bacterial community, abundance of plasticizer-degrading bacterial populations, and functional gene profiles were assessed. In all the microcosms, a decrease in bacterial community diversity and a notable shift in bacterial composition were observed. The enriched potential plasticizer-degrading bacteria were Arthrobacter, Bacillus, Desulfovibrio, Desulfuromonas, Devosia, Gordonia, Mycobacterium, and Sphingomonas, among which Bacillus was recognized as the key plasticizer degrader. Overall, these findings shed light on the factors affecting plasticizer degradation, the microbial communities potentially involved in biodegradation, and the fate of plasticizers in the environment.


Assuntos
Bactérias , Sedimentos Geológicos , Microplásticos , Ácidos Ftálicos , Plastificantes , Cloreto de Polivinila , Poluentes Químicos da Água , Cloreto de Polivinila/química , Plastificantes/metabolismo , Sedimentos Geológicos/microbiologia , Sedimentos Geológicos/química , Ácidos Ftálicos/metabolismo , Poluentes Químicos da Água/análise , Poluentes Químicos da Água/metabolismo , Bactérias/metabolismo , Bactérias/classificação , Biodegradação Ambiental
6.
Environ Monit Assess ; 196(4): 404, 2024 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-38557915

RESUMO

This study aimed to optimize the methods for sampling and analyzing methylmercury (MeHg) concentrated within diffusive gradients in thin films (DGT) and its application to different water bodies. We explored the elution solution for MeHg, comprised of 1.13 mM thiourea and 0.1M HCl, optimizing its volume to 50 mL. In addition, we found that it is necessary to analyze the entire extraction solution after adjusting its pH, to ensure completion of the ethylation reaction. The DGT samplers were deployed in two distinct aquatic environments (i.e., Okjeong Lake and Nakdong River) for up to 6 weeks, and this study demonstrated to predict the time-weighted average concentration with a diffusion coefficient of 7.65 × 10-6 cm2 s-1 for MeHg in the diffusive gel. To assess the diffusive boundary layer (DBL) effects, the DGT samplers with different agarose diffusive gel thickness were deployed. The mass of MeHg accumulated in the DGT resin at a given time decreased with increasing diffusive gel thickness, because of creating longer diffusion pathways within thicker gels. The labile MeHg concentration estimated by the DGT in Okjeong Lake and Nakdong River are found in the range of 61-111 and 55-105 pg L-1, respectively, which were found to be similar to the grab sampling data. Additionally, this study evaluated depth-dependent MeHg in Okjeong Lake. The vertical profile results showed that the concentration of MeHg at the depth of 2.3 and 15.7 m are about 1.5 and 4.6 times of the DGT installed at 0.3 m of the surface layer, respectively, suggesting potential mercury methylation in deep waters. These findings have practical implications for predicting bioavailability, assessing risks, and formulating strategies for water body management and contamination remediation.


Assuntos
Compostos de Metilmercúrio , Poluentes Químicos da Água , Monitoramento Ambiental/métodos , Poluentes Químicos da Água/análise , Lagos , Difusão , Água
7.
Sci Adv ; 10(12): eadi7724, 2024 Mar 22.
Artigo em Inglês | MEDLINE | ID: mdl-38507496

RESUMO

Stretchable bioelectronics has notably contributed to the advancement of continuous health monitoring and point-of-care type health care. However, microscale nonconformal contact and locally dehydrated interface limit performance, especially in dynamic environments. Therefore, hydrogels can be a promising interfacial material for the stretchable bioelectronics due to their unique advantages including tissue-like softness, water-rich property, and biocompatibility. However, there are still practical challenges in terms of their electrical performance, material homogeneity, and monolithic integration with stretchable devices. Here, we report the synthesis of a homogeneously conductive polyacrylamide hydrogel with an exceptionally low impedance (~21 ohms) and a reasonably high conductivity (~24 S/cm) by incorporating polyaniline-decorated poly(3,4-ethylenedioxythiophene:polystyrene). We also establish robust adhesion (interfacial toughness: ~296.7 J/m2) and reliable integration between the conductive hydrogel and the stretchable device through on-device polymerization as well as covalent and hydrogen bonding. These strategies enable the fabrication of a stretchable multichannel sensor array for the high-quality on-skin impedance and pH measurements under in vitro and in vivo circumstances.


