ACS Environmental Au最新文献

Per/polyfluoroalkyl substances (PFASs) are ubiquitous, highly persistent anthropogenic chemicals that bioaccumulate and biomagnify in aquatic food webs and are associated with adverse health effects, including liver and kidney diseases, cancers, and immunosuppression. We investigated the accumulation of PFASs in a marine apex predator, the white shark (Carcharodon carcharias). Muscle (N = 12) and blood plasma (N = 27) samples were collected from 27 sharks during 2018–2021 OCEARCH expeditions along the eastern coast of North America from Nova Scotia to Florida. Samples were analyzed for 47 (plasma) and 43 (muscle) targeted PFASs and screened for >2600 known and novel PFASs using liquid chromatography coupled to high-resolution mass spectrometry (LC-HRMS). Perfluoroalkyl carboxylates with carbon chain-length C11 to C14 were frequently detected above the method reporting limits in plasma samples, along with perfluorooctanesulfonate and perfluorodecanesulfonate. Perfluoropentadecanoate was also detected in 100% of plasma samples and concentrations were estimated semiquantitatively as no analytical standard was available. Total concentrations of frequently detected PFASs in plasma ranged from 0.56 to 2.9 ng mL^–1 (median of 1.4 ng mL^–1). In muscle tissue, nine targeted PFASs were frequently detected, with total concentration ranging from 0.20 to 0.84 ng g^–1 ww. For all frequently detected PFASs, concentrations were greater in plasma than in muscle collected from the same organism. In both matrices, perfluorotridecanoic acid was the most abundant PFAS, consistent with several other studies. PFASs with similar chain-lengths correlated significantly among the plasma samples, suggesting similar sources. Total concentrations of PFASs in plasma were significantly greater in sharks sampled off of Nova Scotia than all sharks from other locations, potentially due to differences in diet. HRMS suspect screening tentatively identified 13 additional PFASs in plasma, though identification confidence was low, as no MS/MS fragmentation was collected due to low intensities. The widespread detection of long-chain PFASs in plasma and muscle of white sharks highlights the prevalence and potential biomagnification of these compounds in marine apex predators.

Nitrogen in wastewater has negative environmental, human health, and economic impacts but can be recovered to reduce the costs and environmental impacts of wastewater treatment and chemical production. To recover ammonia/ammonium (total ammonia nitrogen, TAN) from urine, we operated electrochemical stripping (ECS) for over a month, achieving 83.4 ± 1.5% TAN removal and 73.0 ± 2.9% TAN recovery. With two reactors, we recovered sixteen 500-mL batches (8 L total) of ammonium sulfate (20.9 g/L TAN) approaching commercial fertilizer concentrations (28.4 g/L TAN) and often having >95% purity. While evaluating the operation and maintenance needs, we identified pH, full-cell voltage, product volume, and water flux into the product as informative process monitoring parameters that can be inexpensively and rapidly measured. Characterization of fouled cation exchange and omniphobic membranes informs cleaning and reactor modifications to reduce fouling with organics and calcium/magnesium salts. To evaluate the impact of urine collection and storage on ECS, we conducted experiments with urine at different levels of dilution with flush water, extents of divalent cation precipitation, and degrees of hydrolysis. ECS effectively treated urine under all conditions, but minimizing flush water and ensuring storage until complete hydrolysis would enable energy-efficient TAN recovery. Our experimental results and cost analysis motivate a multifaceted approach to improving ECS’s technical and economic viability by extending component lifetimes, decreasing component costs, and reducing energy consumption through material, reactor, and process engineering. In summary, we demonstrated urine treatment as a foothold for electrochemical nutrient recovery from wastewater while supporting the applicability of ECS to seven other wastewaters with widely varying characteristics. Our findings will facilitate the scale-up and deployment of electrochemical nutrient recovery technologies, enabling a circular nitrogen economy that fosters sanitation provision, efficient chemical production, and water resource protection.

