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1.
Appl Environ Microbiol ; 90(10): e0095124, 2024 Oct 23.
Artigo em Inglês | MEDLINE | ID: mdl-39248462

RESUMO

Bacteriophages offer an opportunity for chemical-free, precise control of problematic bacteria, but this approach can be limited when lytic phages are difficult to obtain for the target host. In such cases, phage-based targeting of cooperating or cross-feeding bacteria (e.g., Streptococcus gordonii) can be an effective approach to control the problematic bacteria (e.g., Porphyromonas gingivalis). Using a dual-species biofilm system, phage predation of S. gordonii (108 PFU·mL-1) decreased the abundance of pathogenic P. gingivalis by >99% compared with no-treatment controls, while also inhibiting the production of cytotoxic metabolic end products (butyric and propionic acids). Phage treatment upregulated genes associated with interspecies co-adhesion (5- to 8-fold) and quorum sensing (10-fold) in residual P. gingivalis, which is conducive to increased potential to bind to S. gordonii. Counterintuitively, lower-titer phage applications (104 PFU·mL-1) increased the production of extracellular polymeric substance (EPS) by 22% and biofilm biomass by 50%. This overproduction of EPS may contribute to the phenomenon where the biofilm separated into two distinct species layers, as observed by confocal laser scanning microscopy. Although more complex mixed-culture systems should be considered to delineate the merits and limitations of this novel biocontrol approach (which would likely require the use of phage cocktails), our results offer proof of concept that indirect phage-based targeting can expand the applicability of phage-based control of pathogenic bacteria for public health protection. IMPORTANCE: Lytic phages are valuable agents for targeted elimination of bacteria in diverse applications. Nevertheless, lytic phages are difficult to isolate for some target pathogens. We offer proof of concept that this limitation may be overcome via indirect phage targeting, which involves knocking out species that interact closely with and benefit the primary problematic target bacteria. Our target (P. gingivalis) only forms a periodontal pathogenic biofilm if the pioneer colonizer (S. gordonii) offers its surface for P. gingivalis to attach. Phage predation of the co-adhesive S. gordonii significantly reduced abundance of the target pathogen by >99%, decreased the total biofilm biomass by >44%, and suppressed its production of cytotoxic metabolic byproducts. Thus, this research extends the scope of phage-based biocontrol for public health protection.


Assuntos
Bacteriófagos , Biofilmes , Porphyromonas gingivalis , Streptococcus gordonii , Porphyromonas gingivalis/virologia , Porphyromonas gingivalis/fisiologia , Bacteriófagos/fisiologia , Bacteriófagos/genética , Streptococcus gordonii/fisiologia , Streptococcus gordonii/virologia , Percepção de Quorum
2.
Environ Sci Technol ; 58(35): 15475-15485, 2024 Sep 03.
Artigo em Inglês | MEDLINE | ID: mdl-39172699

RESUMO

Nanoplastics represent a global environmental concern due to their ubiquitous presence and potential adverse impacts on public and environmental health. There is a growing need to advance the mechanistic understanding of their reactivity as they interact with biological and environmental systems. Herein, for the first time, we report that polystyrene nanoplastics (PSNPs) have intrinsic peroxidase-like activity and are able to mediate oxidative stress. The peroxidase-like activity is dependent on temperature and pH, with a maximum at pH 4.5 and 40 °C. The catalytic activity exhibits saturation kinetics, as described by the Michaelis-Menten model. The peroxidase-like activity of PSNPs is attributed to their ability to mediate electron transfer from peroxidase substrates to H2O2. Ozone-induced PSNP aging can introduce oxygen-containing groups and disrupt aromatic structures on the nanoplastic surface. While ozonation initially enhances peroxidase-like activity by increasing oxygen-containing groups without degrading many aromatic structures, extended ozonation destroys aromatic structures, significantly reducing this activity. The peroxidase-like activity of PSNPs can mediate oxidative stress, which is generally positively correlated with their aromatic structures, as suggested by the ascorbic acid assay. These results help explain the reported oxidative stress exerted by nanoplastics and provide novel insights into their environmental and public health implications.


