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1.
Engineered nano-sized Cu oxide particles are extensively used in diverse applications. Because aquatic environments are the ultimate “sink” for all contaminants, it is expected that nanoparticles (NP) will follow the same fate. In this study, two marine invertebrates Scrobicularia plana and Hediste diversicolor were chosen as ecotoxicological models. The aim was to evaluate behavioural (burrowing kinetics, feeding rate) and biochemical (biomarkers) responses of S. plana and H. diversicolor exposed in the laboratory to Cu (10 μg L−1) added in natural seawater either in the form of engineered nanoparticles (NPs) of CuO or as dissolved Cu in 2% HNO3. Exposure was characterized by considering (i) the physico-chemical fate of NP (ii) the fraction of labile Cu in experimental media and (iii) Cu bioaccumulation. Results showed high aggregation of CuO NPs in seawater and no additional bioavailable Cu concentrations. Behavioural impairments were observed in S. plana exposed to CuO NPs or soluble Cu whereas in H. diversicolor, only the exposure to soluble Cu led to a burrowing decrease. No obvious neurotoxicity effects were revealed since in both species, no changes in cholinesterasic activity occurred in response to both forms of Cu exposure. Biomarkers of oxidative-stress catalase and glutathione-S-transferase were enhanced in both species whereas superoxide dismutase was increased only in S. plana exposed to CuO NPs. Metallothionein-like protein was increased in bivalves exposed to both forms of Cu. Since, no detectable release of soluble Cu from CuO NPs occurred during the time of experiment, ecotoxicity effects seem to be related to CuO NPs themselves.  相似文献   

2.
Gong N  Shao K  Feng W  Lin Z  Liang C  Sun Y 《Chemosphere》2011,83(4):510-516
Adverse effects of manufactured nickel oxide nanoparticles on the microalgae Chlorellavulgaris were determined by algal growth-inhibition test and morphological observation via transmission electron microscopy (TEM). Results showed that the NiO nanoparticles had severe impacts on the algae, with 72 h EC(50) values of 32.28 mg NiOL(-1). Under the stress of NiO nanoparticles, C. vulgaris cells showed plasmolysis, cytomembrane breakage and thylakoids disorder. NiO nanoparticles aggregated and deposited in algal culture media. The presence of algal cells accelerated aggregation of nanoparticles. Moreover, about 0.14% ionic Ni was released when NiO NPs were added into seawater. The attachment of aggregates to algal cell surface and the presence of released ionic Ni were likely responsible for the toxic effects. Interestingly, some NiO nanoparticles were reduced to zero valence nickel as determined by X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) analysis. The maximum ratios of nickel reduction was achieved at 72 h of exposure, in accordance with the time-course of changes in soluble protein content of treated C. vulgaris, implying that some proteins of algae are involved in the process. Our results indicate that the toxicity and bioavailability of NiO nanoparticles to marine algae are reduced by aggregation and reduction of NiO. Thus, marine algae have the potential for usage in nano-pollution bio-remediation in aquatic system.  相似文献   

3.
The toxicity of commercially-available CuO and ZnO nanoparticles (NPs) to pathogenic bacteria was compared for a beneficial rhizosphere isolate, Pseudomonas chlororaphis O6. The NPs aggregated, released ions to different extents under the conditions used for bacterial exposure, and associated with bacterial cell surface. Bacterial surface charge was neutralized by NPs, dependent on pH. The CuO NPs were more toxic than the ZnO NPs. The negative surface charge on colloids of extracellular polymeric substances (EPS) was reduced by Cu ions but not by CuO NPs; the EPS protected cells from CuO NPs-toxicity. CuO NPs-toxicity was eliminated by a Cu ion chelator, suggesting that ion release was involved. Neither NPs released alkaline phosphatase from the cells’ periplasm, indicating minimal outer membrane damage. Accumulation of intracellular reactive oxygen species was correlated with CuO NPs lethality. Environmental deposition of NPs could create niches for ion release, with impacts on susceptible soil microbes.  相似文献   