Assuntos
Hidrogéis , Hidrogéis/química , Impedância Elétrica , Condutividade Elétrica , Polimerização , Ligação de Hidrogênio
8.
Mar Pollut Bull ; 202: 116300, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38555803

RESUMO

This study investigated the contents of total mercury (THg), trace metals, and CH4 and determined the signature microbes involved in various biogeochemical processes in the sediment of the Canadian Beaufort Sea. The THg ranged between 32 and 63 µg/kg and the trace metals such as Fe, Al, Mn, and Zn were significant in distributions. The pH, SO42-, Fe2+, and redox proxy metals were crucial factors in the spatial and vertical heterogeneity of geochemical distributions. CH4 was detected only at the mud volcano site. Microbial analyses identified Clostridium, Desulfosporosinus, Desulfofustis, and Desulftiglans as the predominant Hg methylators and sulfate reducers; Nitrosopumilus and Hyphomicrobium as the major nitrifiers and denitrifiers; Methanosarcina and Methanosaeta as keystone methanogens; and Methyloceanibacter and Methyloprofundus as signature methanotrophs. Altogether, this study expands the current understanding of the microbiological and geochemical features and could be helpful in predicting ecosystem functions in the Canadian Beaufort Sea.


Assuntos
Sedimentos Geológicos , Mercúrio , Poluentes Químicos da Água , Sedimentos Geológicos/química , Sedimentos Geológicos/microbiologia , Mercúrio/análise , Mercúrio/metabolismo , Poluentes Químicos da Água/análise , Monitoramento Ambiental , Bactérias , Metano/análise , Canadá
9.
Environ Res ; 238(Pt 2): 117238, 2023 12 01.
Artigo em Inglês | MEDLINE | ID: mdl-37783324

RESUMO

The potential human health risks associated with soil vapor intrusion and volatile organic compounds (VOCs) exposure were characterized at an industrialized site by the quantification of gaseous VOCs in soil pores using a passive sampling technique. The gaseous tetrachloroethene (PCE) in soil pores varied between 12 and 5,400 µg m-3 showing 3 orders of magnitude variation with dependence on groundwater PCE concentrations. Though the PCE concentration in the air only varied between 0.45 and 1.5 µg m-3 showing negligible variations compared to the variation observed in soil pores. The PCE concentration in the air varied between 0.45 and 1.5 µg m-3. The calculation of fugacity suggested that the PCE in the test site originated from groundwater. Measured PCE in groundwater ranged from 14 to 2,400 times higher than PCE in soil gas. This indicates that conducting a vapor intrusion risk assessment using passive soil gas sampling is critical for accurate risk characterization and assessment. Estimated PCE inhalation cancer risks for street cleaners and indoor residents varied between 10-6 and 10-4 with a low plausible hazard, and between 10-3 and 10-2 with a high risk, respectively. The results of this study demonstrate that passive sampling offers a significantly lower cost and labor-intensive approach compared to traditional methods for assessing pollution distribution in contaminated sites and characterizing risks. This highlights the potential for wider application of passive sampling techniques in environmental studies.


Assuntos
Poluição do Ar em Ambientes Fechados , Água Subterrânea , Poluentes do Solo , Tetracloroetileno , Compostos Orgânicos Voláteis , Humanos , Poluição do Ar em Ambientes Fechados/análise , Solo , Monitoramento Ambiental/métodos , Poluentes do Solo/análise , Gases , Compostos Orgânicos Voláteis/análise
10.
J Am Chem Soc ; 145(36): 19812-19823, 2023 Sep 13.
Artigo em Inglês | MEDLINE | ID: mdl-37656929

