Experiments were conducted to measure biodegradation of polychlorinated biphenyl (PCB) congeners contained in mixture Aroclor 1248 and congeners present in wastewater lagoon sediment contaminated decades earlier at Altavista, Virginia. A well-characterized strain of aerobic PCB-degrading bacteria, Paraburkholderia xenovorans LB400 was incubated in laboratory bioreactors with PCB-contaminated sediment collected at the site. The experiments evaluated strain LB400’s ability to degrade PCBs in absence of sediment and in PCB-contaminated sediment slurry. In absence of sediment, LB400 transformed 76% of Aroclor 1248 within seven days, spanning all homolog groups present in the mixture. In sediment slurry, only mono- and di-chlorinated PCB congeners were transformed. These results show that LB400 is capable of rapidly biodegrading most PCB congeners when they are freely dissolved in liquid but cannot degrade PCB congeners having three or more chlorine substituents in sediment slurry. Finally, using GC/MS-MS triple quadrupole spectrometry, this work distinguishes between physical (sorption to cells) and biological removal mechanisms, illuminates the process by which microorganisms with LB400-type congener specificity can selectively transform lower-chlorinated congeners over time, and makes direct comparisons to other studies where individual congener data is reported.

Chlorinated paraffins (CPs) are pervasive environmental pollutants which have been reported to be hepatotoxic by laboratory cell and animal studies. However, the related epidemiological reports on their hepatotoxic effects to humans are sparse. In this study, we evaluated the associations between six liver enzymes and serum short-chain CP (SCCP) or medium-chain CP (MCCP) concentrations of 197 residents in Jinan, China. Serum S/MCCPs were detected by quadrupole time-of-flight high-resolution mass spectrometry coupled with atmospheric pressure chemical ionization source (APCI-QTOF-HRMS), and quantified by pattern deconvolution method. The associations between total serum S/MCCP concentrations (ΣS/MCCPs) and continuous liver enzyme levels were assessed by linear regression. Odds ratios (ORs) for the effects of serum ΣS/MCCPs concentrations on liver function biomarkers dichotomized by clinical reference intervals were predicted by logistic regression, either treating ΣS/MCCPs as continuous or categorical dependents. After multivariable adjustment, linear regression results illustrated that 1-ln unit increase in serum ΣSCCPs was negatively associated with male PA levels [-6.08, 95% confidence interval (CI): −11.90, −3.25, p < 0.05], positively associated with male TB levels (1.80, 95% CI: 0.28, 3.31, p < 0.05), and positively associated with female AST levels (1.39, 95% CI: 0.07, 2.70, p < 0.05). One-ln unit increase in serum ΣMCCPs was negatively associated male PA levels (−7.56, 95% CI: −17.15, −4.03, p < 0.05). Logistic regression results suggested that male serum ΣSCCPs were associated with increased prevalence of abnormal PA (OR = 1.47 per 1 ln-unit increase, CI = 1.18, 1.82) and TB (OR = 1.75, 95% CI = 1.12, 2.76) levels, and male serum ΣMCCPs were significantly associated with increased prevalence of abnormal PA (OR = 1.43, 95% CI = 1.03, 1.97) levels. In addition, male participants with concentrations above the median ΣS/MCCPs were associated with increased risk for abnormal PA levels [SCCPs, 2.11-fold (95% CI = 1.15, 3.87); MCCPs, 1.94-fold (95% CI = 1.24, 3.03)]. Male participants with concentrations above the median ΣSCCPs were also associated with increased risk for abnormal TB levels (OR = 1.75, 95% CI = 1.12, 2.76). Conclusively, our results revealed that CP internal exposure was associated with disturbed liver biomarker levels, suggesting the hepatotoxicity of both SCCPs and MCCPs to humans.

