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Abstract

Abstract With the large amount of attention being given to microplastics in the environment, several researchers have begun to consider the fragmentation of plastics down to lower scales (i.e., the sub-micrometer scale). The term “nanoplastics” is still under debate, and different studies have set the upper size limit at either 1000 nm or 100 nm. The aim of the present work is to propose a definition of nanoplastics, based on our recently published and unpublished research definition of nanoplastics. We define nanoplastics as particles unintentionally produced (i.e. from the degradation and the manufacturing of the plastic objects) and presenting a colloidal behavior, within the size range from 1 to 1000 nm.

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... Their chemical and physical properties make them ideally suited for many different applications including, but not limited to, medical supplies, food packaging, clothing and construction materials (Worm et al. 2017;Huang et al. 2021). Plastics are made in different sizes and eventually will breakdown and enter the microscale (1 μm-5 mm, in principle, but studies tend to examine the larger fractions) and nanoscale 1-100 or 1-1000 nm (Gigault et al. 2018;Gonçalves and Bebianno 2021). These small plastic materials enter the environment; it has been reported that wastewater treatment plants are one of the main pathways of microplastic pollution, and treated wastewater is an important source of nanoplastic discharge to freshwater sources (Carr et al. 2016;Murray and Örmeci 2020). ...
... Once in the environment, plastics continue to break down into smaller nano-sizes (Gigault et al. 2018;Gonçalves and Bebianno 2021). Nanoplastics pose a risk to human health and the environment because they are persistent, easily ingested by microorganisms, can move to higher trophic levels and act as carriers for harmful chemicals (Hartmann et al. 2017;Cassano et al. 2023). ...
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Environmental context Plastic pollution is widespread and continues to be a major concern, both for the environment and human health. Identifying nanoplastics is challenging but is important to understand how they behave once in the environment. It is shown that a combination of single particle (SP) and single cell (SC) inductively coupled plasma mass spectrometry (ICP-MS) can be used to quantify nanoplastics on a per cell basis after exposure to algal cells. Abstract The effects of plastic pollution on human health and the environment are not well known but there are significant concerns. Although research has increased in recent years, there remain many obstacles to the quantification of nanoplastics. This rapid communication demonstrates that combined single particle (SP)– and single cell (SC)–inductively coupled plasma–mass spectrometry (ICP-MS) provide a novel means to quantify pre-formed core–shell metal–plastic composite nanoparticles when exposed to two freshwater algal cells, Cryptomonas ovata (C. ovata) and Cryptomonas ozolini (C. ozolini). It is shown that individual palladium plastic nanoparticles (Pd NPPs) exposed to algal cells form agglomerates in the cell suspension respectively consisting of 165 and 157 (±3.8) individual Pd NPPs for C. ozolini and C. ovata cells, and that the agglomerates are also cell-associated with 1.75–1.85 agglomerates per cell.
... It may reach 33 billion tons by 2050 (Rochman et al., 2013). Larger plastics, under a variety of environmental forces, including UV radiation, wind action, wave action and microbial activity, are broken down into smaller particles such as microplastics (MPs) (< 5 mm) (NOAA, 2008) and nanoplastics (NPs) of particle size < 100 nm (Galloway et al., 2017) or < 1 μm (Gigault et al., 2018). MPs and NPs have been detected in territorial water (Güven et al., 2017), rivers Sarkar et al., 2019), tidal creeks (Robin et al., 2020), seawaters (Sunitha et al., 2021), coastal areas (Karthik et al., 2018), snow (Aves et al., 2022) and even in clouds (Xu et al., 2023). ...
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The acute toxicity of graded concentrations of polysterene nanoplastic (PS NPs) spheres (Size 0.1 µm) was evaluated to ascertain the effects of NPs on growth, vital photosynthetic pigments, protein and oxidative stress enzymes. The findings show that PS NPs inhibited the growth of microalgae (Chlorella vulgaris and Spirulina (Arthrospira) platensis) in a dose-dependent manner. The growth inhibition percentage reached 40.12% for C. vulgaris and 42.57% for S. platensis, compared to the control. Additionally, pigment content decreased by 31.62% to 35.06%, while protein content dropped by 37.27% to 48.48% of both the tested microalgae as the concentration of PS NPs in the medium increased. The oxidative stress created by PS NPs was evident from an increase in catalase and peroxidase activity. The findings conclusively endorse that NPs pollution in the aquatic environment will disrupt the functioning of ecosystems through its detrimental effects on microalgae forming the base of the food chain and supporting the successive trophic levels in the aquatic environment. This research will give a deeper insight into the ecotoxicological impacts of NPs in aquatic environments and the baseline information will be helpful in developing an effective strategy for mitigation of plastic pollution with a greater emphasis on nanoplastics.
... PLA waste in the environment may undergo various degradation pathways such as photo and thermal-oxidation, hydrolysis, mechanical fragmentation, etc. 2, 11, 12 to form microplastics (MPs) and nanoplastics (NPs). NPs are plastic fragments of size <1000 nm 13 , with altered chemical and structural properties compared to their bulk, and are considered contaminants of emerging concern 13, 14 . As PLA utilization increases, it is important to expand our knowledge of the formation pathways of PLA NPs, their presence in the environment, and their environmental fate. ...
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Due to the well-documented negative environmental impacts of conventional plastics, the use of bioplastics has been increasing. Poly(lactic acid) (PLA) is currently among the most common and industrially available bioplastics. Although PLA is compostable under industrial conditions and generally degrades more quickly than conventional plastics, its breakdown in typical environmental settings remains problematic. PLA’s potential to contribute to plastic pollution through the release of microplastics and nanoplastics makes it crucial to understand how these particles behave, especially in marine environments. However, as for all nanoplastics, identifying, isolating, and quantifying PLA nanoplastics in water presents significant challenges. This study proposes a versatile approach to fabricate PLA nanoplastics through laser ablation in a water environment to mimic realworld samples. Commencing with bulk PLA films, this top-down method yields the formation of nanoplastics with an average diameter of 54.7 ± 26.7 nm. Surface and chemical analyses confirm the presence of carboxylic groups on their surface, potentially resembling the environmental degradation pathway of PLA under exposure to sunlight and humid environments. This indicates that the proposed process results in a PLA nanoplastics system that serves as an invaluable reference model, enabling realistic environmental scenario explorations and simulations for risk assessment evaluations on bio-based nanoplastics.