RESUMO

Singlet exciton fission in organic chromophores has received much attention during the past decade. Inspired by numerous spectroscopic studies in the solid state, there have been vigorous efforts to study singlet exciton fission dynamics in covalently bonded oligomers, which aims to investigate underlying mechanisms of this intriguing process in simplified model systems. In terms of through-space orbital interactions, however, most of covalently bonded pentacene oligomers studied so far fall into weakly interacting systems since they manifest chain-like structures based on various (non)conjugated linkers. Therefore, it remains as a compelling question to answer how through-space interactions in the solid state intervene this photophysical process since it is hypersensitive to displacements and orientations between neighboring chromophores. Herein, as one of experimental studies to answer this question, we introduced a tight-packing dendritic structure whose mesityl-pentacene constituents are coupled via moderate through-space orbital interactions. Based on the comparison with a suitably controlled dendritic structure, which is in a weak coupling regime, important mechanistic viewpoints are tackled such as configurational mixings between singlet, charge-transfer, and triplet pair states and the role of chromophore multiplication. We underscore that our through-space-coupled dendritic oligomer in a quasi-intermediate coupling regime provides a hint on the interplay of multiconfigurational excited-states, which might have drawn complexity in singlet exciton fission kinetics throughout numerous solid-state morphologies.

11.
Environ Res ; 237(Pt 1): 116888, 2023 Nov 15.
Artigo em Inglês | MEDLINE | ID: mdl-37586452

RESUMO

Metal contamination and other geochemical alterations affect microbial composition and functional activities, disturbing natural biogeochemical cycles. Therefore, it is essential to understand the influences of multi-metal and geochemical interactions on microbial communities. This work investigated the distributions of total mercury (THg), methylmercury (MeHg), and trace metals in the anthropogenically affected sediment. The microbial communities and functional genes profiles were further determined to explore their association with Hg-methylation and geochemical features. The levels of THg and MeHg in sediment cores ranged between 10 and 40 mg/kg and 0.01-0.16 mg/kg, respectively, with an increasing trend toward bottom horizons. The major metals present at all depths were Al, Fe, Mn, and Zn. The enrichment and contamination indices confirmed that the trace metals were highly enriched in the anthropogenically affected sediment. Various functional genes were detected in all strata, indicating the presence of active microbial metabolic processes. The microbial community profiles revealed that the phyla Proteobacteria, Bacteroidetes, Bathyarchaeota, and Euryarchaeota, and the genera Thauera, Woeseia, Methanomethylovorans, and Methanosarcina were the dominant microbes. Correlating major taxa with geochemical variables inferred that sediment geochemistry substantially affects microbial community and biogeochemical cycles. Furthermore, archaeal methanogens and the bacterial phyla Chloroflexi and Firmicutes may play crucial roles in enhancing MeHg levels. Overall, these findings shed new light on the microbial communities potentially involved in Hg-methylation process and other biogeochemical cycles.

12.
Adv Mater ; 35(39): e2304533, 2023 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-37390092

RESUMO

The small nanoparticle size and long-chain ligands in colloidal metal halide perovskite quantum dots (PeQDs) cause charge confinement, which impedes exciton dissociation and carrier extraction in PeQD solar cells, so they have low short-circuit current density Jsc , which impedes further increases in their power conversion efficiency (PCE). Here, a re-assembling process (RP) is developed for perovskite nanocrystalline (PeNC) films made of colloidal perovskite nanocrystals to increase Jsc in PeNC solar cells. The RP of PeNC films increases their crystallite size and eliminates long-chain ligands, and thereby overcomes the charge confinement in PeNC films. These changes facilitate exciton dissociation and increase carrier extraction in PeNC solar cells. By use of this method, the gradient-bandgap PeNC solar cells achieve a Jsc = 19.30 mA cm-2 without compromising the photovoltage, and yield a high PCE of 16.46% with negligible hysteresis and good stability. This work provides a new strategy to process PeNC films and pave the way for high performance PeNC optoelectronic devices.

