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Increase in Agricultural-Derived NH<sub> <i>x</i> </sub> and Decrease in Coal Combustion-Derived NO<sub> <i>x</i> </sub> Result in Atmospheric Particulate N-NH<sub>4</sub> <SUP>+</SUP> Surpassing N-NO<sub>3</sub> <SUP>-</SUP> in the South China Sea
No full textThe atmospheric deposition of anthropogenic active nitrogen significantly influences marine primary productivity and contributes to eutrophication. The form of nitrogen deposition has been evolving annually, alongside changes in human activities. A disparity arises between observation results and simulation conclusions due to the limited field observation and research in the ocean. To address this gap, our study undertook three field cruises in the South China Sea in 2021, the largest marginal sea of China. The objective was to investigate the latest atmospheric particulate inorganic nitrogen deposition pattern and changes in nitrogen sources, employing nitrogen-stable isotopes of nitrate (delta 15N-NO3-) and ammonia (delta 15N-NH4+) linked to a mixing model. The findings reveal that the N-NH4+ deposition generally surpasses N-NO3- deposition, attributed to a decline in the level of NO x emission from coal combustion and an upswing in the level of NH x emission from agricultural sources. The disparity in deposition between N-NH4+ and N-NO3- intensifies from the coast to the offshore, establishing N-NH4+ as the primary contributor to oceanic nitrogen deposition, particularly in ocean background regions. Fertilizer (33 +/- 21%) and livestock (20 +/- 6%) emerge as the primary sources of N-NH4+. While coal combustion continues to be a significant contributor to marine atmospheric N-NO3-, its proportion has diminished to 22 (Northern Coast)-35% (background area) due to effective NOx emission controls by the countries surrounding the South China Sea, especially the Chinese Government. As coal combustion's contribution dwindles, the significance of vessel and marine biogenic emissions grows. The daytime higher atmospheric N-NO3- concentration and lower delta N-15-NO3- compared with nighttime further underscore the substantial role of marine biogenic emissions
Estimation and verification of green tide biomass based on UAV remote sensing
No full textSince 2007, the Yellow Sea green tide has broken out every summer, causing great harm to the environment and society. Although satellite remote sensing (RS) has been used in biomass research, there are several shortcomings, such as mixed pixels, atmospheric interference, and difficult field validation. The biomass of green tide has been lacking a high-precision estimation method. In this study, high-resolution unmanned aerial vehicle (UAV) RS was used to quantitatively map the biomass of green tides. By utilizing experimental data from previous studies, a robust relationship was established to link biomass to the red-green-blue floating algae index (RGB-FAI). Then, the lab-based model for green tide biomass from visible images taken by the UAV camera was developed and validated by field measurements. Results show that the accurate and cost-effective method is able to estimate the green tide biomass and its changes in given local waters of the near and far seas. The study provided an effective complement to the traditional satellite RS, as well as high-precision quantitative techniques for decision-making in disaster management
Unveiling the fast adsorption and desorption of heavy metals on/off nanoplastics by real-time in-situ potentiometric sensing
No full textNanoplastics (<1 mu m) can serve as a transport vector of environmental pollutants (e.g., heavy metals) and change their toxicities and bioavailabilities. Up to date the behaviors of adsorption and desorption heavy metals on/off nanoplastics are largely unknown. Herein, polymeric membrane potentiometric ion sensors are proposed for in-situ assessment of the real-time kinetics of heavy metal adsorption and desorption on/off nanoplastics. Results show that nanoplastics can adsorb and release heavy metals in a fast manner, indicating their superior ability in transferring heavy metals. The adsorption behaviors are closely related to the characteristics of nanoplastics and background electrolytes. Particle aggregation and increases in salinity and acidity suppress the adsorption of heavy metals on nanoplastics. The desorption efficiencies of different heavy metals are Pb2+ (31 %) < Cu2+ (40 %) < Cd2+ (97 %). Our proposed method is applicable for the detection of the plastic pollutants with size <100 nm and of the samples with high salinities (e.g., seawater). This work would provide new insights into the assessment of environmental risks posed by nanoplastics and heavy metals
Molecularly imprinted polymers and porous organic frameworks based analytical methods for disinfection by-products in water and wastewater