... "Nanoplastic" refers to the smallest-sized fraction of plastic particles, of (arguably) less than 100 nm in size [1][2][3]. Although nanoplastics (NPLs) can be intentionally manufactured for specific purposes (primarily as water-based dispersions, etc.), those found in the environment are mostly associated with the degradation of larger plastic items (secondary NPLs), which result from the combined action of environmental factors, such as sunlight, heat, and mechanical stress [4,5], and biotic factors, such as the formation of the plastisphere (i.e., the microbiota that take advantage of floating plastic debris and settle there [6]). ...
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To date, the assessment of risks related to nanoplastics (NPLs) has been incipient. Attempts to establish safety levels to support decisions regarding restrictions on the use or reuse of materials derived from petrochemicals are critical, but the complexity of datasets makes it difficult to communicate potential NPLs-related environmental risks. Therefore, it seems essential to reduce the relevant data to a factor/number that makes it easier to clarify whether there is a risk and, above all, easily report relevant information to legislators so that prohibition, reductions, and/or readjustments to monitoring programs can be implemented accordingly. Accordingly, this study aimed to propose an improved and tiered risk assessment for NPLs following the NORMAN network, which may be outlined as follows: (i) conducting screenings to assess the risk level through deterministic methodologies (involving the collection of effective concentrations or, in their absence, the no-effect or lowest-effect concentrations, also known as NOEC and LOEC, respectively); (ii) comparing exceedance levels of risk values obtained previously in relation to predicted non-environmental effective concentrations (PNECs); and (iii) ranking the different NPL types based on prioritization indeces to facilitate future decision-making. Of a total of six polymers for which data are available, it was only possible to deliver prioritization indices for three (two freshwater and one saltwater) due to the lack of PNEC or predicted environmental concentrations (PECs). The majority of the research on this topic is focused on PS. PS is classified as a high-priority polymer, since its estimated prioritization index was ≥65 (the base value is 1). Furthermore, in freshwater, PE was also indicated to be a priority polymer (with a prioritization index exceeding 1000). It should be noted that for other widely used polymers (such as PMMA or PVC), there is insufficient data. It is therefore clear that current management and control measures for products containing PS and PE must be reconsidered to reduce NPLs’ environmental impacts.
... MPs should not be more than 5 mm in size, according to Arthur et al. [26]. NPs are plastic particles and fibers smaller than 1 μm, whereas MPs are those between 1 μm and 1 mm in size [27][28][29][30]. MPs that are 1 to 5 mm in size are considered as large [28,29]. ...
Article
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Micro- and nano-plastics (MPs and NPs) are generated from the breakdown of larger plastic materials or through direct release. Their extensive distribution and persistence have made them a significant global environmental issue. Plastic particles of smaller size, measuring from several μm to nm, affect diverse ecosystems, that includes terrestrial, freshwater and marine environments. Their presence possesses significant consequences for biodiversity, ecosystem balance and human well-being. This review presents a brief examination of the pathways, fate and impacts of MPs and NPs in the environment, as well as their incorporation into the food chain. MPs and NPs serve as the carriers for toxic chemicals and pathogens, thereby enhancing their potential risks. Consumption of these substances by various organisms, including plankton and humans, results in bioaccumulation and biomagnification, which increases significant issues regarding food safety and security. The long-term effects of MPs and NPs on the environment and human health are not yet fully understood, indicating a need for further investigation. This review summarizes the existing knowledge and highlights the critical necessity for interdisciplinary research and global collaboration to address the environmental and food chain risks associated with MPs and NPs, thereby promoting the long-term sustainability of ecological systems and human health.
... The particles can adsorb toxic substances such as pesticides and heavy metals and act as carriers of pathogens [16]. When ingested by humans, microplastics can cause inflammation, disrupt the endocrine system, and provoke oxidative stress [18]. Nanoplastics pose a particular threat, as their small size enables them to penetrate cell membranes and the blood-brain barrier. ...
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This study analyzes microplastic pollution of surface waters of the Zarafshan River flowing through the Samarkand and Navoi regions of Uzbekistan. Microplastics pose a serious threat to aquatic ecosystems due to their ubiquity and ability to accumulate toxic substances. In the Central Asian context, the problem of microplastics remains poorly understood, complicating the development of mitigation strategies. The study was conducted in July 2023. Surface water samples were collected using a microsampler equipped with a 330 μm mesh. Laboratory processing included oxidation of organic matter with hydrogen peroxide and separation of plastic particles by density separation. Raman spectroscopy was used to identify the polymer composition. According to the results, the concentration of MP particles was 3.22±1.64 units∕m3 in the corresponding part of the Zarafshan River in the Navoi region and 2.96±0.78 units∕m3 in the Samarkand region. The particles found in the water have a diameter of 0.15 to 3.00 mm. According to the results of the data analysis, a part of the Zarafshan River flowing through the territory of Samarkand and Navoi regions is polluted with plastic particles due to environmental factors. Existing data on microplastic pollution of freshwater ecosystems in Central Asia are fragmentary, which makes it difficult to assess environmental risks and take appropriate measures. The aim of this paper is to assess the level of microplastic pollution in the Zarafshan River and identify the main sources of pollution. The results of the study highlight the need for regular monitoring and the development of effective measures to reduce the level of microplastic pollution in the region.
... Plastic debris can be found in the ocean in different shapes and sizes. Once the macroplastics (≥5 mm) are disposed of in the natural environment, these debris are exposed to mechanical, chemical, biological, and environmental conditions, leading to their breakdown into microplastics (<5 mm) and nanoplastics (<0.1 µm) (Gigault et al., 2018;Song et al., 2017;da Costa, 2018). Previous studies have been mostly focused on plastic debris impacts and threats to the environment (Borrelle et al., 2020;Thushari and Senevirathna, 2020;Rhodes, 2018;Lau et al., 2020;Millican and Agarwal, 2021;MacLeod et al., 2021). ...
Article
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The increasing volume of plastic waste and the widespread use of plastic products pose significant challenges to the effectiveness of strategies, policies, and management projects aimed at combating ocean plastic pollution. Three billion people's livelihoods depend on marine and coastal resources, and the market value of these resources and related blue industries is estimated at US$3 trillion annually, which is about 5% of global GDP. Plastics make up around 80% of the total waste discarded in the ocean, and each year, over 13 million metric tons of plastic enter the marine environment threatening biodiversity and affecting ecosystem services upon which the economy of coastal countries depends. This paper explores the impact of plastic waste on understudied marine and coastal ecosystem services, utilizing the Millennium Ecosystem Assessment framework as a guide. This study reveals that prioritizing the assessment and study of supporting services is critical for maintaining and sustaining other services. This review provides data on the impact of plastic on marine ecosystem services and highlights the need for effective plastic waste management to sustain these services. Coordinated global actions and initiatives among regions, nations, and industries remain crucial steps in addressing and tackling plastic pollution in the ocean.
