Y. Xu
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The growing demand for nuclear energy has intensified concerns over uranium (U) resource scarcity and the risks of environmental contamination, highlighting the urgency of developing efficient U separation technologies. Herein, we present a scalable synthesis of Mo3S13-intercalated layered double hydroxides (Mo3S13-LDH) by polysulfide clusters incorporation into MgAl-LDH. The resulting Mo3S13-LDH exhibits high affinity for U, achieving a high U adsorption capacity of 854.7 mg·g−1, rapid kinetics with saturation achieved within 2 h, and a removal efficiency exceeding 99.99% across a wide U concentration range (1–500 mg·L−1). Moreover, the Mo3S13-LDH retains high selectivity for U even in multi-ion conditions, as reflected by distribution coefficients ranging from 107 to 109 mL·g−1. Mechanistic analysis reveals that the U removal process involves electron transfer from sulfur to molybdenum, coupled with the reduction of U(VI) to U(IV). In simulated marine contamination experiments using water from the Yellow Sea and Bohai Seas spiked with 3 mg·L−1 U(VI), Mo3S13-LDH achieved 77.9% U removal while maintaining high selectivity amid a complex ionic background. These results position Mo3S13-LDH as a promising material for selective U recovery and emergency remediation in challenging aquatic environments. Beyond its high efficiency and practical applicability, Mo3S13-LDH represents a robust and scalable strategy for mitigating U contamination in diverse environmental contexts.
In the face of rising energy demands for high-salinity wastewater treatment, the abundant salt content presents a novel opportunity for salinity gradient energy harvesting, which can drive metal recovery processes. A “waste-controls-waste” strategy was developed by exploiting the salinity gradient to drive chromium reduction, achieving synergistic energy recovery and heavy metal removal. Based on this, an asymmetric nanochannel was designed to couple high-salinity and Cr-containing wastewater, enabling a green, self-powered treatment process. A cation-selective heterogeneous membrane was fabricated via a facile vacuum filtration method, wherein one-dimensional aramid nanofibers (ANFs) were intercalated between two-dimensional graphene oxide (GO) sheets to form an ordered lamellar structure. The structure was subsequently assembled onto an anodized aluminum oxide (AAO) substrate. The ANF-GO/AAO membrane, with a “line-plane” hybrid architecture, exhibited high cation selectivity and pronounced ion rectification due to its bipolar charge configuration. By mixing high-salinity wastewater and Cr-laden wastewater through the ANF-GO/AAO membrane, substantially high-power density of up to 39.22 W m−2 was achieved, along with an energy conversion efficiency of 25.60% under extreme salinity gradients. Nernst-Planck simulations revealed that ion selectivity and energy conversion in the heterogeneous membranes are dictated by their asymmetric architecture and the negatively charged selective layer. The harvested electrical energy directly drove the electrochemical reduction of Cr (VI), achieving a removal amount of 18.77 mol cm−2 under acidic conditions. A “waste-controls-waste” strategy harnesses salinity gradients to drive Cr(VI) reduction, achieving simultaneous energy recovery and heavy metal removal. An asymmetric nanochannel couples high-salinity and Cr-laden wastewater, enabling a green, self-powered treatment system.
Natural Weathering Reshapes Nanoplastic Aggregation and Deposition Dynamics
Implications for Nanoplastic Removal during Riverbank Filtration
Microplastic-affected pathogens in drinking water supply systems
Survival mechanisms, ecological impacts and control challenges
Microplastics (MPs), as emerging pollutants, can affect pathogens, primarily opportunistic pathogens (OPs), and influence their behavior in aquatic environments. However, evidences regarding their impacts in drinking water supply systems (DWSSs) remain scarce. Focusing on the safety of DWSSs, this review synthesizes how MPs affect pathogen proliferation, transport, and resistance development under typical DWSS conditions characterized by low nutrients, high flow rates, oxidative stress, and user demand. MPs can distinctly promote the growth and reproduction of pathogens, act as mobile carriers enabling cross-watershed transport, and facilitate direct migration from source water to humans, thereby increasing health risks. Furthermore, MPs enhance pathogen resistance at both individual and community levels, thereby complicating subsequent control efforts. This study further summarizes how MPs compromise existing pathogen control measures in DWSSs and introduce secondary risks, including MP additives and the disinfection by-products from MPs. Finally, a strategy integrating “pretreatment interception” and “secondary risk reduction” is proposed to control MP-affected pathogens in DWSSs. The review provides valuable insights into mitigating pathogen risks associated with MPs in DWSSs, addressing a significant knowledge gap in safeguarding water security.