Assuntos
Estresse Oxidativo , Ozônio , Poliestirenos , Poliestirenos/química , Peroxidase/metabolismo , Peróxido de Hidrogênio , Concentração de Íons de Hidrogênio
3.
Environ Sci Technol ; 2024 Jul 17.
Artigo em Inglês | MEDLINE | ID: mdl-39021055

RESUMO

Transition metal catalysts in soil constituents (e.g., clays) can significantly decrease the pyrolytic treatment temperature and energy requirements for efficient removal of polycyclic aromatic hydrocarbons (PAHs) and, thus, lead to more sustainable remediation of contaminated soils. However, the catalytic mechanism and its rate-limiting steps are not fully understood. Here, we show that PAHs with lower ionization potential (IP) are more easily removed by pyro-catalytic treatment when deposited onto Fe-enriched bentonite (1.8% wt. ion-exchanged content). We used four PAHs with decreasing IP: naphthalene > pyrene > benz(a)anthracene > benzo(g,h,i)perylene. Density functional theory (DFT) calculations showed that lower IP results in stronger PAH adsorption to Fe(III) sites and easier transfer of π-bond electrons from the aromatic ring to Fe(III) at the onset of pyrolysis. We postulate that the formation of aromatic radicals via this direct electron transfer (DET) mechanism is the initiation step of a cascade of aromatic polymerization reactions that eventually convert PAHs to a non-toxic and fertility-preserving char, as we demonstrated earlier. However, IP is inversely correlated with PAH hydrophobicity (log Kow), which may limit access to the Fe(III) catalytic sites (and thus DET) if it increases PAH sorption to soil OM. Thus, ensuring adequate contact between sorbed PAHs and the catalytic reaction centers represents an engineering challenge to achieve faster remediation with a lower carbon footprint via pyro-catalytic treatment.

4.
Environ Sci Technol ; 58(22): 9887-9895, 2024 Jun 04.
Artigo em Inglês | MEDLINE | ID: mdl-38775679

RESUMO

Mercury is a ubiquitous heavy-metal pollutant and poses serious ecological and human-health risks. There is an ever-growing demand for rapid, sensitive, and selective detection of mercury in natural waters, particularly for regions lacking infrastructure specialized for mercury analysis. Here, we show that a sensor based on multi-emission carbon dots (M-CDs) exhibits ultrahigh sensing selectivity toward Hg(II) in complex environmental matrices, tested in the presence of a range of environmentally relevant metal/metalloid ions as well as natural and artificial ligands, using various real water samples. By incorporating structural features of calcein and folic acid that enable tunable emissions, the M-CDs couple an emission enhancement at 432 nm and a simultaneous reduction at 521 nm, with the intensity ratio linearly related to the Hg(II) concentration up to 1200 µg/L, independent of matrix compositions. The M-CDs have a detection limit of 5.6 µg/L, a response time of 1 min, and a spike recovery of 94 ± 3.7%. The intensified emission is attributed to proton transfer and aggregation-induced emission enhancement, whereas the quenching is due to proton and electron transfer. These findings also have important implications for mercury identification in other complex matrices for routine, screening-level food safety and health management practices.


Assuntos
Carbono , Mercúrio , Poluentes Químicos da Água , Mercúrio/análise , Carbono/química , Poluentes Químicos da Água/análise , Fluorescência , Pontos Quânticos/química , Água/química
5.
Environ Sci Technol ; 58(26): 11833-11842, 2024 Jul 02.
Artigo em Inglês | MEDLINE | ID: mdl-38910294