No full textDisinfection by-products (DBPs) with heritage toxicity, mutagenicity and carcinogenicity are one kind of important new pollutants, and their detection and removal in water and wastewater has become a common challenge facing mankind. Advanced functional materials with ideal selectivity, adsorption capacity and regeneration capacity provide hope for the determination of DBPs with low concentration levels and inherent molecular structural similarity. Among them, molecularly imprinted polymers (MIPs) are favored, owing to their predictable structure, specific recognition and wide applicability. Also, metal-organic frameworks (MOFs) and covalent-organic frameworks (COFs) with unique pore structure, large specific surface area and easy functionalization, attract increasing interest. Herein, we review recent advances in analytical methods based on the above-mentioned three functional materials for DBPs in water and wastewater. Firstly, MIPs, MOFs and COFs are briefly introduced. Secondly, MIPs, MOFs and COFs as extractants, recognition element and adsorbents, are comprehensively discussed. Combining the latest research progress of solid-phase extraction (SPE), sensor, adsorption and nanofiltration, typical examples on MIPs and MOFs/COFs based analytical and removal applications in water and wastewater are summarized. Finally, the application prospects and challenges of the three functional materials in DBPs analysis are proposed to promote the development of corresponding analytical methods
Molecularly imprinted polymer-coated silica microbeads for high-performance liquid chromatography
No full textMolecularly imprinted polymer (MIP)-based chromatographic separation materials, owing to their advantages of unique selectivity, low cost, suitable reproducibility, and acceptable stability, have attracted a great deal of research in different fields. In this investigation, a new type of MIP-coated silica (MIP/SiO2) separation material was developed using sulfamethoxazole as a template; the specific recognition ability of MIP and appropriate physicochemical properties (abundant Si-OH, suitable pore structure, good stability, etc.) of SiO2 microbeads were combined. The MIP/SiO2 separation materials were characterized carefully. Then, various compounds (such as sulfonamides, ginsenosides, nucleosides, and several pesticides) were used to comprehensively evaluate the chromatographic performances of the MIP/SiO2 column. Furthermore, the chromatographic performances of the MIP/SiO2 column were compared with those of other separation materials (such as non-imprinted polymer-coated silica, C18/SiO2, and bare silica) packed columns. The resolution value of all measured compounds was more than 1.51. The column efficiencies of 13 510 plates per meter (N m-1) for sulfamethoxazole, 11 600 N m-1 for ginsenoside Rd, and 10 510 N m-1 for 2 '-deoxyadenosine were obtained. The acceptable results verified that the MIP/SiO2 column can be applied to separate highly polar drugs such as sulfonamides, ginsenosides, nucleosides, and pesticides.
Molecularly imprinted polymer-based chromatographic separation materials, owing to their advantages of unique selectivity, low cost, suitable reproducibility, and acceptable stability, have attracted a great deal of research in different fields
Spatial distribution, compositional pattern, and source apportionment of colloidal trace metals in the coastal water of Shandong Peninsula, northeastern China
No full textThe Shandong Peninsula (SP) is the largest peninsula in China hosting rich economic and agricultural activities. In this study, we investigated the behavior of dissolved Mn, Fe, Cu, Zn, Cd, and Pb and their colloidal phases in the coastal and estuarine areas of SP. Pb and Zn had the highest contamination factors of 0.22-10.15 and 0.90-4.41, respectively. The <1 kDa accounted for 23-57 % of the total dissolved phase. Mn, Fe, Cu, Zn, Cd, and Pb were more likely to bind to 100 kDa-0.45 mu m colloids (21-57 %). For colloidal Fe and Cu, the adsorption-release behavior had more significant effects on their dynamics. In contrast, the changes in colloidal Mn, Cd, and Pb were mainly controlled by the combined influence of temperature, dissolved oxygen, and microbial activity. However, the 1-3 kDa Zn exhibited a greater pH-dependent dispersion and was significantly positively correlated with it
Removal of enrofloxacin as well as nutrients in mariculture water by<i> Sesuvium</i><i> portulacastrum</i> system: Insights for biodegradation, ecotoxicity of enrofloxacin
No full textAntibiotic contamination and eutrophication in mariculture have become problems that cannot be ignored, and enrofloxacin (ENR), as an example, is especially widely used in mariculture. This study firstly revealed that Sesuvium portulacastrum, a plant with world-wide distribution in coastal zones, with its rhizosphere microorganisms, could remove ENR as well as nutrients. The S. portulacastrum system could degrade ENR to small-molecule products 1,2,3,4-tetrahydroquinolin-4-ol and (2,4-dihydroxyphenyl)-cyclopropylamine. And there were 81.3-39.2 % removals of ENR with 0.01-100 mg/L. Although ENR significantly influenced functions of rhizosphere microbial community, like decreasing nitrogen fixation, shifting trophic strategies from phototrophy to chemoheterotrophy, nutrients (NH4+-N, NO2--N, NO3--N and total dissolved phosphorus) removal of S. portulacastrum system was essentially unaffected at low ENR concentration (< 1 mg/L). The removal mechanism of S. portulacastrum system was explored. Neither of the isolated root exudates and rhizosphere bacteria could degrade ENR, however, without rhizosphere bacteria, ENR removal rate would decrease. Root proteins including oxidase, decarboxylase, dehydrogenase, such as laccase, isocitrate dehydrogenase, delta-1-pyrroline-5-carboxylate dehydrogenase were overexpressed. Additionally, endocytosis is a pathway for antibiotics to enter S. portulacastrum. This study demonstrated that S. portulacastrum system could be used for remediation of antibiotics-nutrients combined pollution, and deepened understanding the antibiotic removal mechanism of macrophytes in mariculture, moreover, provided new macroplant species and a theoretical basis for antibiotics removal in aquatic systems