... MPs are polymeric particles that range in size from 1 to 5 mm. NPs refer to plastic particles smaller than 1 µm (Gigault et al. 2018; Thompson et al. 2004). These MNPs (micro-nanoplastics) serve as conduits for carrying various environmental pollutants, including pesticides, pharmaceuticals, and other organic and inorganic pollutants. ...
Article
Microplastics and nanoplastics (MNPs) are byproducts of plastics created to benefit humanity, but improper disposal and inadequate recycling have turned them into a global menace that we can no longer conceal. As they interact with all living organisms, including humans, their mechanism of interaction and their perilous impact must be meticulously investigated. To uncover the secrets of MNPs, there must be model systems that exist to interlink the two major scenarios: they must represent the environmental impact and be relevant to humans. Therefore, zebrafish and Drosophila are perfect to describe these two cases, as they are well studied and relatable to humans. In this review, 39% zebrafish studies reported higher mortality and hatching rates at greater MNP concentrations, severe oxidative stress as seen by raised malondialdehyde (MDA) levels, and reduced superoxide dismutase (SOD) activity. About 50% of studies showed severe neurotoxic behavior with drop of locomotor activity, suggesting neurotoxicity. MNPs have a significant impact on fertility rate of Drosophila . More than half of the studies revealed genotoxicity in Drosophila as observed by wing spot assays and modified genomic expressions associated with stress and detoxification processes. These findings emphasize the potential of MNPs to bioaccumulate, impair physiological systems, and cause oxidative and neurobehavioral damage. This study underscores the importance for thorough risk evaluations of MNPs and their environmental and health consequences.
... It is known that these large particles will gradually fragment/degrade into smaller meso-, micro-, and nanoplastic particles (Andrady, 2011;Weber et al., 2022;Liro et al., 2023), which is through biochemical and physical forces, arising through interactions between environmental conditions and the inherent instability of plastic materials (Lenaker et al., 2019;Stubbins et al., 2021;Gan et al., 2023). While there is still an ongoing debate on the size definitions of plastics (Hartmann et al., 2019), commonly accepted size limits are 5 < < 20 mm for mesoplastics, < 5 mm for microplastics, and < 1 μm for nanoplastics (Gigault et al., 2018;Liro et al., 2023). ...
... Microplastics are defined as solid plastic particles smaller than 5 mm in size; 7 crumb rubber infill pieces are typically less than 1 mm in diameter, and a study found that 50% of artificial turf fibres sampled were less than 5 mm in size, classifying both as a sources of microplastics. 8 Nanoplastics, defined as plastic particles in size ranging between 1 to 1000 nm, 9 have also been detected in drainage water from artificial turf pitches. 10 As part of wider bans on microplastics, the EU have placed a ban on the sale of granular synthetic polymer infill for use on synthetic sports surfaces, in effect from the 17th October 2031. ...
Article
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The growing use of artificial turf in place of natural turf in residential, recreational and commercial settings has raised concerns regarding its potential impact on human health. A systematic review of databases revealed 5673 articles of which, 30 were deemed eligible. Those performing total concentration analyses, bioaccessibility analyses or human health risk assessments (HHRAs) of artificial turf fibres or crumb rubber infill were of interest. Health hazards and risks were explored in relation to three groups of chemicals of concern: polycyclic aromatic hydrocarbons (PAH), heavy metals and other rubber additives. Twenty-five studies performed total concentration analyses on samples of artificial turf infill and/or turf fibres. Of these studies, median reported concentrations of eight PAHs, cadmium, mercury and zinc exceeded the European limits used. Eight studies performed bioaccessibility assays using synthetic biofluids and simulated organ systems. PAHs were not found to be bioaccessible except for benzo[a]pyrene in gastric fluid; heavy metals were bioaccessible except arsenic, and rubber additives were mostly bioaccessible except for three plasticisers: diisobutyl phthalate, benzyl butyl phthalate and dibutyl phthalate. Fourteen studies performed HHRAs to determine non-carcinogenic and carcinogenic risk. Cancer risks were identified for ingestion exposure to PAH in children with pica and heavy metal exposure via dermal, inhalation and ingestion pathways. Non-carcinogenic risks were identified for the ingestion of cobalt in a child spectator and the ingestion of arsenic, cobalt, thallium and zinc. Potentially hazardous concentrations of chemicals were found across both artificial turf infill and artificial turf fibre samples; bioaccessibility of these chemicals varied. Definitive conclusions were unable to be derived on the human health risks posed to users of artificial turf under real-world exposure scenarios. Future studies are recommended to explore the risks associated with the potential synergistic toxicities of chemical mixtures found in artificial turf.
... Both abiotic and biotic processes, such as bacteria, sunlight, heat, and abrasion, can break plastic litter down at the millimeter, micrometer, or nanometer scale (Chamas et al., 2020). These small plastic particles are known as microplastics (MPs, < 5 mm) or nanoplastics (NPs, <1 μm) (Gigault et al., 2018) and can make up a substantial portion of the plastic pollution problem. For example, microplastics between 0.33 and 5 mm account for about 90 % of the identified plastic particles found in ocean environments (Eriksen et al., 2014). ...