Photochemical weathering and eco-corona formation through natural organic matter (NOM) adsorption play vital roles in the aggregation tendencies of nanoplastics (NPs) in aquatic environments. However, it remains unclear how photochemical weathering alters the adsorption patterns of NOM and the conformation of the eco-corona, subsequently affecting the aggregation tendencies of NPs. This study examined the effect of Suwannee River NOM adsorption on the aggregation kinetics of pristine and photoaged polystyrene (PS) NPs in monovalent electrolyte solutions. The results showed that photochemical weathering influenced the conformation of the eco-corona, which, in turn, determined NP stability in the presence of NOM. Hydrophobic components of NOM predominantly bound to pristine NPs through hydrophobic and π-π interactions, and extended hydrophilic segments in water hindered NP aggregation via steric repulsion. Conversely, hydrogen bonding facilitated the binding of these hydrophilic segments to multiple photoaged NPs, thereby destabilizing them through polymer bridging. Additionally, the stabilization and destabilization capacities of NOM increased with its concentration and molecular weight. These findings shed light on the destabilizing role of NOM in weathered NPs, offering new perspectives on environmental colloidal chemistry and the fate of NPs in complex aquatic environments.
The excessive use and accumulation of water-soluble polymers (WSPs, known as “liquid plastics”) in the environment can pose potential risks to both ecosystems and human health, but the environmental fate of WSPs remains unclear. Here, the adsorption behavior of WSPs with different molecular weight on kaolinite (Kaol) and montmorillonite (Mt) were examined. The results showed that the adsorption of PEG and PVP on minerals were controlled by hydrogen bond and van der Waals force. The Fourier transform infrared (FTIR) spectra and two-dimensional correlation spectroscopy (2D-COS) analysis revealed that there were interactions between the Al-O and Si-O groups of the minerals and the polar O- or N-containing functional groups as well as the alkyl groups of PEG and PVP. The adsorption characteristics of WSPs were closely related to their molecular weight and the pore size of minerals. Due to the relatively large mesopore size of Kaol, both PEG and PVP were absorbed into inner spaces, for which the adsorption capacity increased with molecular weight of the polymers. For Mt, all types of PEG could enter its micropores, while PVP with larger molecular weights appeared to be confined externally, leading to a decrease in the adsorption capacity of PVP with increasing molecular weight. The findings of this study provide a theoretical basis for scientific evaluation of environmental processes of WSPs.
Photodegradation of microplastics (MPs) induced by sunlight plays a crucial role in determining their transport, fate, and impacts in aquatic environments. Dissolved black carbon (DBC), originating from pyrolyzed carbon, can potentially mediate the photodegradation of MPs owing to its potent photosensitization capacity. This study examined the impact of pyrolyzed wood derived DBC (5 mg C/L) on the photodegradation of polystyrene (PS) MPs in aquatic solutions under UV radiation. It revealed that the photodegradation of PS MPs primarily occurred at the benzene ring rather than the aliphatic segments due to the fast attack of hydroxyl radical (•OH) and singlet oxygen (1O2) on the benzene ring. The photosensitivity of DBC accelerated the degradation of PS MPs, primarily attributed to the increased production of •OH, 1O2, and triplet-excited state DBC (3DBC*). Notably, DBC-mediated photodegradation was related to its molecular weight (MW) and chemical properties. Low MW DBC (<3 kDa) containing more carbonyl groups generated more •OH and 1O2, accelerating the photodegradation of MPs. Nevertheless, higher aromatic phenols in high MW DBC (>30 kDa) scavenged •OH and generated more O2•-, inhibiting the photodegradation of MPs. Overall, this study offered valuable insights into UV-induced photodegradation of MPs and highlighted potential impacts of DBC on the transformation of MPs.