Novel visible-light-driven Ag (X)-doped Bi₂Zr₂O₇ (BZO) nanocomposites in pudina (P) extract (Mentha spicata L.), X-1, 3, 5, 7, and 9 mol %, were synthesized by the one-pot greener solution combustion method. The as-synthesized nanocomposite materials were characterized by using various spectral [X-ray diffraction (XRD), Fourier transform infrared, UV–visible, UV– diffuse reflectance spectra, X-ray photoelectron spectroscopy], electrochemical (cyclic voltammetry, electrochemical impedance spectroscopy), and analytical (scanning electron microscopy–energy-dispersive X-ray spectroscopy, transmission electron microscopy, Brunauer–Emmett–Teller) techniques. The average particle size of the nanocomposite material was found to be between 14.8 and 39.2 nm by XRD. The well-characterized Ag-doped BZOP nanocomposite materials exhibited enhanced photocatalytic degradation activity toward hazardous dyes such as methylene blue (MB) and rose bengal (RB) under visible light irradiation ranges between 400 and 800 nm due to their low energy band gap. As a result, 7 mol % of Ag-doped BZOP nanocomposite material exhibited excellent photodegradation activity against MB (D.E. = 98.7%) and RB (D.E. = 99.3%) as compared to other Ag-doped BZOP nanocomposite materials and pure BZOP nanocomposite, respectively, due to enhanced semiconducting and optical behaviors, high binding energy, and mechanical and thermal stabilities. The Ag-doped BZOP nanocomposite material-based electrochemical sensor showed good sensing ability toward the determination of lead nitrate and dextrose with the lowest limit of detection (LOD) of 18 μM and 12 μM, respectively. Furthermore, as a result of the initial antibacterial screening study, the Ag-doped BZOP nanocomposite material was found to be more effective against Gram-negative bacteria (Escherichia coli) as compared to Gram-positive (Staphylococcus aureus) bacteria. The scavenger study reveals that radicals such as O₂^•– and ^•OH are responsible for MB and RB mineralization. TOC removal percentages were found to be 96.8 and 98.5% for MB and RB dyes, and experimental data reveal that the Ag-doped BZOP enhances the radical (O₂^•– and ^•OH) formation and MB and RB degradation under visible-light irradiation.

Membrane-based water purification is poised to play an important role in tackling the potable water crisis for safe and clean water access for the general population. Several studies have focused on near two-dimensional membranes for this purpose, which is based on an ion rejection technique. However, membrane swelling in these materials has emerged as a significant challenge because it leads to the loss of function. Herein, we report a self-cross-linked MXene-intercalated graphene oxide (GO) membrane that retains ion and dye rejection properties because the physical cross-linking interaction between Ti–O–Ti and neighboring nanosheets effectively suppresses the swelling of the membrane. In addition to the associative Ti–O–Ti bonds, C–O–C, O═C–O, and C–OH bonds are also formed, which are important for inhibiting the swelling of the membrane. To ensure the longevity of these membranes in a service context, they were subjected to heat pressurization and subsequent thermal annealing. The membrane subjected to this novel processing history exhibits minimal swelling upon immersion in solutions and retains function, rejecting salt and dyes over a wide range of salt and dye concentrations. Furthermore, these membranes successfully rejected dye and salt over a period of 72 h without a degradation of function, suggesting that these membranes have the requisite durability for water filtration applications.

Activated carbon-based supercapacitor electrodes synthesized from biomass or waste-derived biomass have recently attracted considerable attention because of their low cost, natural abundance, and power delivery performance. In this work, purple-corncob-based active carbons are prepared by KOH activation and subsequently evaluated as a composite electrode for supercapacitors using either an acidic or an alkali solution as the electrolyte. The synthesis of the material involves mixing the purple corncob powder with different concentrations of KOH (in the range of 5% to 30%) and a thermal treatment at 700 °C under an inert atmosphere. Physicochemical characterizations were performed using scanning electron microscopy, Raman spectroscopy, N₂ physisorption analysis, Fourier-transform infrared spectroscopy, and X-ray photoelectron spectroscopy, while the electrochemical characteristics were determined using cyclic voltammetry, a galvanostatic charge/discharge curve, and electrochemical impedance techniques measured in a three- and two-electrode system. Composite electrodes activated with 10% KOH had a specific surface area of 728 m² g^–1, and high capacitances of 195 F g^–1 at 0.5 A g^–1 in 1 mol L^–1 H₂SO₄ and 116 F g^–1 at 0.5 A g^–1 in 1 mol L^–1 KOH were obtained. It also presented a 76% capacitance retention after 50 000 cycles. These properties depend significantly on the microporous area and micropore volume characteristics of the activated carbon. Overall, our results indicate that purple corncob has an interesting prospect as a carbon precursor material for supercapacitor electrodes.