Article
Plastic pollution is a growing environmental concern due to its ubiquitous impact on aquatic ecosystems. Nanoplastics can be generated from the breakdown of plastic waste and interact with organisms at the cellular level, potentially disrupting cellular physiology. We investigated the effects of 44 nm polystyrene nanoparticles (44 nm NanoPS) on the development and physiology of zebrafish (Danio rerio) in the presence of sublethal heat stress (32 °C vs control, 28 °C). We hypothesized that the simultaneous exposure to nanoplastics and rising temperatures seriously threaten developing fish. This combination could create a critical imbalance: rising temperatures may lead to heightened energy demands, while nanoplastic exposure reduces energy production, threatening animal survival. As expected, 32 °C increased markers associated with animal metabolism and developmental timing, such as growth, hatching, heart rate, and feeding. Changes in apoptosis dynamics, oxygen consumption rates, and a decrease in mitochondrial content were detected as adaptive processes to temperature. 44 nm NanoPS alone did not alter development but decreased mitochondrial efficiency in ATP production and increased apoptosis in the heart. Surprisingly, exposure to 44 nm NanoPS at 32 °C did not cause major implications to survival, developmental success, or morphology. Still, 44 nm NanoPS mitigated the temperature-driven change in heart rate, increased oxidative stress, and decreased the coupling efficiency of the less abundant and highly active mitochondria under heat stress. We highlight the interplay between temperature and nanoplastics exposure and suggest that the combined impact of nanoplastics and temperature stress results in a scenario where physiological adaptations are strained, potentially leading to compromised development. This research underscores the need for further investigation into the metabolic costs of plastic pollution, particularly in the context of global warming, to better understand its long-term implications for aquatic life.
... This has led to concern not only for the natural environment, but also for the potential effects of plastic on human health (Vandenberg et al., 2007;Halden, 2010;Barbir et al., 2021). Plastics in the marine environment may fragment to micro (<5 mm) and even nano-sized particles (1-1000 nm) (Gigault et al., 2018), are rapidly colonized by microorganisms within hours (Latva et al., 2022), and sorb pollutants (Mato et al., 2001;Capriotti et al., 2021). Plastic quickly forms a scaffold for a new ecological niche called the plastisphere (Zettler et al., 2013). ...
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Plastics are a ubiquitous pollutant, and are rapidly colonized by biofilms that sorb inorganic and organic components, forming the interface between plastics and the environment. This study provides a proof of concept for the use of automated quantitative mineralogy (AQM) to illuminate and analyse the metal and mineral component of the plastisphere on plastics sampled from temperate and tropical aquatic localities. The method is non-destructive and requires minimal sample preparation, providing a 2-dimensional visualisation and semi-quantitative analysis of the arrangement of biogenic and abiogenic components, highlighting potential interactions between these components. Our results also communicate the potential role of plastic structure on mineral retention in relation to environmental parameters that can influence mechanical degradation. AQM provides a novel avenue to understand the minerals associated with plastics, and increases our knowledge of the interfacial composition, which can inform potential interactions, transformations and insights into the long-term fate of plastic pollutants.
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Microplastic (MPs) pollution has engulfed global aquatic systems, and the concerns about MPs translocation and bioaccumulation in fish, crabs, and other marine organisms are now an unpleasant truth. In the past few years, MPs pollution in freshwater systems, particularly rivers, and subsequently in freshwater organisms, especially in crabs, has caught the attention of researchers. Rivers provide livelihood to approximately 40% of the global population through food and potable water. Hence, assessment of emerging contaminants like MPs in waterways and the associated fauna is crucial. This study assessed MPs in crab S. serrata across the largest riverine system of south India, the Kaveri River. The MPs were characterized by optical microscopy, and field emission scanning electron microscopy‐energy dispersive X‐ray (FESEM–EDX) analysis for their number, shape, size, and color. Polymer composition was analyzed using attenuated total reflectance Fourier‐transform infrared spectroscopy (ATR‐FTIR) and Raman spectroscopy. Polypropylene (PP), polystyrene (PS), polyamide (PA), and polyvinyl chloride (PVC) were the dominant plastic polymers in the crab intestine. Additionally, the FE‐SEM analysis revealed that the MPs have differential surface morphology with rough surfaces, porous structures, fissures, and severe damage. Most MPs comprised Na, Si, Mg, Cl, K, and Ca, according to EDX analyses. The findings might provide insight into the status of MPs in S. serrata at Kavery river that could help in formulating regulations for MPs reduction and contamination in rivers eventually to protect the environment and human health. Practitioner Points The first findings on the identity and properties of MPs in crabs from the Kaveri River at Mettur Dam. A simple and cost‐effective approach for extracting microplastics from crab samples from Mettur Dam, Kaveri River, Salem District, Tamil Nadu, India. Microplastics were detected using optical microscopy, ATR‐FTIR, and FE‐SEM.
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Microplastics have received increased attention due to their negative impacts on the environment and human health. To minimize these impacts, mitigation strategies that are efficient and cost‐effective for a range of plausible conditions need to be developed. Models can be used to support these mitigation‐related decisions. However, modeling studies related to the export of microplastics from terrestrial to aquatic systems have been limited. Here, we review such modeling studies, the trends over time and geography of focus, and discuss pertinent concepts and the underlying physical, chemical, and biological processes. We categorize the published modeling studies, discuss their limitations, and provide recommendations for future research to fill key knowledge gaps. Future modeling efforts should focus on collecting more comprehensive field data for validation, developing continuous models over event‐based, conducting experimental studies to better understand the fundamental processes, developing hybrid modeling frameworks, adopting sediment transport modeling approaches, incorporating land management practices in the models, integrating surface and sub‐surface processes at the watershed scale, and utilizing advanced data‐driven models like foundation models.
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Plastic pollution has emerged as one of our most pervasive and pressing environmental issues, impacting ecosystems, wildlife, and even human health globally. Microplastic research has primarily focused on oceans, whether in water, sediments, or organisms, generating a significant gap in understanding their presence and impact on other environments like rivers, which is a concern worldwide, and of paramount importance for us in Latin America and the Caribbean. To address this situation, we examined the current research on microplastics in South American rivers by conducting a Google Scholar search with keywords and Boolean operators, which allowed us to recover a series of articles related to this topic. We reviewed 49 articles published in 2023 to know methods for collecting and analyzing river samples. Our findings revealed limited information on microplastics in South America, with data only from Argentina, Brazil, Colombia, Ecuador, Paraguay, and Peru. Additionally, we found considerable variations in sample collection and analysis methods, hindering study comparisons. Bridging this knowledge gap is crucial for comprehending the extent of plastic pollution in the region. Since rivers are major microplastic contributors to oceans, this research will significantly aid in environmental protection efforts, emphasizing the global relevance of addressing riverine plastic pollution.