It remains unclear how the source and rate of nitrogen (N) fertilizers affect N₂O concentration and effluxes along the soil profile under the drip-fertigated agricultural system. A plot-based field study was performed in 2017 and 2018 in a cotton field in arid northwestern China, with an objective to elucidate the impact of the applications of conventional urea (Urea), polymer-coated urea (ESN) and stabilized urea (SuperU) at rates of 120 and 240 kg N ha⁻¹ on concentration and efflux of N₂O in the soil profile and its relationship with N₂O surface emissions. The in-situ N₂O concentrations at soil depths of 5, 15, 30 and 60 cm were measured and used to estimate soil profile N₂O effluxes. Estimates of surface N₂O flux using the concentration gradient-based (GM) were compared with those measured using the chamber-based (CM) method. In both years, soil N₂O concentrations at all depths increased in response to basal N application at planting or in-season fertigation events. However, N rate or source did not affect soil N₂O concentrations or effluxes at each depth. Surface emissions of N₂O were mostly associated with that presented in the top layer of 0–15 cm. Surface N₂O efflux determined by GM was poorly or not associated with those of chamber measurements, which was attributed to the low N₂O production restricted by soil moisture condition under the drip-fertigated condition. These results highlight the challenge of applying the enhanced efficiency N fertilizer products in the drip-fertigated agricultural system.

Rice has been confirmed as one of the principal intake pathways for methylmercury (MeHg) in human, however, the impact of edible organisms, such as snails, loaches and eels, living in the rice-based ecosystem to the overall MeHg intake has been overlooked. Here, we conducted a cross-sectional ecological study, and the results showed that bioaccumulation of MeHg in these edible organisms was significantly higher than in paddy soils and rice roots (p < 0.001), even though rice roots and grains have significantly higher total Hg (THg) (p < 0.001). The MeHg/THg ratios were consistently and significantly higher in those edible organisms than in rice grains, suggesting a potential elevated MeHg exposure risk through consumption. Based on results of bioaccumulation factors (BAFs) for MeHg, it was clear that MeHg was bioaccumulated and biotransformed from paddy soils to earthworms and then to eels, as well as from paddy soils to snails and then to eels and loaches, potentially indicating that the consumption of eels and loaches was absolutely pernicious to people regularly feeding on them. Overall, MeHg was biomagnified along the food chain of the paddy ecosystem from soil to the organisms, and it was of potential higher risks for local residents to eat them, especially eels and loaches. Therefore, it is intensely indispensable for people fond of such diets to attenuate their consumption of rice, eels and loaches, thus mitigating their MeHg exposure risks.

Cadmium (Cd) pollution in alkaline soil in some areas of northern China has seriously threatened wheat production and human health. However, there are still few effective amendments for alkaline soil, and the mechanism of amendments with a good immobilization effect remains unclear. In this study, soil sterilization experiments were conducted to investigate the effects of soil microorganisms on the immobilization of a novel amendment—mercapto palygorskite (MPAL) in Cd-contaminated alkaline soils. The results showed that the mercapto on the MPAL surface was not affected by autoclaving. Compared with the control, the available Cd concentration in 0.025% MPAL treatments decreased by 18.80-29.23% after 1 d of aging and stabled after 10 d of aging. Importantly, the immobilization of MPAL on Cd in sterilized soil was significantly better than that in natural soil due to the changes in Cd fractions. Compared with MPAL-treated natural soil, exchangeable Cd fraction and carbonate-bound Cd fraction in MPAL-treated sterilized soil decreased by 20.79–27.09% and 20.05–26.45%, while Fe/Mn oxide-bound Cd fraction and organic matter-bound Cd fraction increased by 17.77–22.68% and 18.85–27.32%. Phylogenetic investigation of communities by reconstruction of unobserved states (PICRUSt) analysis found that the potential functions of the microbial community in normal and sterilized soil were different significantly. Soil sterilization increased the soil pH and decreased the arylsulfatase activity, but did not change the soil zeta potential and available sulfur. The changes in Cd fractions in MPAL-treated sterilized soil may be related to the reduction in the bacterial community and the changes in function microbial, but not to the soil properties. In addition, MPAL application had little effects on the bacterial community, soil pH value, zeta potential, available sulfur, and arylsulfatase. These results showed that the immobilization of MPAL on Cd in alkaline soil was stable and effective, and was not affected by soil sterilization and soil microorganism reduction.

The binding of PAHs with DNA to form PAH-DNA adducts is a crucial step in PAH-induced carcinogenesis. How functional groups affect this binding is largely unknown. Here, we observed that functional group substitutions strongly inhibited PAH-DNA binding. Additionally, –OH substitution has the most potent inhibitory effect as it causes the smallest change in the electrostatic surface potential. Fourier transform infrared spectroscopy and molecular docking analyses demonstrated that PAH derivatives bind with guanine via intercalation and groove binding and then non-specifically insert into the major/minor grooves of DNA. Quantum chemical calculations suggested that hydrogen/halogen bonding may be essential in affecting the binding of functional group-substituted PAHs with DNA. It was further revealed that Log KOA and the PAH derivatives’ melting points correlated significantly with binding affinity, implying that changes in the physicochemical characteristics are important factors. This study opens a new window for understanding the relationship between highly toxic PAH derivatives and genetic materials.