Synthetic textiles are a significant source of microplastic fibre pollution. While the microplastic fibre release mechanism during the washing of textiles is well studied, little is known about the release of nanoplastics. The first investigations on the nanoplastic fraction released during the washing and abrasion of polyester textiles have been published; however, questions were raised regarding the chemical composition of the observed submicrometre particles. Using a combination of analytical methods, we show here that 12 different polyester textiles released 4.6 × 1010 to 8.9 × 1011 particles per gram of textile during washing, with a mean size of 122–191 nm. The number of released submicrometre particles was not significantly influenced by the cutting method nor by the textile structure, but positively correlated (P < 0.01) with the number of submicrometre particles present on the fibre surface before washing. We found that 34–89% of the extracted submicrometre particles were soluble in ethanol. These particles are most likely water-insoluble poly(ethylene terephthalate) oligomers. Our results clearly show the urgent need to better understand the contribution of water-insoluble oligomer particles to the pollution of the environment by anthropogenic nanoplastics.
Increasing wildfire frequency, a consequence of global climate change, releases incomplete combustion byproducts such as aquatic pyrogenic dissolved organic matter (DOM) and black carbon (DBC) into waters, posing a threat to water security. In August 2022, a series of severe wildfires occurred in Chongqing, China. Samples from seven locations along the Yangtze and Jialing Rivers revealed DBC, quantified by the benzene poly(carboxylic acid) (BPCA) method, comprising 9.5-19.2% of dissolved organic carbon (DOC). High concentrations of BPCA-DBC with significant polycondensation were detected near wildfire areas, likely due to atmospheric deposition driven by wind. Furthermore, Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) revealed that wildfires were associated with an increase in condensed aromatics, proteins, and unsaturated hydrocarbons, along with a decrease in lignins. The condensed aromatics primarily consisted of dissolved black nitrogen (DBN), contributing to abundant high-nitrogen-containing compounds in locations highly affected by wildfires. Meanwhile, wildfires potentially induced the input of recalcitrant sulfur-containing protein-like compounds, characterized by high oxidation, aliphatic nature, saturation, and low aromaticity. Overall, this study revealed the appearance of recalcitrant DBC and dissolved organic sulfur in river waters following wildfire events, offering novel insights into the potential impacts of wildfires on water quality and environmental biogeochemistry.
The occurrence and removal of microplastics (MPs) in drinking water treatment plants (DWTPs) have been evaluated based on particle number, while the mass concentration and removal characteristics based on the mass of MPs, and especially nanoplastics (NPs), remain unknown. This study employed pyrolysis gas chromatography-mass spectrometry (Py-GC/MS) to determine the mass concentration of MPs and NPs with different size ranges (0.01-1, 1-50, and 50-1000 μm) across the entire treatment process in a DWTP. The total polymers were measured at 9.63 ± 1.52 μg/L in raw water and 0.77 ± 0.05 μg/L in treated water, with the dominant polymers being polypropylene and polyethylene terephthalate. NPs (0.01-1 μm) accounted for only 3.2-5.3% of the total polymers, with an average concentration of 0.38 μg/L in raw water and 0.04 μg/L in treated water. Notably, NPs and sub-MPs (1-50 μm) demonstrated relatively low efficiency in the DWTP at 88.9 ± 3.2 and 88.0 ± 2.5%, respectively, compared with that of the large MPs (50-1000 μm) at 92.9 ± 0.3%. Overall, this study examined the occurrence of MPs and NPs, in a DWTP, emphasizing the significance of considering the mass concentration of MPs and NPs when assessing their pollution levels and removal characteristics.
Photo-oxidation of Micro-and Nanoplastics
Physical, Chemical, and Biological Effects in Environments
Correction to
Oligomers are a major fraction of the submicrometre particles released during washing of polyester textiles (Nature Water, (2024), 2, 2, (151-160), 10.1038/s44221-023-00191-5)
Correction to: Nature Waterhttps://doi.org/10.1038/s44221-023-00191-5, published online 8 February 2024. In the version of the article initially published, there was an error in the title: the phrase “submicrometre particles released during washing” originally appeared as “released submicrometre particles released during washing”. This has now been corrected in the HTML and PDF versions of the article.
The level of microplastics (MPs) in wastewater treatment plants (WWTPs) has been well evaluated by the particle number, while the mass concentration of MPs and especially nanoplastics (NPs) remains unclear. In this study, pyrolysis gas chromatography-mass spectrometry was used to determine the mass concentrations of MPs and NPs with different size ranges (0.01-1, 1-50, and 50-1000 μm) across the whole treatment schemes in two WWTPs. The mass concentrations of total MPs and NPs decreased from 26.23 and 11.28 μg/L in the influent to 1.75 and 0.71 μg/L in the effluent, with removal rates of 93.3 and 93.7% in plants A and B, respectively. The proportions of NPs (0.01-1 μm) were 12.0-17.9 and 5.6-19.5% in plants A and B, respectively, and the removal efficiency of NPs was lower than that of MPs (>1 μm). Based on annual wastewater effluent discharge, it is estimated that about 0.321 and 0.052 tons of MPs and NPs were released into the river each year. Overall, this study investigated the mass concentration of MPs and NPs with a wide size range of 0.01-1000 μm in wastewater, which provided valuable information regarding the pollution level and distribution characteristics of MPs, especially NPs, in WWTPs.