RESUMO

Atomic hydrogen (H*) is a powerful and versatile reductant and has tremendous potential in the degradation of oxidized pollutants (e.g., chlorinated solvents). However, its application for groundwater remediation is hindered by the scavenging side reaction of H2 evolution. Herein, we report that a composite material (Fe0@Fe-N4-C), consisting of zerovalent iron (Fe0) nanoparticles and nitrogen-coordinated single-atom Fe (Fe-N4), can effectively steer H* toward reductive dechlorination of trichloroethylene (TCE), a common groundwater contaminant and primary risk driver at many hazardous waste sites. The Fe-N4 structure strengthens the bond between surface Fe atoms and H*, inhibiting H2 evolution. Nonetheless, H* is available for dechlorination, as the adsorption of TCE weakens this bond. Interestingly, H* also enhances electron delocalization and transfer between adsorbed TCE and surface Fe atoms, increasing the reactivity of adsorbed TCE with H*. Consequently, Fe0@Fe-N4-C exhibits high electron selectivity (up to 86%) toward dechlorination, as well as a high TCE degradation kinetic constant. This material is resilient against water matrix interferences, achieving long-lasting performance for effective TCE removal. These findings shed light on the utilization of H* for the in situ remediation of groundwater contaminated with chlorinated solvents, by rational design of earth-abundant metal-based single-atom catalysts.


Assuntos
Água Subterrânea , Ferro , Solventes , Poluentes Químicos da Água , Água Subterrânea/química , Ferro/química , Solventes/química , Poluentes Químicos da Água/química , Hidrogênio/química , Tricloroetileno/química , Halogenação , Recuperação e Remediação Ambiental/métodos , Oxirredução , Adsorção
6.
Environ Sci Technol ; 58(16): 7186-7195, 2024 Apr 23.
Artigo em Inglês | MEDLINE | ID: mdl-38598770

RESUMO

Remediation of large and dilute plumes of groundwater contaminated by oxidized pollutants such as chromate is a common and difficult challenge. Herein, we show that in situ formation of FeS nanoparticles (using dissolved Fe(II), S(-II), and natural organic matter as a nucleating template) results in uniform coating of aquifer material to create a regenerable reactive zone that mitigates Cr(VI) migration. Flow-through columns packed with quartz sand are amended first with an Fe2+ solution and then with a HS- solution to form a nano-FeS coating on the sand, which does not hinder permeability. This nano-FeS coating effectively reduces and immobilizes Cr(VI), forming Fe(III)-Cr(III) coprecipitates with negligible detachment from the sand grains. Preconditioning the sand with humic or fulvic acid (used as model natural organic matter (NOM)) further enhances Cr(VI) sequestration, as NOM provides additional binding sites of Fe2+ and mediates both nucleation and growth of FeS nanoparticles, as verified with spectroscopic and microscopic evidence. Reactivity can be easily replenished by repeating the procedures used to form the reactive coating. These findings demonstrate that such enhancement of attenuation capacity can be an effective option to mitigate Cr(VI) plume migration and exposure, particularly when tackling contaminant rebound post source remediation.


Assuntos
Cromo , Água Subterrânea , Oxirredução , Poluentes Químicos da Água , Água Subterrânea/química , Cromo/química , Poluentes Químicos da Água/química , Nanopartículas/química , Recuperação e Remediação Ambiental/métodos , Substâncias Húmicas , Compostos Ferrosos/química , Benzopiranos/química
7.
Environ Sci Technol ; 2024 Sep 16.
Artigo em Inglês | MEDLINE | ID: mdl-39279665

RESUMO

Conventional approaches for in situ remediation of mercury (Hg)-contaminated soils and sediments rely mostly on precipitation or adsorption. However, this can generate Hg-rich surfaces that facilitate microbial production of methylmercury (MeHg), a potent, bioaccumulative neurotoxin. Herein, we prove the concept that the risk of mercury methylation can be effectively minimized by adding sulfur-intercalated layered double hydroxide (S-LDH) to Hg-contaminated soils. Hg bound to S-LDH has minimal methylation potential when incubated with model methylating bacteria Pseudodesulfovibrio mercurii ND132 and Geobacter sulfurreducens PCA. With a combination of spectroscopic and microscopic evidence, as well as theoretical calculations, we confirm that dissolved Hg(II) tends to enter the interlayers of S-LDH to bind to the sulfur groups intercalated within, leading to the formation of nanoscale metacinnabar (ß-HgS). This not only physically blocks the contact of methylating microorganisms but also inhibits secondary release of bound mercury in the presence of strong binding ligands in porewater. This study highlights the promising concept of in situ risk reduction of heavy metal contamination by inducing precipitation within (nano)confined domains, achieving a sustainable outcome of enhanced removal and reduced bioaccessibility for pollutants that may otherwise be bioavailable in the form of nanoprecipitates.