Ironically, healthcare systems are key agents in respiratory-related diseases and estimated deaths because of the high impact of their greenhouse gas emissions, along with industry, transportation, and housing. Based on safety requirements, hospitals and related services use an extensive number of consumables, most of which end up incinerated at the end of their life cycle. A thorough assessment of the carbon footprint of such devices typically requires knowing precise information about the manufacturing process, which is rarely available in detail because of the many materials, pieces, and steps involved during the fabrication. Yet, the tools most often used for determining the environmental impact of consumer goods require a bunch of parameters, mainly based on the material composition of the device. Here, we report a basic set of analytical methods that provide the information required by the software OpenLCA to calculate the main outcome related to environmental impact, greenhouse gas emissions. Through thermogravimetry, calorimetry, infrared spectroscopy, and elemental analysis, we proved that obtaining relevant data for the calculator in the exemplifying case of endoscopy tooling or accessories is possible. This routine procedure opens the door to a broader, more accurate analysis of the environmental impact of everyday work at hospital services, offering potential alternatives to minimize it.

Analyzing the molecular composition change of dissolved organic matter (DOM) during transportation in estuaries can enhance our understanding of the fate of DOM. However, the impact of hydrologic conditions resulting from large river plumes on the DOM cycle are less explored, and previous studies were insufficient to capture the molecular fate that occur during the transportation process. In this study, we used a range of bulk and optical techniques, as well as Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS), to determine the concentration and characteristics of DOM along two trajectories of downstream plumes of diluted water of the Yangtze (Changjiang) River estuary (YRE) during the high discharge season. These two plumes situated along the route of the summer Changjiang diluted water (CDW) have been identified and named CDW-North (CDW-N) and CDW-South (CDW-S), respectively. Despite having the same riverine end-member origin, the turbidity zone in YRE significantly modifies the molecular characteristics and composition of DOM. The results of FT-ICR MS indicated a spatial variation of DOM composition in the coastal zone of the two plumes. The relative intensities of the CHO, CHOS, and CHONS compounds are negatively correlated with salinity. In addition, the coastal zones of both CDW-N and CDW-S are characterized by more autochthonous DOM sources. More CHON compounds in CDW-N are probably due to the production of autochthonous DOM in offshore waters. The activity of phytoplankton increased the surface dissolved oxygen level of CDW-N in the coastal zone. However, the hypoxic zone formed at the bottom of the CDW-N due to microbial degradation of organic matter and may further benefit the preservation of CHON compounds. Our study emphasizes that the characteristics and composition of the estuarine DOM can be significantly shaped by distinct large river plumes. Furthermore, using FT-ICR MS in combination with complementary techniques can better assist in identifying the sources and transformation mechanisms of estuarine DOM in large river plume-affected systems and provide more valuable insights into the role of DOM in the estuarine biogeochemical cycle.

Effective techniques for eliminating antibiotics from water environments are in high demand. The peracetic acid (PAA)-based advanced oxidation process has recently drawn increasing attention for its effective antibiotic degrading capability. However, current applications of PAA-based techniques are limited and tend to have unsatisfactory performance. An additional catalyst for PAA activation could provide a promising solution to improve the performance of PAA. Bulky metal–organic framework gels (MOGs) stand out as ideal catalysts for PAA activation owing to their multiple advantages, including large surface areas, high porosity, and hierarchical pore systems. Herein, a bimetallic hierarchical porous structure, i.e., FeMn13BTC, was synthesized through a facile one-pot synthesis method and employed for PAA activation in ofloxacin (OFX) degradation. The optimized FeMn MOG/PAA system exhibited efficient catalytic performance, characterized by 81.85% OFX degradation achieved within 1 h owing to the specific hierarchical structure and synergistic effect between Fe and Mn ions, which greatly exceeded the performance of the only PAA-catalyzed system. Furthermore, the FeMn MOG/PAA system maintained >80% OFX degradation in natural water. Quenching experiments, electron spin resonance spectra, and model molecular degradation revealed that the primary reactive oxygen species responsible for the catalytic effect was R–O^•, especially CH₃C(═O)OO^•, with minor contributions of ^•OH and ¹O₂. Overall, introduction of the MOG catalyst strategy for PAA activation achieved high antibiotic degradation performance, establishing a paradigm for the design of heterogeneous hierarchical systems to broaden the scope of catalyzed water treatment applications.