13.
Sci Total Environ ; 874: 162412, 2023 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-36858231

RESUMO

In the present study, the migration of plasticizers from modeled and commercial polyvinyl chloride (mPVC and cPVC, respectively) to poly(dimethylsiloxane) via artificial sebum was assessed to mimic the dermal migration of plasticizers. In addition, the various factors affecting migration of phthalic acid esters (PAEs) from diverse PVC products were investigated. The migrated mass and migration ratio of PAEs increased but the migration rate decreased over time. The migration rate increased with sebum mass, contact time, and temperature but decreased under higher pressure. Low-molecular-weight PAEs (dimethyl phthalate and diethyl phthalate) migrated in higher amounts than high-molecular-weight PAEs (dicyclohexyl phthalate [DCHP] and diisononyl phthalate [DINP]). Diffusion of all PAEs in mPVC increased with temperature, with diffusion coefficients ranging from 10-13 to 10-15, 10-12 to 10-14, and 10-10 to 10-12 cm2·s-1 at 25 °C, 40 °C, and 60 °C, respectively; the enthalpy of activation ranged between 127 and 194 kJ·mol-1. Moreover, migration depended on total PAE content of the product, as the diffusion coefficient for DINP in cPVC (softer PVC) was approximately three orders of magnitude higher than that for DINP in mPVC (harder PVC); this may be due to the increase in free volume with increasing plasticizer content. Finally, the daily exposure doses of the plasticizers were estimated. These findings will be helpful for estimating dermal exposure risk.


Assuntos
Ácidos Ftálicos , Plastificantes , Cloreto de Polivinila , Sebo
14.
J Hazard Mater ; 448: 130933, 2023 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-36860070

RESUMO

Phthalic acid esters (PAEs) or phthalates are endocrine-disrupting chemicals and among the most frequently detected hydrophobic organic pollutants, which can be gradually released from consumer products into the environment (e.g., water). This study measured the equilibrium partition coefficients for 10 selected PAEs, with a wide range of logarithms of the octanol-water partition coefficient (log Kow) from 1.60 to 9.37, between poly(dimethylsiloxane) (PDMS) and water (KPDMSw) using the kinetic permeation method. The desorption rate constant (kd) and KPDMSw for each PAEs were calculated from kinetic data. The experimental log KPDMSw for the PAEs ranges from 0.8 to 5.9, which is linearly correlated with log Kow values up to 8 from the literature (R2 > 0.94); however, it slightly deviated for the PAEs with log Kow values greater than 8. In addition, KPDMSw decreased with the temperature and enthalpy for PAEs partitioning in PDMS-water in an exothermic manner. Furthermore, the effects of dissolved organic matter and ionic strength on the partitioning of PAEs in PDMS were investigated. PDMS was used as a passive sampler to determine the aqueous concentration of plasticizers in river surface water. The results of this study can be used to evaluate the bioavailability and risk of phthalates in real environmental samples.

15.
Sci Total Environ ; 879: 163071, 2023 Jun 25.
Artigo em Inglês | MEDLINE | ID: mdl-36965723

RESUMO

The exposure levels of selected terpenes (limonene, α- and ß-pinenes, and γ-terpinene) emitted by essential oil diffusers in vehicles and studio apartments were assessed using a passive sampling method. A previously developed passive sampler composed of an expanded polytetrafluoroethylene membrane and adsorbent (ePTFE PS) was enlarged and made wearable. Before field deployment, the sampling performance of the modified ePTFE PS for selected terpenes was compared with that of active sampling in a lab-scale 5 m3 test chamber under constant exposure conditions, supporting that passive sampling provides reasonable estimates of the time-weighted exposure concentration. Fifty volunteers were recruited and asked to wear the ePTFE PS while using an essential oil diffuser inside their own vehicle while commuting and in their studio apartment while sleeping. Terpene levels without an essential oil diffuser were very low in vehicles and 47, 3.6, 1.6, and 0.62 µg m-3 for average concentrations of limonene, α- and ß-pinenes, and γ-terpinene in studio apartments, respectively, close to those reported in previous studies. The indoor concentrations of all selected terpenes in vehicles and studio apartments were elevated by the use of essential oil diffusers, especially in vehicles. The average concentration of limonene in vehicles after the use of essential oil diffusers was 11 µg m-3, which was greater than that before use by a factor of 30. Therefore, cautious usage of essential oil diffusers indoors where the volume is limited, such as a vehicle, is needed to reduce exposure to terpenes.