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Nano-plastics (NPs) and heavy metals have attracted growing scientific attention because of both pollutants’ wide distribution and ecotoxicity. However, the long-term combined toxicity of NPs and mercury (Hg) on planktonic copepods, a crucial presence in marine environments, is unknown. Here, our study aimed to investigate the multigenerational phenotypic responses of the planktonic copepod Pseudodiaptomus annandalei to polystyrene NPs (about 50 nm) and Hg (alone or combined) at environmentally realistic concentrations (23 μg/L for NPs and 1 μg/L for Hg), and the underlying molecular mechanisms were explored. Despite the insignificant effect on survival, NPs could threaten the development and reproduction of P. annandalei, being ascribed to down-regulated genes in ingestive and reproductive functions. Hg exposure revealed inhibition of reproduction probably as an energy trade-off strategy. Importantly, in combined NPs and Hg, development and reproduction were further negatively impacted, even relative to NPs or Hg alone. Correspondingly, combined NPs and Hg presented the most pronounced transcriptomic response with a series of changes in cell functions and down-regulation of key genes in the DNA replication pathway and reproductive function as compared to NPs or Hg alone. The findings indicated adverse combined effects of NPs and Hg on P. annandalei under multigenerational scenarios, being a greater ecological risk for planktonic copepod than NPs or Hg alone. This study provides molecular insights into the long-term toxicity of combined NPs and Hg to planktonic copepods, underlining the increased risk in the population sustainability of marine zooplankton facing co-existing plastics and Hg pollution.
Preprint
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Plastic pollution is ubiquitous, and animals are exposed to diverse plastic shapes and sizes. When plastics enter natural environments, they break down into microplastics (MPs; <5 mm) and likely become more accessible to smaller animals. Insects play critical environmental and economic roles, ingest plastics in the wild, and can physically degrade ingested MPs into smaller and more harmful nanoplastics. While particle size and body size undoubtedly impact plastic ingestion, we have no predictive understanding of how these factors interact to influence which plastics are a threat to which animals. To uncover these potential interactions, we studied how a model cricket species (Gryllodes sigillatus) interacts with plastics of differing sizes throughout a twentyfold change in body size during growth and development. We fed crickets a range of MP sizes of 38 to 500 mμ with clearly defined particle size thresholds. We investigated whether crickets would avoid MPs when given a choice and found that they do not; instead they gradually began to consume more of the plastic diet over time. We then studied how MP ingestion is influenced by body size and mouth size, and the extent of breakdown that occurs once MPs are ingested. We found that crickets would only consume whole beads when their mouth size was larger than the MP. While small MPs were more likely to be excreted whole, larger MPs were more extensively broken down as crickets grew. We conclude that crickets do not exhibit avoidance behaviour towards plastic and ingest it once a particle can be consumed whole. These effects of insect behaviour and body size on the likelihood of plastic ingestion and the degree to which MPs are degraded have important implications for regulating the size classes of plastic particles entering natural environments and how plastics move through those environments once discarded.
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An analytical processing design is proposed to accumulate nano-plastics diluted in water-based solvents and evaluate their individual IR spectral properties.
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A collection of abstracts presented during the Third Workshop of SETAC ITALIAN LANGUAGE BRANCH, helded in Milan in 7-8 october 2024.
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Nanoplastics pose a growing threat to marine ecosystems, particularly affecting the early developmental stages of marine organisms. This study investigates the effects of amino-modified polystyrene nanoparticles (PS-NH2, 50 nm) on the embryonic development of Phallusia mammillata, a model ascidian species. Both chorionated and dechorionated embryos were exposed to increasing concentrations of PS-NH2 so morphological alterations could be assessed with a high-content analysis of the phenotypes and genotoxicity. PS-NH2 induced the same morphological alterations in both chorionated and dechorionated embryos, with dechorionated embryos being more sensitive (EC50 = 3.0 μg mL−1) than chorionated ones (EC50 = 6.26 μg mL−1). Interestingly, results from the morphological analysis showed two concentration-dependent mechanisms of action: (i) at concentrations near the EC50, neurodevelopmental abnormalities resembling the ones induced by exposure to known endocrine disruptors (EDs) were observed, and (ii) at higher concentrations (15 μg mL−1 and 7.5 μg mL−1 for chorionated and dechorionated embryos, respectively), a nonspecific toxicity was evident, likely due to general oxidative stress. The phenotypes resulting from the PS-NH2 treatment were not related to DNA damage, as revealed by a genotoxicity assay performed on neurula embryos. Our data suggest that PS-NH2-induced toxicity is primarily mediated through oxidative stress, probably triggered by interactions between the positive charges of the PS NPs and the negative charges on the cell membranes. The lack of a protective chorion further exacerbated these effects, highlighting its role in mitigating/protecting against NP-induced damage.
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Single nanoparticle analysis is crucial for various applications in biology, materials, and energy. However, precisely profiling and monitoring weakly scattering nanoparticles remains challenging. Here, it is demonstrated that deep learning‐empowered plasmonic microscopy (Deep‐SM) enables precise sizing and collision detection of functional chemical and biological nanoparticles. Image sequences are recorded by the state‐of‐the‐art plasmonic microscopy during single nanoparticle collision onto the sensor surface. Deep‐SM can enhance signal detection and suppresses noise by leveraging spatio‐temporal correlations of the unique signal and noise characteristics in plasmonic microscopy image sequences. Deep‐SM can provide significant scattering signal enhancement and noise reduction in dynamic imaging of biological nanoparticles as small as 10 nm, as well as the collision detection of metallic nanoparticle electrochemistry and quantum coupling with plasmonic microscopy. The high sensitivity and simplicity make this approach promising for routine use in nanoparticle analysis across diverse scientific fields.
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The paper relates to a systematic literature review about the citizen science experiences, to study odour emissions in the framework of the Directive 2010/75/EU.
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Microplastics (MPs) are ubiquitous in the marine environment and impact organisms at multiple levels. Understanding their actual effects on wild populations is urgently needed. This study develops a toolkit to monitor changes in gene expression induced by MPs in natural environments, focusing on filter-feeding and bioindicator species from diverse ecological and taxonomic groups. Six candidate genes —Caspase, HSP70, HSP90, PK, SOD, and VTG— and nine filter-feeding species —two branchiopods, one copepod, five bivalves and one fish— were selected based on differential expression in response to MPs exposure (mainly the widely used polystyrene and polyethylene polymers) reported in over 30 publications. Some genes are particularly determinant, such as HSP70 and HSP90 (key to managing a wide range of stressors) and SOD (critical for addressing oxidative stress), as they are more directly related to stress. PK is related to carbohydrate metabolism (alterations in energy metabolism); VTG is associated with reproductive problems; Caspase mediates in apoptosis. Each gene in the toolkit plays a role depending on the type of stress assessed, and their combination provides a comprehensive understanding of the impacts of MPs. Differences in gene expressions between species and the exposure thresholds were found. These genes were examined in various scenarios with different types, concentrations, and sizes of MPs, alone or with other stressors. The toolkit offers significant advantages, allowing a comprehensive study of the impact of MPs and focusing on filtering bioindicator species, thus enabling pollution assessment and long-term monitoring. It will outperform traditional methods like tissue counts of MPs where only physical damage is visible, providing a deeper understanding. To our knowledge, this is the first toolkit of its kind.