4.
Impact of silver nanoparticles on natural marine biofilm bacteria   总被引:1,自引:0,他引:1  
There has been a recent increase in the use of silver nanoparticles (Ag NPs) in a wide range of consumer products due to their highly effective antimicrobial properties. However, Ag NPs give cause for concern since their wide use makes them likely to be released into aquatic ecosystems and potentially affect natural bacterial communities. In this study marine biofilms were grown in situ in a coastal site (Singapore Harbour) and exposed in the laboratory for a further 24 h to 0-2000 μg L−1 of well characterised Ag NPs. Increasing concentrations of Ag NPs caused a significant decrease in biofilm volume and biomass, and Ag uptake by biofilms per unit of volume was also dependent on concentration. Terminal fragment length polymorphisms and subsequent cluster and phylogenetic analysis showed the presence of major bacterial groups in biofilms irrespective of treatment with Ag NPs. This implies that even at the highest concentrations studied these taxonomic groups were not displaced. Nevertheless, biofilm succession was impeded on Ag NP treated biofilms, affecting the relative abundance of major bacterial groups in the biofilm community, with potential longer term effects on biofilm development and function.  相似文献   

5.

Background, aim, and scope  

Sorption of hydrophobic organic compounds (HOCs) to natural organic matter (NOM) is an important process that affects the transport, transformation, bioavailability, and fate of HOCs in the environment. Manufactured nanoparticles (NPs) such as nano-oxides will inevitably enter the environment in the processes of their production, transfer, and use and could be coated by the ubiquitous NOM. Thus, sorption of HOCs to NOM in the environment could be affected by the NP interactions with NOM. Furthermore, the toxicity of nano-oxides could be increased due to the adsorbed HOCs. Therefore, sorption of phenanthrene by nano-Al2O3 coated with humic acid (HA) was examined in this study to explore the possible effect of nanoparticles (NPs) on the environmental behavior of HOCs and the potential environmental and health risks of NPs.  相似文献   

6.
Copper oxide nanoparticles (CuO NPs) are frequently used in a polymer-coated form, to be included in paints or fabrics for antimicrobial properties. Their application in antifouling paints may lead to the contamination of aquatic ecosystems. However, the toxicological risk of NPs in the environment is hard to evaluate due to a lack of knowledge on the mechanisms of NP interaction with biological systems. In this study, we investigated the effect of polymer coating on CuO NP toxicity in the green alga Chlamydomonas reinhardtii by comparing bare and polymer-coated CuO NPs prepared from the same CuO nanopowder. Both CuO NP suspensions were toxic to C. reinhardtii after 6 h treatment to concentrations of 0.005-0.04 g L−1. Bare and polymer-coated CuO NPs induced a decrease of Photosystem II activity and the formation of reactive oxygen species. Polymer-coated CuO NP was found to be more toxic than the uncoated CuO NP. The higher toxicity of CS-CuO NP was mainly associated with the increased capacity of polymer-coated CuO NP to penetrate the cell compared to bare CuO NPs. These results indicates that the high toxicity of polymer-coated CuO NPs in algal cells results of intracellular interactions between NPs and the cellular system.  相似文献   

7.
Fagopyrum esculentum commonly named as buckwheat plant is pseudocereal food crops and healthy herbs but is not known as a bioindicator of environmental condition. In the present study, the effects of ZnO nanoparticles (NPs) and microparticles (MPs) on plant growth, bioaccumulation, and antioxidative enzyme activity in buckwheat were estimated under hydroponic culture. The significant biomass reduction at concentrations of 10–2,000 mg/L was 7.7–26.4 % for the ZnO NP and 11.4–23.5 % for the ZnO MP treatment, (p?<?0.05). ZnO NPs were observed in root cells and root cell surface by scanning electron microscopy and transmission electron microscopy analysis. Zn bioaccumulation in plant increased with increasing treatment concentrations. The upward translocation (translocation factor <0.2) of Zn in plant was higher with the ZnO NP treatment than that with the ZnO MP treatment. Additionally, reactive oxygen species generation by ZnO NPs was estimated as the reduced glutathione level and catalase activity, which would be a predictive biomarker of nanotoxicity. The results are the first study to evaluate the phytotoxicity of ZnO NPs to medicinal plant. F. esculentum can be as a good indicator of plant species in NP-polluted environment.  相似文献   

