Journal of hazardous materials最新文献

The efficient treatment of phenol wastewater is of great necessity since it induces serious pollution of water and soil ecosystems. Using biochar-immobilized functional microorganisms can innovatively and sustainably deal with the existing problem. In this study, we utilized response surface methodology (RSM) combined with life cycle assessment (LCA) to improve phenol biodegradation rate through a novel separated alkali-resistant and thermophilic strain Bacillus halotolerans ACY. Bioinformatic analysis revealed the genetic foundation of ACY to adapt to harsh environments. The characteristics of pig manure biochar (PMB) produced at varying pyrolysis temperatures (300-700 ℃) and adsorption experiment were investigated, immobilization of the phenol-degrading ACY on PMB600 under alkaline and high pollution load promoted phenol removal and extreme environment resistance, and the phenol removal rate reached 99.5 % in 7d in actual phenol wastewater, which increased compared with those achieved by PMB (50.6 %) and free bacteria (80.5 %) alone. Scanning Electron Microscope (SEM) and Fourier transform infrared spectrometry (FTIR) observations indicated the successful bacterial immobilization on PMB600. Reusability and economic cost study further demonstrated PMB600 as an excellent carrier for wastewater treatment. LC-MS, toxicology and carbon footprint analyses demonstrated that bacterial metabolism exerted synergy with adsorption for phenol removal, while biodegradation exerted the predominant impact on the immobilized bacterial system. This study provides an eco-friendly and effective approach to treat phenol wastewater.

Antibiotic resistance (AR) is a major public health concern. Antibiotic intermediates (AIs) used in the production of semisynthetic antibiotics have the same bioactive structure as parent antibiotics and synthetic antibiotic production wastewater usually contains high concentrations of residual AIs; however, the effects of AIs and their interactive effects with antibiotics on the emergence of AR are unknown. In this study, antibiotic-sensitive E. coli K12 was exposed to five types of β-lactam AIs and their parent antibiotic ampicillin to analyze their impact on the evolution of multiple AR. The results indicated that AI 6-APA inhibits bacterial growth and stimulates the production of reactive oxygen species, as well as induces AR and antibiotic persistence like the parent antibiotic AMP. Combined exposure to 6-APA and AMP synergistically stimulated the induction of multiple AR and antibiotic persistence. The resistance mutation frequency increased up to 6.1 × 10⁶-fold under combined exposure and the combination index reached 1326.5, indicating a strong synergy of 6-APA and AMP. Phenotypic and genotypic analyses revealed that these effects were associated with the overproduction of reactive oxygen species, enhanced stress response signatures, and activation of efflux pumps. These findings provide evidence and mechanistic insights into AR induction by AIs in antibiotic production wastewater.

How the anion ligands of manganese precursors affect the catalytic activity of amorphous manganese oxides (MnOx) in Fenton-like process is poorly understood. Here, five amorphous MnOx synthesized by Mn(II) precursors with different ligands were characterized and adopted to activate peracetic acid (PAA) for bisphenol A (BPA) degradation. Although > 90 % BPA removal was achieved in the five MnOx/PAA processes via both adsorption and oxidation, the oxidation k_obs greatly differentiates by the ligands types with the order of MnOx-N > MnOx-S > MnOx-Cl > MnOx-AA > MnOx-OA. Ligands types would affect the specific surface area of MnOx and their ability to adsorb BPA, however which is not the decisive factor in determining the contaminant oxidation efficiency. Multiple experimental results indicate that the generation of oxygen vacancies induced by the ligands alters the Mn(III)/Mn(IV) ratio, ultimately contributing to the different efficiency of BPA oxidation driven by the direct electron transfer mechanism. Moreover, amorphous MnOx holds the promise of practical applications in catalytic PAA of various micropollutants with good stability. This study advances the fundamental understanding of ligand-regulated amorphous MnOx-catalyzed PAA process.