Shining light on carbon dots: Toward enhanced antibacterial activity for biofilm disruption
No full textIn spite of tremendous efforts dedicated to addressing bacterial infections and biofilm formation, the post-antibiotic ear continues to witness a gap between the established materials and an easily accessible yet biocompatible antibacterial reagent. Here we show carbon dots (CDs) synthesized via a single hydrothermal process can afford promising antibacterial activity that can be further enhanced by exposure to light. By using citric acid and polyethyleneimine as the precursors, the photoluminescence CDs can be produced within a one-pot, one-step hydrothermal reaction in only 2 h. The CDs demonstrate robust antibacterial properties against both Gram-positive and Gram-negative bacteria and, notably, a considerable enhancement of antibacterial effect can be observed upon photo-irradiation. Mechanistic insights reveal that the CDs generate singlet oxygen (1O2) when exposed to light, leading to an augmented reactive oxygen species level. The approach for disruption of biofilms and inhibition of biofilm formation by using the CDs has also been established. Our findings present a potential solution to combat antibacterial resistance and offer a path to reduce dependence on traditional antibiotics.
Shining carbon dots (CDs) produced by a single-step hydrothermal method can afford enhanced antibacterial activity against both Gram-positive and Gram-negative bacteria. Mechanistic insights reveal that the CDs generate singlet oxygen (1O2) under light irradiation, contributing to an augmented ROS level, facilitating disruption of biofilms and inhibition of biofilm formation. imag
Multiple serial correlations in global air temperature anomaly time series
No full textSerial correlations within temperature time series serve as indicators of the temporal consistency of climate events. This study delves into the serial correlations embedded in global surface air temperature (SAT) data. Initially, we preprocess the SAT time series to eradicate seasonal patterns and linear trends, resulting in the SAT anomaly time series, which encapsulates the inherent variability of Earth's climate system. Employing diverse statistical techniques, we identify three distinct types of serial correlations: short-term, long-term, and nonlinear. To identify short-term correlations, we utilize the first-order autoregressive model, AR(1), revealing a global pattern that can be partially attributed to atmospheric Rossby waves in extratropical regions and the Eastern Pacific warm pool. For long-term correlations, we adopt the standard detrended fluctuation analysis, finding that the global pattern aligns with long-term climate variability, such as the El Ni & ntilde;o-Southern Oscillation (ENSO) over the Eastern Pacific. Furthermore, we apply the horizontal visibility graph (HVG) algorithm to transform the SAT anomaly time series into complex networks. The topological parameters of these networks aptly capture the long-term correlations present in the data. Additionally, we introduce a novel topological parameter, Delta sigma, to detect nonlinear correlations. The statistical significance of this parameter is rigorously tested using the Monte Carlo method, simulating fractional Brownian motion and fractional Gaussian noise processes with a predefined DFA exponent to estimate confidence intervals. In conclusion, serial correlations are universal in global SAT time series and the presence of these serial correlations should be considered carefully in climate sciences
Enhanced Selectivity in Microdroplet-Mediated Enzyme Catalysis
No full textNatural enzymes with enhanced catalytic activity and selectivity have long been studied by tuning the microenvironment around the active site, but how to modulate the active-site electric field in a simple fashion remains challenging. Here, we demonstrate that microdroplets as a simple yet versatile reactor can enhance the electric field at the active site of an enzyme. By using horseradish peroxidase as a model, improved selectivity in microdroplet-mediated enzyme catalysis can be obtained. Quantum mechanical/molecular dynamics calculations and vibrational Stark spectroscopy reveal that the electric field at the microdroplet interface can influence the electrostatic preorganization and orientation of the enzyme to enhance its internal electric field. As a result, the free energies of the substrate and heme can be tuned by the internal electric field, thereby changing its catalytic reaction pathway for a classical substrate, 3,3 ',5,5 '-tetramethylbenzidine, and enabling selective C-N additions for specific substrates. This finding provides a green, simple, and effective way to modulate enzyme-catalyzed reactions and holds promise for a broad spectrum of biosensing and biosynthesis applications