8.
The increased use of silver nanomaterials presents a risk to aquatic systems due to the high toxicity of silver. The stability, dissolution rates and toxicity of citrate- and polyvinylpyrrolidone-coated silver nanoparticles (AgNPs) were investigated in synthetic freshwater and natural seawater media, with the effects of natural organic matter investigated in freshwater. When sterically stabilised by the large PVP molecules, AgNPs were more stable than when charge-stabilised using citrate, and were even relatively stable in seawater. In freshwater and seawater, citrate-coated AgNPs (Ag–Cit) had a faster rate of dissolution than PVP-coated AgNPs (Ag–PVP), while micron-sized silver exhibited the slowest dissolution rate. However, similar dissolved silver was measured for both AgNPs after 72 h in freshwater (500–600 μg L−1) and seawater (1300–1500 μg L−1), with higher concentrations in seawater attributed to chloride complexation. When determined on a mass basis, the 72-h IC50 (inhibitory concentration giving 50% reduction in algal growth rate) for Pseudokirchneriella subcapitata and Phaeodactylum tricornutum and the 48-h LC50 for Ceriodaphnia dubia exposure to Ag+ (1.1, 400 and 0.11 μg L−1, respectively), Ag–Cit (3.0, 2380 and 0.15 μg L−1, respectively) and Ag–PVP (19.5, 3690 and 2.0 μg L−1, respectively) varied widely, with toxicity in the order Ag+ > Ag–Cit > Ag–PVP. Micron-sized silver treatments elicited much lower toxicity than ionic Ag+ or AgNP to P. subcapitata. However, when related to the dissolved silver released from the nanoparticles the toxicities were similar to ionic silver treatments. The presence of natural organic matter stabilised the particles and reduced toxicity in freshwater. These results indicate that dissolved silver was responsible for the toxicity and highlight the need to account for matrix components such as chloride and organic matter in natural waters that influence AgNP fate and mitigate toxicity.  相似文献   

9.
Kumar A  Pandey AK  Singh SS  Shanker R  Dhawan A 《Chemosphere》2011,83(8):1124-1132
Extensive production and consumption of nanomaterials such as ZnO and TiO2 has increased their release and disposal into the environment. The accumulation of nanoparticles (NPs) in ecosystem is likely to pose threat to non-specific targets such as bacteria. The present study explored the effect of ZnO and TiO2 NPs in a model bacterium, Salmonella typhimurium. The uptake of ZnO and TiO2 bare NPs in nano range without agglomeration was observed in S. typhimurium. TEM analysis demonstrated the internalization and uniform distribution of NPs inside the cells. Flow cytometry data also demonstrates that both ZnO and TiO2 NPs were significantly internalized in the S. typhimurium cells in a concentration dependent manner. A significant increase in uptake was observed in the S. typhimurium treated even with 8 and 80 ng mL−1 of ZnO and TiO2 NPs with S9 after 60 min, possibly the formation of micelles or protein coat facilitated entry of NPs. These NPs exhibited weak mutagenic potential in S. typhimurium strains TA98, TA1537 and Escherichia coli (WP2uvrA) of Ames test underscoring the possible carcinogenic potential similar to certain mutagenic chemicals. Our study reiterates the need for re-evaluating environmental toxicity of ZnO and TiO2 NPs presumably considered safe in environment.  相似文献   

10.
A multiplex surface plasmon resonance (SPR) biosensor method for the detection of paralytic shellfish poisoning (PSP) toxins, okadaic acid (and analogues) and domoic acid was developed. This method was compared to enzyme-linked immunosorbent assay (ELISA) methods. Seawater samples (n?=?256) from around Europe were collected by the consortia of an EU project MIcroarrays for the Detection of Toxic Algae (MIDTAL) and evaluated using each method. A simple sample preparation procedure was developed which involved lysing and releasing the toxins from the algal cells with glass beads followed by centrifugation and filtering the extract before testing for marine biotoxins by both multi-SPR and ELISA. Method detection limits based on IC20 values for PSP, okadaic acid and domoic acid toxins were 0.82, 0.36 and 1.66 ng/ml, respectively, for the prototype multiplex SPR biosensor. Evaluation by SPR for seawater samples has shown that 47, 59 and 61 % of total seawater samples tested positive (result greater than the IC20) for PSP, okadaic acid (and analogues) and domoic acid toxins, respectively. Toxic samples were received mainly from Spain and Ireland. This work has demonstrated the potential of multiplex analysis for marine biotoxins in algal and seawater samples with results available for 24 samples within a 7 h period for three groups of key marine biotoxins. Multiplex immunological methods could therefore be used as early warning monitoring tools for a variety of marine biotoxins in seawater samples.  相似文献   