This study systematically explored the role of Mn(II) in the removal of 4-chlorophenol (4-CP) by electro-oxidation (EO) employing anodes with low oxygen evolution potential (OEP), i.e., Ti/RuO₂-IrO₂, Ti/Pt, and Ti/Ti₄O₇, as well as anodes with high OEP, namely, Ti/PbO₂, Ti/SnO₂, and boron-doped diamond (Si/BDD). Mn(II) significantly promoted 4-CP removal on the anodes with low OEP at fairly low current density (0.04 to 1 mA/cm²), but had minimal to negative impact on those with high OEP. Cyclic voltammetry and X-ray photoelectron spectra revealed that Mn(II) was oxidized to Mn(III), then to Mn(IV) on the anodes with low OEP, whereas its was oxidized directly to Mn(IV) on those with high OEP. Deposition of manganese oxide on the anodes with low OEP suppressed oxygen evolution reaction (OER) in EO process, but enhanced OER on those with high OEP. Quenching and spectral results consistently indicated that Mn(III) and Mn(IV) were the primary species responsible for enhancing 4-CP removal on the anodes with low OEP. These findings provide mechanistic insights into the redox transformation of Mn(II) in EO and the theoretical basis for a novel strategy to boost pollutant degradation in EO systems using low OEP anodes through coupling with the redox chemistry of manganese.

The catalytic membrane-based oxidation-filtration process integrates physical separation and chemical oxidation, offering a highly efficient water purification strategy. However, the oxidation-filtration process is limited in practical applications due to the short residence time of milliseconds within the catalytic layer and the interference of coexisting organic pollutants in real water. Herein, a dual-layer membrane containing a top selective layer and a bottom catalytic layer was fabricated using an in situ co-casting method with a double-blade knife. Experimental results demonstrated that the selective layer rejected macromolecular organic pollutants, thereby alleviating their interference with bisphenol A (BPA) degradation. Concurrently, the catalytic layer activated peracetic acid oxidant and achieved a high BPA degradation exceeding 90 % in milliseconds with reactive oxygen species (especially •OH). The finite-element analysis confirmed a high-concentration reaction field occupying the pore cavity of the catalytic layer, enhancing collision probability between reactive oxygen species and BPA, i.e., the nano-confinement effect. Additionally, the dual-layer membrane achieved a long-term stable performance for emerging contaminant degradation in surface water treatment. This work underscores a novel catalytic membrane structure design for high-performance oxidation-filtration processes and elucidates its mechanisms underlying ultrafast degradation.

The dissolved organic matter (DOM) derived from microplastics (MPs-DOM) can be one of the photoactive components in DOM. However, information on the properties and photoreactivity of MPs-DOM during phototransformation is limited. Here, we investigated the properties and photoreactivity of MPs-DOM from polyolefins (MPs-DOM-POs), MPs-DOM derived from benzene-containing polymers (MPs-DOM-BCPs), and Suwannee River natural organic matter (SR-NOM), during a 168-hour phototransformation. After phototransformation, all examined types of DOM exhibit a decrease in concentration and molecular weight. Notably, MPs-DOM-POs display increased aromaticity and saturation, while MPs-DOM-BCPs and SR-NOM show reduced aromaticity and saturation. MPs-DOM-POs present higher steady-state concentrations of •OH but much lower steady-state concentrations of ¹O₂ than those of MPs-DOM-BCPs. In comparison, MPs-DOM produce more •OH but less ¹O₂ than SR-NOM. This study proposes that the diversification of aliphatic C─H bonds (arylation and carbonylation) by reactive intermediates (especially •OH) is the main pathway for MPs-DOM-POs phototransformation for the first time. On the other hand, the cleavage on the aromatic carboxylic acids by reactive intermediates (especially ¹O₂) is the main mechanism for MPs-DOM-BCPs and SR-NOM phototransformation. Our findings provide new insights into the phototransformation and photoreactivity of MPs-DOM and help to understand the potential risks of MPs in aqueous environment.