8.
Environ Sci Technol ; 58(29): 13110-13119, 2024 Jul 23.
Artigo em Inglês | MEDLINE | ID: mdl-38989600

RESUMO

Transition-metal dichalcogenides (TMDs) have shown great promise as selective and high-capacity sorbents for Hg(II) removal from water. Yet, their design should consider safe disposal of spent materials, particularly the subsequent formation of methylmercury (MeHg), a highly potent and bioaccumulative neurotoxin. Here, we show that microbial methylation of mercury bound to MoS2 nanosheets (a representative TMD material) is significant under anoxic conditions commonly encountered in landfills. Notably, the methylation potential is highly dependent on the phase compositions of MoS2. MeHg production was higher for 1T MoS2, as mercury bound to this phase primarily exists as surface complexes that are available for ligand exchange. In comparison, mercury on 2H MoS2 occurs largely in the form of precipitates, particularly monovalent mercury minerals (e.g., Hg2MoO4 and Hg2SO4) that are minimally bioavailable. Thus, even though 1T MoS2 is more effective in Hg(II) removal from aqueous solution due to its higher adsorption affinity and reductive ability, it poses a higher risk of MeHg formation after landfill disposal. These findings highlight the critical role of nanoscale surfaces in enriching heavy metals and subsequently regulating their bioavailability and risks and shed light on the safe design of heavy metal sorbent materials through surface structural modulation.


Assuntos
Mercúrio , Metilação , Adsorção , Nanoestruturas/química , Poluentes Químicos da Água/química , Compostos de Metilmercúrio , Molibdênio/química
9.
Environ Sci Technol ; 58(41): 18368-18378, 2024 Oct 15.
Artigo em Inglês | MEDLINE | ID: mdl-39370945

RESUMO

Mercury nanoparticles are abundant in natural environments. Yet, understanding their contribution to global biogeochemical cycling of mercury remains elusive. Here, we show that microbial transformation of nanoparticulate divalent mercury can be an important source of elemental and methylmercury.Geobacter sulfurreducensPCA, a model bacterium predominant in anoxic environments (e.g., paddy soils), simultaneously reduces and methylates nanoparticulate Hg(II). Moreover, the relative prevalence of these two competing processes and the dominant transformation pathways differ markedly between nanoparticulate Hg(II) and its dissolved and bulk-sized counterparts. Notably, even when intracellular reduction of Hg(II) nanoparticles is constrained by cross-membrane transport (a rate-limiting step that also regulates methylation), the overall Hg(0) formation remains substantial due to extracellular electron transfer. With multiple lines of evidence based on microscopic and electrochemical analyses, gene knockout experiments, and theoretical calculations, we show that nanoparticulate Hg(II) is preferentially associated with c-type cytochromes on cell membranes and has a higher propensity for accepting electrons from the heme groups than adsorbed ionic Hg(II), which explains the surprisingly larger extent of reduction of nanoparticles than dissolved Hg(II) at relatively high mercury loadings. These findings have important implications for the assessment of global mercury budgets as well as the bioavailability of nanominerals and mineral nanoparticles.


Assuntos
Mercúrio , Mercúrio/metabolismo , Metilação , Transporte de Elétrons , Oxirredução , Geobacter/metabolismo , Nanopartículas/química , Nanopartículas Metálicas/química
10.
Environ Sci Technol ; 58(1): 3-16, 2024 Jan 09.
Artigo em Inglês | MEDLINE | ID: mdl-38193155