11.
Christen V  Fent K 《Chemosphere》2012,87(4):423-434
Engineered silica nanoparticles (SiO2-NPs) find widespread application and may lead to exposure of humans and the environment. Here we compare the effects of SiO2-NPs and SiO2-NPs doped with silver (SiO2-Ag-NPs) on survival and cellular function of human liver cells (Huh7) and Pimephales promelas (fathead minnow) fibroblast cells (FMH). In Huh7 cells we investigate effects on the endoplasmatic reticulum (ER), including ER stress, and interactions of nanoparticles (NPs) with metabolizing enzymes and efflux transporters. The NPs formed agglomerates/aggregates in cell culture media as revealed by SEM and TEM. SiO2 and SiO2-1% Ag-NPs were taken up into cells as demonstrated by agglomerates occurring in vesicular-like structures or freely dispersed in the cytosol. Cytotoxicity was more pronounced in Huh7 than in FMH cells, and increased with silver content in silver-doped NPs. Dissolved silver was the most significant factor for cytotoxicity. At toxic and non-cytotoxic concentrations SiO2-NPs and SiO2-1% Ag-NPs induced perturbations in the function of ER. In Huh7 cells NPs induced the unfolded protein response (UPR), or ER stress response, as demonstrated in induced expression of BiP and splicing of XBP1 mRNA, two selective markers of ER stress. Additionally, SiO2-1% Ag-NPs and AgNO3 induced reactive oxygen species. Pre-treatment of Huh7 cells with SiO2-1% Ag-NPs followed by exposure to the inducer benzo(a)pyrene caused a significant reduced induction of CYP1A activity. NPs did not alter the activity of ABC transporters. These data demonstrate for the first time that SiO2-NPs and SiO2-1% Ag-NPs result in perturbations of the ER leading to the ER stress response. This represents a novel and significant cellular signalling pathway contributing to the cytotoxicity of NPs.  相似文献   

12.
Yi AX  Leung KM  Lam MH  Lee JS  Giesy JP 《Chemosphere》2012,89(9):1015-1025
The state of scientific knowledge regarding analytical methods, environmental fate, ecotoxicity and ecological risk of triphenyltin (TPT) compounds in marine ecosystems as well as their exposure and health hazard to humans was reviewed. Since the 1960s, TPT compounds have been commonly applied as biocides for diverse industrial and agricultural purposes. For instance, they are used as active ingredients in antifouling systems on marine vessels and mariculture facilities, and as fungicides in agriculture. Due to their intensive use, contamination of coastal waters by TPT and its products of transformation has become a worldwide problem. The proportion of quantified TPT to total phenyltin compounds in the marine environment provides evidence that TPT is photodegradable in water and sediment but resistant to biotransformation. Concentrations of TPT in marine biota are consistently greater than concentrations in water and sediment, which implies potential of TPT to bioaccumulate. TPT is toxic to both marine plants and animals. The predicted no effect concentration (PNEC) for TPT, as determined by use of the species sensitivity distribution approach, is 0.64 ng L−1. In some parts of the world, concentrations of TPT in seawater exceed the PNEC, indicating that TPT can pose risks to marine life. Although there is negligible risk of TPT to average human consumers, TPT has been detected in blood of Finnish people and the concentration was greater in fishermen who ate more seafood. It is, therefore, advocated to initiate regular monitoring of TPT in blood and breast milk of populations that consume greater amounts of seafood.  相似文献   

13.
Although silver nanoparticles (NPs) are increasingly used in various consumer products and produced in industrial scale, information on harmful effects of nanosilver to environmentally relevant organisms is still scarce. This paper studies the adverse effects of silver NPs to two aquatic crustaceans, Daphnia magna and Thamnocephalus platyurus. For that, silver NPs were synthesized where Ag is covalently attached to poly(vinylpyrrolidone) (PVP). In parallel, the toxicity of collargol (protein-coated nanosilver) and AgNO3 was analyzed. Both types of silver NPs were highly toxic to both crustaceans: the EC50 values in artificial freshwater were 15–17 ppb for D. magna and 20–27 ppb for T. platyurus. The natural water (five different waters with dissolved organic carbon from 5 to 35 mg C/L were studied) mitigated the toxic effect of studied silver compounds up to 8-fold compared with artificial freshwater. The toxicity of silver NPs in all test media was up to 10-fold lower than that of soluble silver salt, AgNO3. The pattern of the toxic response of both crustacean species to the silver compounds was almost similar in artificial freshwater and in natural waters. The chronic 21-day toxicity of silver NPs to D. magna in natural water was at the part-per-billion level, and adult mortality was more sensitive toxicity test endpoint than the reproduction (the number of offspring per adult).  相似文献   