It has been reported that tripolyphosphate (TPP) can effectively enhance the activation of O₂ by Fe(II) to remove organic pollutants in the environment. However, the influence of solution pH on the generation and conversion of reactive oxygen species (ROS) and their degradation of pollutants in the Fe(II)/O₂/TPP system needs further investigation. In this study, we demonstrated that O₂^•- and •OH were the main ROS responsible for degradation in the system at different pH conditions, and their formation rates were calculated using a steady-state model. Experiments combined with density functional theory (DFT) calculations showed that the p-nitrophenol (PNP) degradation pathway in the Fe(II)/O₂/TPP system is regulated by solution pH. Specifically, at pH = 3, the existence of Fe(II) in the solution is dominated by [Fe(II)(HTPP)₂]^2-, which leads to a rapid conversion from O₂ and HO₂• to generate •OH, and PNP is primarily oxidatively degraded. However, at pH = 5/7, [Fe(II)(TPP)₂]^4- is taking the lead with which O₂^•- is accumulated in the solution due to the slow conversion to •OH in this condition, and the PNP is mainly reductively degraded. This study proposes a new strategy to achieve the targeted oxidative/reductive removal of different types of pollutants by simply varying the solution pH in the Fe(II)/O₂/TPP system.

The presence of pathogenic bacteria and antibiotic resistance genes (ARGs) in urban air poses a significant threat to public health. While prevailing research predominantly focuses on the airborne transmission of ARGs by bacteria, the potential influence of other vectors, such as bacteriophages, is often overlooked. This study aims to investigate the characteristics of phages and ARGs in aerosols originating from hospitals, public transit centers, wastewater treatment plants, and landfill sites. The average abundance of ARGs carried by phages in the public transit centers was 8.81 ppm, which was 2 to 3 times higher than that at the other three sites. Additionally, the abundance of ARGs across different risk levels at this site was also significantly higher than at the other three sites. The assembled phage communities bearing ARGs in public transit centers are chiefly governed by homogeneous selection processes, likely influenced by human movement. Furthermore, observations at public transit sites revealed that the average abundance ratio of virulent phages to their hosts was 1.01, and the correlation coefficient between their auxiliary metabolic genes and hosts' metabolic genes was 0.59, which were 20 times and 3 times higher, respectively, than those of temperate phages. This suggests that virulent phages may enhance their survival by altering host metabolism, thereby aiding the dispersion of ARGs and bacterial resistance. These revelations furnish fresh insights into phage-mediated ARG transmission, offering scientific substantiation for strategies aimed at preventing and controlling resistance within aerosols.

Antibiotic resistance is currently an unfolding global crisis threatening human health worldwide. While antibiotic resistance genes (ARGs) are known to be pervasive in environmental media, the occurrence of antibiotic resistance at interfaces between two or more adjacent media is largely unknown. Here, we designed a microcosm study to simulate plastic pollution in paddy soil and used a novel method, stimulated Raman scattering coupled with deuterium oxide (D₂O) labelling, to compare the antibiotic resistance in a single medium with that at the interface of multiple environmental media (plastic, soil, water). Results revealed that the involvement of more types of environmental media at interfaces led to a higher proportion of active resistant bacteria. Genotypic analysis showed that ARGs (especially high-risk ARGs) and mobile genetic elements (MGEs) were all highly enriched at the interfaces. This enrichment was further enhanced by the co-stress of heavy metal (arsenic) and antibiotic (ciprofloxacin). Our study is the first to apply stimulated Raman scattering to elucidate antibiotic resistance at environmental interfaces and reveals novel pathway of antibiotic resistance dissemination in the environment and overlooked risks to human health.

Plastic products offer remarkable convenience for modern life. However, growing concerns are emerging regarding the potential health hazards posed by nanoplastics, which formed as plastics break down. Currently, the biological effects and mechanisms induced by nanoplastics are largely underexplored. In this study, we report that polystyrene nanoplastics can enter the bloodstream and enhance thrombus formation. Our findings show that polystyrene nanoplastics adsorb plasma proteins, particularly coagulation factor XII and plasminogen activator inhibitor-1, play a key role in this process, as demonstrated by proteomics, bioinformatic analyses, and molecular dynamics simulations. The adsorption of these proteins by nanoplastics is an essential factor in thrombosis enhancement. This newly uncovered pathway of protein adsorption leading to enhanced thrombosis provides new insights into the biological effects of nanoplastics, which may inform future safety and environmental risk assessment of plastics.