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Nanoplastics (NPs) and microplastics (MPs) are an emerging threat to global health. They negatively impact ecosystems and many physiological processes, causing alterations in xenobiotic metabolism, nutrient uptake, energy metabolism, or cytotoxicity. In humans, we are beginning to analyze these plastics for the mechanisms by which they enter the organism, accumulate, and diffuse as well as for their pathogenic potential. NP accumulation has been demonstrated in human tissues, such as blood or placenta, while in others it remains largely unstudied. In this work, we detected NP accumulation in bronchoalveolar lavage fluids (BALFs), cerebrospinal fluids (CSFs), lymph nodes (LNs), urine, pleural fluids (PFs), ascitic fluids (AFs), and peripheral blood (PB) by combining fluorescence and nanocytometry techniques. NP analysis was compared with two strains of mice, and the results support that inhalation is the main route of NP accumulation.
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This study investigated the direct and indirect toxic effects of microplastics and nanoplastics toward zebrafish (Danio rerio) larvae locomotor activity. Results showed that microplastics alone exhibited no significant effects except for the upregulated zfrho visual gene expression; whereas nanoplastics inhibited the larval locomotion by 22% during the last darkness period, and significantly reduced larvae body length by 6%, inhibited the acetylcholinesterase activity by 40%, and upregulated gfap, α1-tubulin, zfrho and zfblue gene expression significantly. When co-exposed with 2 μg/L 17 α-ethynylestradiol (EE2), microplastics led to alleviation on EE2's inhibition effect on locomotion, which was probably due to the decreased freely dissolved EE2 concentration. However, though nanoplastics showed stronger adsorption ability for EE2, the hypoactivity phenomenon still existed in the nanoplastics co-exposure group. Moreover, when co-exposed with a higher concentration of EE2 (20 μg/L), both plastics showed an enhanced effect on the hypoactivity. Principal component analysis was performed to reduce data dimensions and four principal components were reconstituted in terms of oxidative stress, body length, nervous and visual system related genes explaining 84% of total variance. Furthermore, oxidative damage and body length reduction were evaluated to be main reasons for the hypoactivity. Therefore, nanoplastics alone suppressed zebrafish larvae locomotor activity and both plastic particles can change the larvae swimming behavior when co-exposed with EE2. This study provides new insights into plastic particles' effects on zebrafish larvae, improving the understanding of their environmental risks to the aquatic environment.
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Microplastics (MPs) have been identified as contaminants of emerging concern in aquatic environments and research into their behavior and fate has been sharply increasing in recent years. Nevertheless, significant gaps remain in our understanding of several crucial aspects of MP exposure and risk assessment, including the quantification of emissions, dominant fate processes, types of analytical tools required for characterization and monitoring, and adequate laboratory protocols for analysis and hazard testing. This Feature aims at identifying transferrable knowledge and experience from engineered nanoparticle (ENP) exposure assessment. This is achieved by comparing ENP and MPs based on their similarities as particulate contaminants, while critically discussing specific differences. We also highlight the most pressing research priorities to support an efficient development of tools and methods for MPs environmental risk assessment.
Chapter
This chapter concerns the structure, chemical composition, properties and degradation of plastic materials in the environment. Detailed diagrams of the chemical structure of the most common plastics are provided as well as background information. Furthermore, many properties of plastics are discussed, such as the glass transition temperature, the limiting oxygen index and their resistance to ultraviolet light. Additionally, details of the minimum and maximum operating temperatures of the most common materials are indicated. In terms of degradation, the latest information regarding biotic degradation is discussed as well as the provision of a list of known plastic-degrading organisms. Furthermore, the various forms of abiotic degradative effects on plastic materials are covered in detail, as well as the effects of additives in modifying and improving the properties of plastic materials.
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To investigate processes possibly underlying accumulation and ecological effects of plastic nano-particles we have characterized their interaction with the cell wall of green algae. More specifically, we have investigated the influence of particle surface functionality and water hardness (Ca²⁺ concentration) on particle adsorption to algae cell walls. Polystyrene nanoparticles with different functional groups (non-functionalized, −COOH and −NH2) as well as coated (starch and PEG) gold nanoparticles were applied in these studies. Depletion measurements and atomic force microscopy (AFM) showed that adsorption of neutral and positively charged plastic nanoparticles onto the cell wall of P. subcapitata was stronger than that of negatively charged plastic particles. Results indicated that binding affinity is a function of both inter-particle and particle-cell wall interactions which are in turn influenced by the medium hardness and particle concentration. Physicochemical modeling using DLVO theory was used to interpret the experimental data, using also values for interfacial surface free energies. Our study shows that material properties and medium conditions play a crucial role in the rate and state of nanoparticle bio-adsorption for green algae. The results show that the toxicity of nanoparticles can be better described and assessed by using appropriate dose metrics including material properties, complexation/agglomeration behavior and cellular attachment and adsorption. The applied methodology provides an efficient and feasible approach for evaluating potential accumulation and hazardous effects of nanoparticles to algae caused by particle interactions with the algae cell walls.
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There has been a considerable increase on research of the ecological consequences of microplastics released into the environment, but only a handful of works have focused on the nano-sized particles of polymer-based materials. Though their presence has been difficult to adequately ascertain, due to the inherent technical difficulties for isolating and quantifying them, there is an overall consensus that these are not only present in the environment – either directly released or as the result of weathering of larger fragments – but that they also pose a significant threat to the environment and human health, as well. The reduced size of these particulates (< 1 μm) makes them susceptible of ingestion by organisms that are at the base of the food-chain. Moreover, the characteristic high surface area-to-volume ratio of nanoparticles may add to their potential hazardous effects, as other contaminants, such as persistent organic pollutants, could be adsorbed and undergo bioaccumulation and bioamplification phenomena.