14.
Hu J  Wang D  Wang J  Wang J 《Chemosphere》2012,89(5):536-541
Although engineered nanoparticles (NPs) could negatively impact environmental organisms, the synergistic effect of NPs and other toxic substances, which could be more significant than that of NP alone, have seldom been examined. The effect of two common NPs, nano-CeO2 and nano-TiO2, on the toxicity of Pb was evaluated using Ceriodaphnia dubia (C. dubia) as the model organism. Standard EPA procedures were followed in the toxicity evaluation. The toxicity of bare NPs (without Pb) was first evaluated and safe doses (levels without causing lethal effect) of NPs were used in the synergistic studies. It was found that the overall toxicity of Pb in the system containing NPs was greater than that of Pb alone, as indicted by the reduced median lethal concentration (LC50) of soluble Pb. The sorption of Pb onto the NP, and the uptake of NPs in the gastrointestinal tract of C. dubia were validated. Therefore, the uptake of Pb-loaded NPs increased the exposure of C. dubia to Pb, resulting in the enhanced toxicity. Reducing the solution pH could shift Pb speciation and enhance the overall toxicity of Pb, with or without the presence of NPs.  相似文献   

15.
Concentrations of neutral poly- and perfluoroalkyl substances (PFASs), such as fluorotelomer alcohols (FTOHs), perfluoroalkane sulfonamides (FASAs), perfluoroalkane sufonamidoethanols (FASEs), and fluorotelomer acrylates (FTACs), have been simultaneously determined in surface seawater and the atmosphere of the North Sea. Seawater and air samples were taken aboard the German research vessel Heincke on the cruise 303 from 15 to 24 May 2009. The concentrations of FTOHs, FASAs, FASEs, and FTACs in the dissolved phase were 2.6–74, <0.1–19, <0.1–63, and <1.0–9.0 pg L?1, respectively. The highest concentrations were determined in the estuary of the Weser and Elbe rivers and a decreasing concentration profile appeared with increasing distance from the coast toward the central part of the North Sea. Gaseous FTOHs, FASAs, FASEs, and FTACs were in the range of 36–126, 3.1–26, 3.7–19, and 0.8–5.6 pg m?3, which were consistent with the concentrations determined in 2007 in the North Sea, and approximately five times lower than those reported for an urban area of Northern Germany. These results suggested continuous continental emissions of neutral PFASs followed by transport toward the marine environment. Air–seawater gas exchanges of neutral PFASs were estimated using fugacity ratios and the two-film resistance model based upon paired air–seawater concentrations and estimated Henry's law constant values. Volatilization dominated for all neutral PFASs in the North Sea. The air–seawater gas exchange fluxes were in the range of 2.5?×?103–3.6?×?105 pg m?2 for FTOHs, 1.8?×?102–1.0?×?105 pg m?2 for FASAs, 1.1?×?102–3.0?×?105 pg m?2 for FASEs and 6.3?×?102–2.0?×?104 pg m?2 for FTACs, respectively. These results suggest that the air–seawater gas exchange is an important process that intervenes in the transport and fate for neutral PFASs in the marine environment.  相似文献   