The extracellular polymeric substances (EPS) from activated sludge played significant roles in the removal of nanoparticles from wastewater. A series of batch experiments were carried out to determine the adsorption mechanism of three nano-Ag by activated sludge, as well as the contributions of EPS fractions including dissolved EPS (DEPS), loosely bound EPS (LB-EPS) and tightly bound EPS (TB-EPS). The results demonstrated that the adsorption of nano-Ag by sludge biomass agreed with pseudo-second-order kinetic reaction model and Freundlich isotherm model. About 26.0-41.2% of nano-Ag was trapped by the bound EPS (BEPS) matrix of activated sludge (especially LB-EPS) and 42.5-52.6% of them was adsorbed onto the inner cells after the adsorption. Moreover, the interaction energy contributions of EPS fractions followed the order of EDE > 0 > ETB > ELB, suggesting DEPS in wastewater went against the removal of nano-Ag due to steric repulsion while LB-EPS and TB-EPS were positive to nano-Ag adsorption by modifying biomass surface and providing extensive binding sites. Besides, EPS fractions played significant roles in the adsorption of nano-Ag with low initial concentrations but had limited effect at high concentrations. Overall, this study investigated the effect of EPS fractions on the adsorption behaviors of nano-Ag by activated sludge biomass, which is meaningful to understand the removal mechanism of nanoparticles in sewage and the potential role of EPS fractions.
Influence of dissolved black carbon on the aggregation and deposition of polystyrene nanoplastics
Comparison with dissolved humic acid
Dissolved black carbon (DBC), widely found in soil and water environments is likely to affect the transport of nanoplastics in aquatic environments. The aggregation and deposition behaviors of fresh and aged polystyrene nanoplastics (PSs) with and without DBC in NaCl solution were investigated by time-resolved dynamic light scattering (DLS) and quartz crystal microbalance with dissipation monitoring equipment (QCM-D) techniques. The results suggest that DBC can screen the surface charges of PSs by interacting with PSs through hydrogen bonding, hydrophobic interactions and π-π interactions, although they were negatively charged. DBC promoted the aggregation of PSs under relatively low ionic strengths, and it minimally affected the stability of PSs under high ionic strength. Deposition experiments showed that both DBC in salt solution and DBC adsorption on silica surface facilitated the deposition of fresh PSs while HA inhibited both deposition processes. After aging, PSs were more stable, and the effects of DBC and HA were weakened. This study investigated the influence mechanism of DBC on the aggregation and deposition behaviors, which provides new insights into the stability and transport of PSs in complex aquatic environments.
Nanoplastics (NPs) are currently considered an environmental pollutant of concern, but the actual extent of NP pollution in environmental water bodies remains unclear and there is not enough quantitative data to conduct proper risk assessments. In this study, a pretreatment method combining ultrafiltration (UF, 100 kDa) with hydrogen peroxide digestion and subsequent detection with pyrolysis gas chromatography-mass spectrometry (Py-GC/MS) was developed and used to identify and quantify six selected NPs in surface water (SW) and groundwater (GW), including poly(vinylchloride) (PVC), poly(methyl methacrylate) (PMMA), polypropylene (PP), polystyrene (PS), polyethylene (PE), and poly(ethylene terephthalate) (PET). The results show that the proposed method could detect NPs in environmental water samples. Nearly all selected NPs could be detected in the surface water at all locations, while PVC, PMMA, PS, and PET NPs were frequently below the detection limit in the groundwater. PP (32.9-69.9%) and PE (21.3-44.3%) NPs were the dominant components in both surface water and groundwater, although there were significant differences in the pollution levels attributed to the filtration efficiency of riverbank, with total mass concentrations of 0.283-0.793 μg/L (SW) and 0.021-0.203 μg/L (GW). Overall, this study quantified the NPs in complex aquatic environments for the first time, filling in gaps in our knowledge about NP pollution levels and providing a useful methodology and important reference data for future research.