ACS Environmental Au最新文献

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.

Residential wood combustion contributing to airborne particulate matter (PM₁₀) was studied for 1 year at two sites in the village of Melpitz. Significant excess pollution was observed at the Melpitz center compared to that at the TROPOS research station Melpitz reference site, situated only 700 m away. Local concentration increments at the village site for the combustion PM constituents organic carbon, elemental carbon, levoglucosan, and benzo[a]pyrene were determined under appropriate wind directions, and their winter mean values were 0.7 μg m^–3, 0.3 μg m^–3, 0.1 μg m^–3, and 0.4 ng m^–3, representing relative increases over the regional background concentration of 24, 70, 61, and 107%, respectively. Yearly, weekly, and diurnal profiles of village increments suggest residential heating as the dominant source of this excess pollution, mainly originating from wood combustion. Receptor modeling using positive matrix factorization quantified 4.5 μg m^–3 wood combustion PM at the village site, representing an increment of 1.9 μg m^–3 and an increase of ∼75% over the 2.6 μg m^–3 regional background wood combustion PM. This increment varied with season, temperature, and boundary layer height and reached daily mean values of 4–6 μg m^–3 during unfavorable meteorological conditions. Potential health effects were estimated and resulted in an all-cause mortality from short-term exposure to wood combustion PM of 2.1 cases per 100,000 inhabitants and year for areas with similar wood smoke levels as observed in Melpitz. The excess cancer risk from the concentrations of polycyclic aromatic hydrocarbons was 6.4 per 100,000. For both health metrics, the very local contributions from the village itself were about 40–50%, indicating a strong potential for mitigation through local-scale policies. A compilation of literature data demonstrates wood combustion to represent a major source of PM pollution in Germany, with average winter-time contributions of 10–20%. The present study quantifies the negative impacts of heating with wood in rural residential areas, where the continuous monitoring of air quality is typically lacking. Further regulation of this PM source is warranted in order to protect human health.

Manual dismantling, shredding, and mechanical grinding of waste from electrical and electronic equipment (WEEE) at recycling facilities inevitably lead to the accidental formation and release of both coarse and fine particle aerosols, primarily into the ambient air. Since diffuse emissions to air of such WEEE particles are not regulated, their dispersion from the recycling plants into the adjacent environment is possible. The aim of this interdisciplinary project was to collect and characterize airborne WEEE particles smaller than 1 μm generated at a Nordic open waste recycling facility from a particle concentration, shape, and bulk and surface composition perspective. Since dispersed airborne particles eventually may reach rivers, lakes, and possibly oceans, the aim was also to assess whether such particles may pose any adverse effects on aquatic organisms. The results show that WEEE particles only exerted a weak tendency toward cytotoxic effects on fish gill cell lines, although the exposure resulted in ROS formation that may induce adverse effects. On the contrary, the WEEE particles were toxic toward the crustacean zooplankter Daphnia magna, showing strong effects on survival of the animals in a concentration-dependent way.

Human occupants themselves constitute an important source of volatile organic compounds (VOCs) in indoor environments through breath and dermal emissions. In order to quantify VOC emissions from occupants under real-world settings, previous indoor observational studies often determined emission factors (i.e., average emission rates per person). However, the values obtained across these studies exhibited large variability, and the causes of this variability still need to be understood. Herein we report 10-day real-time VOC measurements in a university student office, using a proton transfer reaction-quadrupole interface-time-of-flight mass spectrometer. A method was developed to identify VOCs of primary human origin and to quantify the corresponding emission factors, accounting for the dynamically changing occupancy level and ventilation rate in the assessed office. We found that the emission factors of many dermally emitted VOCs strongly increased as the ozone concentration increased from <3 to 10–15 ppb. These VOCs include geranyl acetone, 6-methyl-5-hepten-2-one (6-MHO), and C₁₀-C₁₂ saturated aldehydes, which align with characteristic first-generation ozonolysis products of skin oil. The strongest increase occurred for 6-MHO, from 113 to 337 μg/h/p. In comparison, acetone and isoprene, which are primarily emitted from human breath, varied little with the ozone level. In light of this finding, we conducted an integrated analysis of emission factors reported in the literature for two frequently reported species, namely, 6-MHO and decanal. Ozone concentration alone can explain 94–97% of the variation in their emission factors across previous studies, and the best-estimated ozone dependence obtained using the literature data is consistent with those obtained in the current study. These results suggest that the ozone concentration is a key factor regulating emission factors of many dermally emitted VOCs in real indoor environments, which has to be considered when reporting or using the emission factors.

Triazine hydrolase fromArthrobacter aurescens TC1 (TrzN) was successfully immobilized on mesoporous silica nanomaterials (MSNs) for the first time. For both nonfunctionalized MSNs and MSNs functionalized with Zn(II), three pore sizes were evaluated for their ability to immobilize wild-type TrzN: Mobile composition of matter no. 41 (small, 3 nm pores), mesoporous silica nanoparticle material with 10 nm pore diameter (MSN-10) (medium, 6–12 nm pores), and pore-expanded MSN-10 (large, 15–30 nm pores). Of these six TrzN:MSN biomaterials, it was shown that TrzN:MSN-10 was the most active (3.8 ± 0.4 × 10^–5 U/mg) toward the hydrolysis of a 50 μM atrazine solution at 25 °C. The TrzN:MSN-10 biomaterial was then coated in chitosan (TrzN:MSN-10:Chit) as chitosan has been shown to increase stability in extreme conditions such as low/high pH, heat shock, and the presence of organic solvents. TrzN:MSN-10:Chit was shown to be a superior TrzN biomaterial to TrzN:MSN-10 as it exhibited higher activity under all storage conditions, in the presence of 20% MeOH, at low and high pH values, and at elevated temperatures up to 80 °C. Finally, the TrzN:MSN-10:Chit biomaterial was shown to be fully active in river water, which establishes it as a functional biomaterial under actual field conditions. A combination of these data indicate that the TrzN:MSN-10:Chit biomaterial exhibited the best overall catalytic profile making it a promising biocatalyst for the bioremediation of atrazine.