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The global estimation of microplastic afloat in the ocean is only approximately 1% of global plastic inputs. This reflects fundamental knowledge gaps in the transformation, fragmentation and fates of microplastics in the ocean. In order to better understand microplastic fragmentation we proceeded to a thorough physicochemical characterization of samples collected from the North Artlantic sub-tropical gyre during the sea campaign Expedition 7th Continent in May 2014. The results were confronted with a mathematical approach. The introduction of mass distribution in opposition to the size distribution commonly proposed in this area clarify the fragmentation pattern. The mathematical analysis of the mass distribution points out a lack of mass for debris lighter than 1 mg, which corresponds to a size of 2 mm. Characterization by means of microscopy, microtomography and infrared microscopy gives a better understanding of the behavior of microplastic at sea. Flat pieces of debris (5-2 mm), referred to as parallelepipeds, float with one face preferentially exposed to the sun. This face is more photodegraded and biofilm also develops preferentially on it. Smaller debris, with a cubic shape (below 2 mm), seems to roll at sea. All faces are evenly photodegraded and they are less colonized. The breakpoint in the mathematical model and the experimental observation around 2 to 1 mm leads to the conclusion that there is a discontinuity in the rate of fragmentation: we hypothesized that the smaller microplastics, the cubic ones mostly, are fragmented much faster than the parallelepipeds.
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In this work, we present for the first time undeniable evidence of nano-plastic occurrence due to solar light degradation of marine micro-plastics under controlled and environmentally representative conditions. As observed during our recent expedition (Expedition 7th Continent), plastic pollution will be one of the most challenging ecological threats for the next generation. Up to now, all studies have focused on the environmental and the economic impact of millimeter scale plastics. These plastics can be visualized, collected and studied. We are not aware of any studies reporting the possibilities of nano-plastics in marine water. Here, we developed for the first time a new solar reactor equipped with a nanoparticle detector to investigate the possibility of the formation of nano-plastics from millimeter scale plastics. With this system, correlated with electronic microscopy observations, we identified for the first time the presence of plastics at the nano-scale in water due to UV degradation. Based on our observations large fractal nano-plastic particles (i.e., >100 nm) are produced by UV light after the initial formation of the smallest nano-plastic particles (i.e., <100 nm). These unprecedented results show the new and unprecedented potential hazards of plastic waste at the nanoscale, which had not been taken into account previously.
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Plastic debris is a prolific contaminant effecting freshwater and marine ecosystems across the globe. Of growing environmental concern are 'microplastics' and 'nanoplastics', encompassing tiny particles of plastic derived from manufacturing and macroplastic fragmentation. Pelagic zooplankton are susceptible to consuming microplastics, however the threat posed to larvae of commercially important bivalves is currently unknown. We exposed Pacific oyster (Crassostrea gigas) larvae (3-24 d.p.f.) to polystyrene particles spanning 70 nm-20 µm in size, including plastics with differing surface properties, and tested the impact of microplastics on larval feeding and growth. The frequency and magnitude of plastic ingestion over 24 hours varied by larval age and size of polystyrene particle (ANOVA, P<0.01), and surface properties of the plastic, with aminated particles ingested and retained more frequently (ANOVA, P<0.01). A strong, significant correlation between propensity for plastic consumption and plastic load per organism was identified (Spearmans, r=0.95, P<0.01). Exposure to 1 and 10 µm PS for up to 8 days had no significant effect on C. gigas feeding or growth at <100 microplastics mL-1. In conclusion, whilst micro- and nanoplastics were readily ingested by oyster larvae, exposure to plastic concentrations exceeding those observed in the marine environment resulted in no measurable effects on the development or feeding capacity of the larvae over the duration of the study.
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High concentrations of plastic debris have been observed in the oceans. Much of the recent concern has focussed on microplastics in the marine environment. Recent studies of the size distribution of the plastic debris suggested that continued fragmenting of microplastics into nano-sized particles may occur. In this review we assess the current literature on the occurrence of environmentally released micro- and nanoplastics in the human food production chain and their potential health impact. The currently used analytical techniques introduce a great bias in the knowledge, since they are only able to detect plastic particles well above the nano-range. We discuss the potential use of the very sensitive analytical techniques that have been developed for the detection and quantification of engineered nanoparticles. We recognize three possible toxic effects of plastic particles: firstly due to the plastic particles themselves, secondly to the release of persistent organic pollutant adsorbed to the plastics, and thirdly to the leaching of additives of the plastics. The limited data on microplastics in foods do not predict adverse effect of these pollutants or additives. Potential toxic effects of microplastic particles will be confined to the gut. The potential human toxicity of nanoplastics is poorly studied. Based on our experiences in nanotoxicology we prioritized future research questions.
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Plastic debris are resistant to degradation, and therefore tend to accumulate in marine environment. Nevertheless recent estimations of plastic concentrations at the surface of the ocean were lower than expected leading the communities to seek new sinks. Among the different processes suggested we chose to focus on the transport of microplastics from the surface to deeper layers of the ocean via phytoplankton aggregates that constitute most of the sinking flux. Interactions between microplastics and aggregates were studied by building a new device: the flow-through roller tank that mimics the behaviour of laboratory made aggregates sinking through a dense layer of microplastics. Three types of aggregates formed from two different algae species (the diatom Chaetoceros neogracile, the cryptophyte Rhodomonas salina and a mix) were used as model. With their frustule made of biogenic silica which is denser than the organic matter, diatom aggregates sunk faster than R. salina aggregates. Diatom aggregates were on average bigger and stickier while aggregates from R. salina were smaller and more fragile. With higher concentrations measured in R. salina aggregates, all model-aggregates incorporated and concentrated microplastics, substantially increasing the microplastic sinking rates from tenths to hundreds of metres per day. Our results clearly show that marine aggregates can be an efficient sink for microplastics by influencing their vertical distribution in the water column. Furthermore, despite the high plastic concentrations tested, our study opens new questions regarding the impact of plastics on sedimentation fluxes in oceans. As an effect of microplastic incorporation, the sinking rates of diatom aggregates strongly decreased meanwhile sinking rates of cryptophyte aggregates increased.