16.
A large number of bacteria, including agents responsible for diseases, characterise sewage-polluted seawaters. Apart from standards for bathing waters and bivalve aquaculture waters, there are no general microbiological standards applicable to seawaters to help decide if bacterial pollution is within acceptable ranges. This study represents an attempt towards the issue of comparing the susceptibility of different marine invertebrates subjected to polluted seawater with a high microbial contamination. We explored the survival rates and the microbiological accumulation of mollusc bivalves, echinoderms and crustaceans species exposed to sewage-polluted seawaters. Microbiological analyses were performed on the polluted seawater and on the homogenates of exposed and unexposed specimens. Culturable bacteria (22 °C and 37 °C) and microbial pollution indicators (total coliforms, Escherichia coli and intestinal enterococci) were measured. When exposed to the sewage-polluted seawater, the examined invertebrates showed different survival rates. In the filter feeders, bacterial densities at 22 °C and 37 °C rose after 96 h of exposure to sewage. The highest concentrations of total coliforms and intestinal enterococci were found in exposed bivalve Mytilus galloprovincialis. The concentrations of bacteria growing at 37 °C were lower in the exposed deposit feeders compared to the polluted seawater. Some yeasts were absent in several exposed species although these yeasts were present in the polluted seawater. Our data suggest that the examined filter feeders, given their capability to survive and accumulate bacteria, may counteract the effects of sewage and restore seawater quality.  相似文献   

17.
Little research has been conducted on the occurrence of pharmaceuticals and personal care products (PPCPs) in the marine environment despite being increasingly impacted by these contaminants. This article reviews data on the occurrence of PPCPs in seawater, sediment, and organisms in the marine environment. Data pertaining to 196 pharmaceuticals and 37 personal care products reported from more than 50 marine sites are analyzed while taking sampling strategies and analytical methods into account. Particular attention is focused on the most frequently detected substances at highest concentrations. A snapshot of the most impacted marine sites is provided by comparing the highest concentrations reported for quantified substances. The present review reveals that: (i) PPCPs are widespread in seawater, particularly at sites impacted by anthropogenic activities, and (ii) the most frequently investigated and detected molecules in seawater and sediments are antibiotics, such as erythromycin. Moreover, this review points out other PPCPs of concern, such as ultraviolet filters, and underlines the scarcity of data on those substances despite recent evidence on their occurrence in marine organisms. The exposure of marine organisms in regard to these insufficient data is discussed.  相似文献   

18.
In November 2002 the oil tanker ‘Prestige’ released 65 000 tons of a heavy fuel oil throughout the Galician coastline (NW Spain), causing extensive damage to marine life, natural resources and economic activities at Northern Portugal, Spain and SW France. To evaluate the impact of the oil spill on the aquatic system, 30 polycyclic aromatic hydrocarbons (PAHs), including alkylated derivatives, were analyzed in seawater on five different sampling campaigns from 2002 to 2004. Sampling was made along the Galician continental shelf. In each station three samples were collected at three different depths (surface, mid-depth and bottom). Four different approaches for 3-way analyses (Catenated-PCA, Matrix-Augmented Principal Components Analysis, Parallel Factor Analysis and Procrustes rotation) have been used to asses the major sources of PAHs into the seawater. They revealed two main pollution patterns: one related to oil spillages and discharge of petroleum products, and another more associated with a diffuse anthropogenic origin.  相似文献   

19.
The growing application of engineered nanomaterials is leading to an increased occurrence of nanoparticles (NPs) in the environment. Thus, there is a need to better understand their potential impact on the environment. This study evaluated the toxicity of nanosized TiO2, ZrO2, Fe0, Fe2O3, and Mn2O3 towards the yeast Saccharomyces cerevisiae based on O2 consumption and cell membrane integrity. In addition, the state of dispersion of the nanoparticles in the bioassay medium was characterized.  相似文献   

20.
Huang XL  Zhang JZ 《Chemosphere》2011,85(8):1227-1232
Organophosphonate, characterized by the presence of a stable, covalent, carbon to phosphorus (C-P) bond, is a group of synthetic or biogenic organophosphorus compounds. The fate of these organic phosphorus compounds in the environment is not well studied. This study presents the first investigation on the sorption of phosphorus (P) in the presence of two model phosphonate compounds, 2-aminothylphosphonoic acid (2-AEP) and phosphonoformic acid (PFA), on marine carbonate sediments. In contrast to other organic P compounds, no significant inorganic phosphate exchange was observed in seawater. P was found to adsorb on the sediment only in the presence of PFA, not 2-AEP. This indicated that sorption of P from phosphonate on marine sediment was compound specific. Compared with inorganic phosphate sorption on the same sediments, P sorption from organic phosphorus is much less in the marine environment. Further study is needed to understand the potential role of the organophosphonate compounds in biogeochemical cycle of phosphorus in the environment.  相似文献   

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