RESUMO

Water reuse is rapidly becoming an integral feature of resilient water systems, where municipal wastewater undergoes advanced treatment, typically involving a sequence of ultrafiltration (UF), reverse osmosis (RO), and an advanced oxidation process (AOP). When RO is used, a concentrated waste stream is produced that is elevated in not only total dissolved solids but also metals, nutrients, and micropollutants that have passed through conventional wastewater treatment. Management of this RO concentrate─dubbed municipal wastewater reuse concentrate (MWRC)─will be critical to address, especially as water reuse practices become more widespread. Building on existing brine management practices, this review explores MWRC management options by identifying infrastructural needs and opportunities for multi-beneficial disposal. To safeguard environmental systems from the potential hazards of MWRC, disposal, monitoring, and regulatory techniques are discussed to promote the safety and affordability of implementing MWRC management. Furthermore, opportunities for resource recovery and valorization are differentiated, while economic techniques to revamp cost-benefit analysis for MWRC management are examined. The goal of this critical review is to create a common foundation for researchers, practitioners, and regulators by providing an interdisciplinary set of tools and frameworks to address the impending challenges and emerging opportunities of MWRC management.


Assuntos
Ultrafiltração , Águas Residuárias , Epicloroidrina , Nutrientes , Água
11.
J Environ Manage ; 370: 122527, 2024 Sep 26.
Artigo em Inglês | MEDLINE | ID: mdl-39332296

RESUMO

Ecosystem multi-functionality is a key concept when measured to protect forests from natural and anthropogenic disturbances, such as fire prevention techniques, must be adopted. Despite this importance, scarce studies have analysed the impacts of prescribed burning and aboveground vegetation management on ecosystem functions and overall multi-functionality. To fill this gap, this study has evaluated the changes in some ecosystem properties and structure (associated with soil characteristics and plant diversity, respectively), in important forest functions, and the overall ecosystem multi-functionality in a Mediterranean pine forest of Castilla La Mancha (Central Eastern Spain) under three site conditions: (i) undisturbed ecosystem; (ii) forest subjected to mechanical shredding of aboveground vegetation (hereafter "AVMS"); and (iii) forest treated as above and then with prescribed fire ("AVMS + PF"). The results of the study have shown that neither the PF nor AVMS have significantly modified the structure, properties and functions as well as the overall multi-functionality of the forest ecosystem. These slight impacts of the treatments are due to the low fire severity of the prescribed burning and the long time elapsed from the vegetation management. Among the studied ecosystem functions, organic matter decomposition (driven by the enzymatic activities and soil basal respiration), water cycle (influenced by soil water content and water infiltration), carbon stock (linked to soil organic matter) and biomass production decreased, when species richness and plant diversity increased. The study is useful to indicate the feasibility of forest management actions for fire prevention in delicate forest ecosystems of the Mediterranean environments.

12.
J Environ Manage ; 354: 120316, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38382429

RESUMO

Traditional management practices, such as grazing, can have adverse impact on soils. Despite an extensive body of literature exploring the effects of grazing on soil and plants worldwide, there is a notable lack of research on its impacts in Mediterranean forests within the Iberian Peninsula Furthermore, there is a knowledge gap on the enzymatic activities and basal respiration of soil in forest after grazing. To address these gaps, this study aimed to investigate the impact of grazing on various important physicochemical and biological soil properties along with vegetation richness in a Mediterranean forest located in Castilla-La Mancha (Central Eastern Spain). Relative to undisturbed sites, grazing significantly reduced soil water content (-53%) and available water (-59%). However, soil hydraulic conductivity remained unaffected by animal trampling and the soil water repellency observed in ungrazed sites disappeared. Grazed soils experienced a slight increase in pH (+18%). Among the biochemical properties studied, only dehydrogenase showed a significant increase (+100%) while basal respiration exhibited a notable decrease (-24%). Grazing resulted in a reduction of plant species richness (-34%) indicating a loss of biodiversity in grazed areas. The observed significant alterations in key soil and plant properties due to livestock activity suggest that grazing has the potential to modify the overall soil quality of these sites. Certain variables that exhibited noteworthy differences between grazed and ungrazed sites could serve as indicators of grazing impacts in Mediterranean forests. These indicators may be considered proxies for establishing effective land management strategies to mitigate degradation in the Mediterranean forest ecosystem.