Assuntos
Óleos Voláteis , Terpenos , Humanos , Limoneno , Monoterpenos Cicloexânicos
16.
Chemosphere ; 325: 138419, 2023 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-36925016

RESUMO

An equilibrium passive sampler made of polydimethylsiloxane (PDMS) fiber was developed to measure volatile organic compounds (VOCs) in soil vapor. Expanded polytetrafluoroethylene (ePTFE) was used to protect PDMS from pollution and direct contact with soil components. For all tested VOCs, equilibrium was reached after 7 days at 5 °C. The equilibrium partition coefficients of VOCs between PDMS, gas, and water were measured at three different temperatures. The analyte concentrations in PDMS exposed to gas and water separately were almost the same, which suggests that Cgas and Cwater in soil pores can be accurately deduced from CPDMS after equilibrium at various temperatures. To evaluate the passive sampler, active sampling measurements were performed simultaneously. Concentrations of VOCs deduced from the passive sampler were consistent with the concentrations measured by active sampling near the 1:1 line. Tests with artificial soils were conducted to observe the effects of soil components on passive sampling. The results suggest that the effect of water saturation can be ignored; in other words, the developed passive sampler can be applied in the vadose zone, which has fluctuating water saturation. With a holder for the sampler made of stainless steel, the developed in situ passive sampler can measure VOCs in contaminated soil vapor. The developed passive sampler was proven to be an alternative for measuring VOCs in soil vapor, which can be helpful for soil risk assessment and for observing the diffusion of VOCs in contaminated sites.


Assuntos
Compostos Orgânicos Voláteis , Solo , Água , Gases , Dimetilpolisiloxanos , Monitoramento Ambiental/métodos
17.
Environ Pollut ; 320: 121089, 2023 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-36669717

RESUMO

Volatile organic compounds (VOCs) have been globally reported at various sites. Currently, limited literature is available on VOC bioremediation using bacterial-immobilized biochar (BC-B). In this study, multiple VOC-degrading bacteria were enriched and isolated using a newly designed diffusion bioreactor. The most effective VOC-degrading bacteria were then immobilized on rice husk-derived pristine biochar (BC) to develop BC-B. Finally, the performances of BC and BC-B for VOCs (benzene, toluene, xylene, and trichloroethane) bioremediation were evaluated by establishing batch microcosm experiments (Control, C; bioconsortium, BS; pristine biochar, BC; and bacterial-immobilized biochar, BC-B). The results revealed that the newly designed diffusion bioreactor effectively simulated native VOC-contaminated conditions, easing the isolation of 38 diverse ranges of VOC-degrading bacterial strains. Members of the genus Pseudomonas were isolated in the highest (26.33%). The most effective bacterial strain was Pseudomonas sp. DKR-23, followed by Rhodococcus sp. Korf-18, which degraded multiple VOCs in the range of 52-75%. The batch microcosm experiment data showed that BC-B remediated the highest >90% of various VOCs, which was comparatively higher than that of BC, BS, and C. In addition, compared with C, the BS, BC, and BC-B microcosms abundantly reduced the half-life of various VOCs, implying a beneficial impact on the degradation behavior of VOCs. Altogether, this study suggests that a diffusion bioreactor system can be used as a cultivation device for the isolation of a wide range of VOC-degrading bacterial strains, and a compatible combination of biochar and bacteria may be an attractive and promising approach for the sustainable bioremediation of multiple VOCs.