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Microscopic plastic debris, termed "microplastics", are of increasing environmental concern. Recent studies have demonstrated that a range of zooplankton, including copepods, can ingest microplastics. Copepods are a globally abundant class of zooplankton that form a key trophic link between primary producers and higher trophic marine organisms. Here we demonstrate that ingestion of microplastics can significantly alter the feeding capacity of the pelagic copepod Calanus helgolandicus. Exposed to 20 μm polystyrene beads (75 microplastics mL(-1)) and cultured algae ([250 μg C L(-1)) for 24 h, C. helgolandicus ingested 11% fewer algal cells (P = 0.33) and 40% less carbon biomass (P < 0.01). There was a net downward shift in the mean size of algal prey consumed (P < 0.001), with a 3.6 fold increase in ingestion rate for the smallest size class of algal prey (11.6-12.6 μm), suggestive of postcapture or postingestion rejection. Prolonged exposure to polystyrene microplastics significantly decreased reproductive output, but there were no significant differences in egg production rates, respiration or survival. We constructed a conceptual energetic (carbon) budget showing that microplastic-exposed copepods suffer energetic depletion over time. We conclude that microplastics impede feeding in copepods, which over time could lead to sustained reductions in ingested carbon biomass.
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Dynamic light scattering has evolved as a fast, convenient tool for particle size analysis of non-interacting spherical colloids. In this instructional review, we discuss the basic principle, data analysis and important precautions to be taken while analysing colloids using DLS. The effect of particle interaction, polydispersity, anisotropy, light absorption etc on measured diffusion coefficient is discussed. New developments in this area such as diffusing wave spectroscopy, particle tracking analysis, microrheological studies using DLS etc are discussed in a manner that can be understood by a beginner.
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With the accelerating introduction of engineered nanomaterials into commercial products and their potential use in water-treatment processes, it is inevitable that these materials will ultimately reside at some level in our recreational and drinking waters, thereby creating a critical need to detect and to quantify them in those media.Much is known about the diversity of engineered nanoparticles (ENPs) in the environment but almost nothing about their characterization and detection in the natural aquatic environment.There is no conventional treatment that can absolutely protect the consumer from exposure to ENPs either through recreational use or consumption of drinking waters. The question is whether this exposure poses a significant public health risk.Unfortunately, we are far from having methods to obtain data on occurrence levels, fate, and transport of ENPs in aquatic systems. Before a sound analytical approach can be developed, we need a fuller understanding of the nanomaterial domain which requires an evaluation of the matrix of source materials, their transformation in the natural aquatic environment, and their physical/chemical behavior that is specific to the water medium.We review characterization techniques that are used for identifying different types of ENP, and then, by extrapolation from isolation techniques appropriate for extracting ENPs from water, suggest approaches to analyzing them in a variety of waters.
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Nanoparticles are important in natural environments due to their size, tunable properties and accessible surfaces and our control over these properties can be exploited to create or add value to a variety of technologies. Many consumer products that incorporate nanoparticles, such as sunscreens and clothing, are already in the marketplace, and the industry is growing fast. This book highlights also the many valuable environmental technologies that can come from the applications of unique nanomaterial properties. As this nascent technology area matures, the debate about the whether the unknown risks of nanomaterial use balances its established benefits will only intensify.
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In this work we study the kinetics of coagulation of monodisperse spherical colloids in aqueous suspension at the early stage of coagulation. We have performed the measurements on a multiangle static and dynamic light scattering instrument using a fiber-optics-based detection system which permits simultaneous time-resolved measurements at different angles. The absolute coagulation rate constants are determined from the change of the scattering light intensity as well as from the increase of the hydrodynamic radius at different angles. The combined evaluation of static and dynamic light scattering results permits the determination of coagulation rate constants without the explicit use of light scattering form factors for the aggregates. For different electrolytes fast coagulation rate constants were estimated. Stability curves were measured as a function of ionic strength using different particle concentrations.
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This review discusses the mechanisms of generation and potential impacts of microplastics in the ocean environment. Weathering degradation of plastics on the beaches results in their surface embrittlement and microcracking, yielding microparticles that are carried into water by wind or wave action. Unlike inorganic fines present in sea water, microplastics concentrate persistent organic pollutants (POPs) by partition. The relevant distribution coefficients for common POPs are several orders of magnitude in favour of the plastic medium. Consequently, the microparticles laden with high levels of POPs can be ingested by marine biota. Bioavailability and the efficiency of transfer of the ingested POPs across trophic levels are not known and the potential damage posed by these to the marine ecosystem has yet to be quantified and modelled. Given the increasing levels of plastic pollution of the oceans it is important to better understand the impact of microplastics in the ocean food web.
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Nanotechnology has widespread application in agricultural, environmental and industrial sectors ranging from fabrication of molecular assemblies to microbial array chips. Despite the booming application of nanotechnology, there have been serious implications which are coming into light in the recent years within different environmental compartments, namely air, water and soil and its likely impact on the human health. Health and environmental effects of common metals and materials are well-known, however, when the metals and materials take the form of nanoparticles--consequential hazards based on shape and size are yet to be explored. The nanoparticles released from different nanomaterials used in our household and industrial commodities find their way through waste disposal routes into the wastewater treatment facilities and end up in wastewater sludge. Further escape of these nanoparticles into the effluent will contaminate the aquatic and soil environment. Hence, an understanding of the presence, behavior and impact of these nanoparticles in wastewater and wastewater sludge is necessary and timely. Despite the lack of sufficient literature, the present review attempts to link various compartmentalization aspects of the nanoparticles, their physical properties and toxicity in wastewater and wastewater sludge through simile drawn from other environmental streams.
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The industrial scale production and wide variety of applications of manufactured nanoparticles (NPs) and their possible release in considerable amounts into the natural aquatic environment have produced an increasing concern among the nanotechnology and environmental science community. In order to address this issue, it is important to understand NP chemistry, preparation, reactivity and possible mechanisms involved in their interaction with the naturally occurring aquatic components, particularly natural colloids and NPs present in the aquatic systems. In this review, an overview of the chemistry of both manufactured and natural aquatic NPs is outlined. This review discusses the physico-chemical aspects of both type of NPs as an essential point to assess possible routes involved in manufactured NP fate in the natural aquatic environment and their toxicity. Key advances related to the characterisation of the manufactured NPs and natural colloids.
Nanoplastic in the North atlantic subtropical gyre
  • A Ter Halle
  • L Jeannau
  • M Martignac
  • E Jard E
  • B Pedrono
  • L Brach
  • J Gigault
Ter Halle, A., Jeannau, L., Martignac, M., Jard e, E., Pedrono, B., Brach, L., Gigault, J., 2017. Nanoplastic in the North atlantic subtropical gyre. Env. Sci Technol. 51 (23), 13689e13697.