Assuntos
Ecossistema , Solo , Animais , Solo/química , Espanha , Florestas , Plantas , Água
13.
Environ Sci Technol ; 57(33): 12153-12179, 2023 08 22.
Artigo em Inglês | MEDLINE | ID: mdl-37535865

RESUMO

Urbanization and industrialization have exerted significant adverse effects on water quality, resulting in a growing need for reliable and eco-friendly treatment technologies. Persulfate (PS)-based advanced oxidation processes (AOPs) are emerging as viable technologies to treat challenging industrial wastewaters or remediate groundwater impacted by hazardous wastes. While the generated reactive species can degrade a variety of priority organic contaminants through radical and nonradical pathways, there is a lack of systematic and in-depth comparison of these pathways for practical implementation in different treatment scenarios. Our comparative analysis of reaction rate constants for radical vs. nonradical species indicates that radical-based AOPs may achieve high removal efficiency of organic contaminants with relatively short contact time. Nonradical AOPs feature advantages with minimal water matrix interference for complex wastewater treatments. Nonradical species (e.g., singlet oxygen, high-valent metals, and surface activated PS) preferentially react with contaminants bearing electron-donating groups, allowing enhancement of degradation efficiency of known target contaminants. For byproduct formation, analytical limitations and computational chemistry applications are also considered. Finally, we propose a holistically estimated electrical energy per order of reaction (EE/O) parameter and show significantly higher energy requirements for the nonradical pathways. Overall, these critical comparisons help prioritize basic research on PS-based AOPs and inform the merits and limitations of system-specific applications.


Assuntos
Poluentes Químicos da Água , Purificação da Água , Poluentes Químicos da Água/análise , Oxirredução , Águas Residuárias , Purificação da Água/métodos
14.
Environ Sci Technol ; 57(38): 14373-14383, 2023 09 26.
Artigo em Inglês | MEDLINE | ID: mdl-37683087

RESUMO

Transition metal catalysts can significantly enhance the pyrolytic remediation of soils contaminated with polycyclic aromatic hydrocarbons (PAHs). Significantly higher pyrene removal efficiency was observed after the pyrolytic treatment of Fe-enriched bentonite (1.8% wt ion-exchanged content) relative to natural bentonite or soil (i.e., 93% vs 48% and 4%) at the unprecedentedly low temperature of 150 °C with only 15 min treatment time. DFT calculations showed that bentonite surfaces with Fe3+ or Cu2+ adsorb pyrene stronger than surfaces with Zn2+ or Na+. Enhanced pyrene adsorption results from increased charge transfer from its aromatic π-bonds to the cation site, which destabilizes pyrene allowing for faster degradation at lower temperatures. UV-Vis and GC-MS analyses revealed pyrene decomposition products in extracts of samples treated at 150 °C, including small aromatic compounds. As the pyrolysis temperature increased above 200 °C, product distribution shifted from extractable compounds to char coating the residue particles. No extractable byproducts were detected after treatment at 400 °C, indicating that char was the final product of pyrene decomposition. Tests with human lung cells showed that extracts of samples pyrolyzed at 150 °C were toxic; thus, high removal efficiency by pyrolytic treatment does not guarantee detoxification. No cytotoxicity was observed for extracts from Fe-bentonite samples treated at 300 °C, inferring that char is an appropriate treatment end point. Overall, we demonstrate that transition metals in clay can catalyze pyrolytic reactions at relatively low temperatures to decrease the energy and contact times required to meet cleanup standards. However, mitigating residual toxicity may require higher pyrolysis temperatures.