Assuntos
Compostos Orgânicos Voláteis , Biodegradação Ambiental , Carvão Vegetal , Bactérias
18.
Mar Pollut Bull ; 185(Pt A): 114319, 2022 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-36343547

RESUMO

In this study, total mercury (THg), methylmercury (MeHg), various trace elements, and microbial communities were measured in surface sediments of the East Siberian Sea (ESS). The results showed that the average values of THg and MeHg were 58.8 ± 15.21 µg/kg and 0.50 ± 0.22 µg/kg, respectively. The notable levels of trace elements present in both surface sediment and porewater were Al, Fe, and Mn. The enrichment factor and geoaccumulation index analyses found that both natural phenomena and anthropogenic activities contributed to elevated concentrations of metals in the ESS. The redox proxy metals, pH, and SO42- were the major factors influencing the THg and MeHg distributions. Microbial profiles were substantially affected by metals and other abiotic factors. Proteobacteria and Thaumarchaeota were the most abundant phyla. Overall, the findings presented here facilitate the understanding of the current status of metal contamination, its influencing factors, and metal-microbiota-interactions in ESS.


Assuntos
Mercúrio , Compostos de Metilmercúrio , Microbiota , Oligoelementos , Poluentes Químicos da Água , Mercúrio/análise , Oligoelementos/análise , Sedimentos Geológicos/análise , Monitoramento Ambiental/métodos , Poluentes Químicos da Água/análise , Compostos de Metilmercúrio/análise
19.
J Hazard Mater ; 438: 129464, 2022 09 15.
Artigo em Inglês | MEDLINE | ID: mdl-35999716

RESUMO

S-impregnation of biochar through elemental S streaming is known to increase its sorption performance against Hg and methyl mercury (MeHg). However, the effects of %S-loading on biochar's mechanism and sorption capacities for MeHg, and its consequent impact when used as an amendment material for Hg-contaminated sediments, are poorly understood, and thus, were investigated in this work. Our results showed that a minimum sulfur loading of 1% was the most effective in reducing MeHg levels in sediments. At higher %S-loading (3-20%), the reduction in surface area, pore blockage due to unreacted sulfur particles, and presence of poorly bound sulfur species resulted in lowered effectiveness for MeHg control. Increasing S-functionalization during impregnation shifted the sorption process of MeHg from Hg-O to Hg-S in S-impregnated biochar (BCS). Our 60-day slurry experiment showed a significant reduction in pore water THg (40-70%) and MeHg (30-55%), as well as sediment MeHg (50-60%) in biochar-amended sediments. The reduction in the bioavailable Hg resulted in lowered Hg methylation, as supported by the suppression of both the Fe- and SO42--reduction activities in the amended sediments. The microbial community structure in BCS-amended sediments showed a shift towards sulfur-consuming, iron-reducing, thiosulfate-oxidizing, and sulfate-reducing bacterial populations. At the genus level, the overall relative abundance of principal Hg methylators was also lower in the BCS treatment than in the unamended sediments. This study highlights the application of BCS as a promising strategy for remediation of Hg-contaminated sediments.


Assuntos
Mercúrio , Compostos de Metilmercúrio , Microbiota , Poluentes Químicos da Água , Carvão Vegetal , Sedimentos Geológicos/química , Mercúrio/análise , Metilação , Compostos de Metilmercúrio/metabolismo , Enxofre , Poluentes Químicos da Água/análise
20.
Nat Commun ; 13(1): 4488, 2022 Aug 02.
Artigo em Inglês | MEDLINE | ID: mdl-35918327

RESUMO

Dye arrays from dimers up to larger oligomers constitute the functional units of natural light harvesting systems as well as organic photonic and photovoltaic materials. Whilst in the past decades many photophysical studies were devoted to molecular dimers for deriving structure-property relationship to unravel the design principles for ideal optoelectronic materials, they fail to accomplish the subsequent processes of charge carrier generation or the detachment of two triplet species in singlet fission (SF). Here, we present a slip-stacked perylene bisimide trimer, which constitutes a bridge between hitherto studied dimer and solid-state materials, to investigate SF mechanisms. This work showcases multiple pathways towards the multiexciton state through direct or excimer-mediated mechanisms by depending upon interchromophoric interaction. These results suggest the comprehensive role of the exciton coupling, exciton delocalization, and excimer state to facilitate the SF process. In this regard, our observations expand the fundamental understanding the structure-property relationship in dye arrays.

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