Assuntos
Bentonita , Hidrocarbonetos Policíclicos Aromáticos , Humanos , Temperatura , Bentonita/química , Pirólise , Pirenos/química , Solo
15.
Environ Sci Technol ; 57(41): 15736-15746, 2023 10 17.
Artigo em Inglês | MEDLINE | ID: mdl-37802050

RESUMO

Biofilms give rise to a range of issues, spanning from harboring pathogens to accelerating microbial-induced corrosion in pressurized water systems. Introducing germicidal UV-C (200-280 nm) irradiation from light-emitting diodes (LEDs) into flexible side-emitting optical fibers (SEOFs) presents a novel light delivery method to inhibit the accumulation of biofilms on surfaces found in small-diameter tubing or other intricate geometries. This work used surfaces fully submerged in flowing water that contained Pseudomonas aeruginosa, an opportunistic pathogen commonly found in water system biofilms. A SEOF delivered a UV-C gradient to the surface for biofilm inhibition. Biofilm growth over time was monitored in situ using optical conference tomography. Biofilm formation was effectively inhibited when the 275 nm UV-C irradiance was ≥8 µW/cm2. Biofilm samples were collected from several regions on the surface, representing low and high UV-C irradiance. RNA sequencing of these samples revealed that high UV-C irradiance inhibited the expression of functional genes related to energy metabolism, DNA repair, quorum sensing, polysaccharide production, and mobility. However, insufficient sublethal UV-C exposure led to upregulation genes for SOS response and quorum sensing as survival strategies against the UV-C stress. These results underscore the need to maintain minimum UV-C exposure on surfaces to effectively inhibit biofilm formation in water systems.


Assuntos
Incrustação Biológica , Pseudomonas aeruginosa/fisiologia , Fibras Ópticas , Desinfecção/métodos , Biofilmes/efeitos da radiação , Água , Percepção de Quorum
16.
Environ Sci Technol ; 57(1): 128-138, 2023 01 10.
Artigo em Inglês | MEDLINE | ID: mdl-36525597

RESUMO

In situ aging can change biochar properties, influencing their ecosystem benefits or risks over time. However, there is a lack of field verification of laboratory methods that attempt simulation of long-term natural aging of biochar. We exploited a decade-scale natural charcoal (a proxy for biochar) aging event to determine which lab-aging methods best mimicked field aging. We oxidized charcoal by ultraviolet A radiation (UVA), H2O2, or monochloramine (NH2Cl), and compared it to 10-year field-aged charcoal. We considered seven selected charcoal properties related to surface chemistry and organic matter release, and found that oxidation with 30% H2O2 most representatively simulated 10-year field aging for six out of seven properties. UVA aging failed to approximate oxidation levels while showing a distinctive dissolved organic carbon (DOC) release pattern. NH2Cl-aged charcoal was the most different, showing an increased persistent free radical (PFR) concentration and lower hydrophilicity. All lab oxidation techniques overpredicted polycyclic aromatic hydrocarbon release. The O/C ratio was well-correlated with DOC release, PFR concentration, surface charge, and charcoal pH, indicating the possibility to accurately predict biochar aging with a reduced suite of physicochemical properties. Overall, our rapid and verified lab-aging methods facilitate research toward derisking and enhancing long-term benefits of biochar application.


Assuntos
Carvão Vegetal , Poluentes do Solo , Carvão Vegetal/química , Solo/química , Ecossistema , Peróxido de Hidrogênio
17.
Environ Sci Technol ; 57(10): 4266-4275, 2023 03 14.
Artigo em Inglês | MEDLINE | ID: mdl-36849443

RESUMO

Four-nitrogen-coordinated transitional metal (MN4) configurations in single-atom catalysts (SACs) are broadly recognized as the most efficient active sites in peroxymonosulfate (PMS)-based advanced oxidation processes. However, SACs with a coordination number higher than four are rarely explored, which represents a fundamental missed opportunity for coordination chemistry to boost PMS activation and degradation of recalcitrant organic pollutants. We experimentally and theoretically demonstrate here that five-nitrogen-coordinated Mn (MnN5) sites more effectively activate PMS than MnN4 sites, by facilitating the cleavage of the O-O bond into high-valent Mn(IV)-oxo species with nearly 100% selectivity. The high activity of MnN5 was discerned to be due to the formation of higher-spin-state N5Mn(IV)═O species, which enable efficient two-electron transfer from organics to Mn sites through a lower-energy-barrier pathway. Overall, this work demonstrates the importance of high coordination numbers in SACs for efficient PMS activation and informs the design of next-generation environmental catalysts.


Assuntos
Manganês , Peróxidos , Domínio Catalítico , Manganês/química , Oxirredução
18.
Environ Sci Technol ; 57(45): 17324-17337, 2023 11 14.
Artigo em Inglês | MEDLINE | ID: mdl-37930060

RESUMO

Phages are increasingly recognized for their importance in microbial aggregates, including their influence on microbial ecosystem services and biotechnology applications. However, the adaptive strategies and ecological functions of phages in different aggregates remain largely unexplored. Herein, we used membrane bioreactors to investigate bacterium-phage interactions and related microbial functions within suspended and attached microbial aggregates (SMA vs AMA). SMA and AMA represent distinct microbial habitats where bacterial communities display distinct patterns in terms of dominant species, keystone species, and bacterial networks. However, bacteria and phages in both aggregates exhibited high lysogenicity, with 60% lysogenic phages in the virome and 70% lysogenic metagenome-assembled genomes of bacteria. Moreover, substantial phages exhibited broad host ranges (34% in SMA and 42% in AMA) and closely interacted with habitat generalist species (43% in SMA and 49% in AMA) as adaptive strategies in stressful operation environments. Following a mutualistic pattern, phage-carried auxiliary metabolic genes (pAMGs; 238 types in total) presumably contributed to the bacterial survival and aggregate stability. The SMA-pAMGs were mainly associated with energy metabolism, while the AMA-pAMGs were mainly associated with antioxidant biosynthesis and the synthesis of extracellular polymeric substances, representing habitat-dependent patterns. Overall, this study advanced our understanding of phage adaptive strategies in microbial aggregate habitats and emphasized the importance of bacterium-phage symbiosis in the stability of microbial aggregates.


Assuntos
Bacteriófagos , Microbiota , Bacteriófagos/genética , Simbiose , Bactérias/genética , Metagenoma
19.
Environ Sci Technol ; 57(26): 9713-9721, 2023 07 04.
Artigo em Inglês | MEDLINE | ID: mdl-37310875

RESUMO

Surveillance of antibiotic resistance genes (ARGs) has been increasingly conducted in environmental sectors to complement the surveys in human and animal sectors under the "One-Health" framework. However, there are substantial challenges in comparing and synthesizing the results of multiple studies that employ different test methods and approaches in bioinformatic analysis. In this article, we consider the commonly used quantification units (ARG copy per cell, ARG copy per genome, ARG density, ARG copy per 16S rRNA gene, RPKM, coverage, PPM, etc.) for profiling ARGs and suggest a universal unit (ARG copy per cell) for reporting such biological measurements of samples and improving the comparability of different surveillance efforts.


Assuntos
Antibacterianos , Genes Bacterianos , Animais , Humanos , Antibacterianos/farmacologia , RNA Ribossômico 16S/genética , Resistência Microbiana a Medicamentos/genética , Metagenômica/métodos
20.
Sensors (Basel) ; 23(3)2023 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-36772647

RESUMO

Wearable technology is playing an increasing role in the development of user-centric applications. In the field of sports, this technology is being used to implement solutions that improve athletes' performance, reduce the risk of injury, or control fatigue, for example. Emotions are involved in most of these solutions, but unfortunately, they are not monitored in real-time or used as a decision element that helps to increase the quality of training sessions, nor are they used to guarantee the health of athletes. In this paper, we present a wearable and a set of machine learning models that are able to deduce runners' emotions during their training. The solution is based on the analysis of runners' electrodermal activity, a physiological parameter widely used in the field of emotion recognition. As part of the DJ-Running project, we have used these emotions to increase runners' motivation through music. It has required integrating the wearable and the models into the DJ-Running mobile application, which interacts with the technological infrastructure of the project to select and play the most suitable songs at each instant of the training.


Assuntos
Desempenho Atlético , Aplicativos Móveis , Dispositivos Eletrônicos Vestíveis , Humanos , Motivação , Aprendizado de Máquina
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