Deamination is ubiquitous in nature and has important biological significance. Leucobacter triazinivorans JW-1, recently isolated from sludge, can rapidly degrade s-triazine herbicides. The responsible enzymes, however, have not been purified and characterized.Herein, we purified an amidohydrolase, i.e., N-isopropylammelide isopropylaminohydrolase (AtzC) from JW-1 cells by ammonium sulfate precipitation and three chromatography steps. The purified AtzC catalyzed amidohydrolysis of N-isopropylammelide to cyanuric acid. The optimal catalytic conditions of the purified AtzC were 42 °C and pH 7.0, and the Kₘ and Vₘₐₓ of AtzC was 0.811 mM and 28.19 mmol/min·mg. AtzC could catalyze amidohydrolysis of an N-alkyl substituent from dihydroxy s-triazines to cyanuric acid. Molecular docking and structural alignments were used to infer AtzC catalytic mechanism. The structural architecture of AtzC resembled that of cytosine deaminase in class III amidohydrolase, with a single Zn²⁺ coordinated by His and Asp. Interestingly, the AtzC lacks an acidic residue putatively to activate water for hydrolysis as compared to the other amidohydrolases. His253 in AtzC probably functions as a single general acid-base catalyst. These findings further enhance our understanding how aminohydrolases catalyze the metabolism of s-triazine herbicides.

Photodegradation is a major elimination route of many pharmaceutically active compounds (PhACs) in natural surface waters, yet their photolytic behavior in estuarine waters with salinity gradient change is largely unknown. Herein, sulfamethazine and carbamazepine were taken as representative PhACs to explore the photolytic kinetic differences in Qinzhou Bay estuarine water samples collected from upper to lower reaches. Rapid photodegradation of sulfamethazine was found in lower estuarine water relative to upstream estuarine water; whereas for carbamazepine, photolytic rate was inversely proportional to the salinity of estuarine waters. Experiments with extracted estuarine dissolved organic matter (E-DOM) imply that the multivariate effects of triplet-excited E-DOM (³E-DOM∗) and halide ions are responsible for the enhancement photolysis of sulfamethazine. Radical scavenging experiments suggest that the photolysis enhancement can be ascribed to the contribution of reactive halogen species (RHS), while their contribution to carbamazepine is negligible and ³E-DOM∗ is the dominant reactive species for its photodegradation. This indicates that the reactivity differences with RHS and ³DOM∗ affect the photolytic kinetics of PhACs from upper estuarine waters to lower reaches, which is also supported by a good linear relationship between the ratios of photolytic rates for ten PhACs in E-DOM solution with/without halides and the ratios of the reactivity of these pollutants with RHS and ³DOM∗. These findings show that the different reactivity of PhACs with ³E-DOM∗ and RHS influences the photolytic kinetics in estuarine waters with different salinity, and highlights the photochemical behavior of organic micropollutants from upstream to downstream estuarine waters.

Discarded micro/nano-plastic inputs into the environment are emerging global concerns. Yet the quantification of micro/nanoplastics in complex environmental matrices is still a major challenge, notably for soluble ones. We herein develop in-laboratory built nanostructures (zinc oxide, titanium oxide and cobalt) coupled to mass spectrometry techniques, for picogram quantification of micro/nanoplastics in water and snow matrices, without sample pre-treatment. In parallel, an ultra-trace quantification method for micro/nanoplastics based on nanostructured laser desorption/ionization time-of-flight mass spectrometry (NALDI-TOF-MS) is developed. The detection limit is ∼5 pg for ambient snow. Soluble polyethylene glycol and insoluble polyethylene fragments were observed and quantified in fresh falling snow in Montreal, Canada. Complementary physicochemical studies of the snow matrices and reference plastics using laser-based particle sizers, inductively coupled plasma tandem mass spectrometry, and high-resolution scanning/transmission electron microscopy, produced consistent results with NALDI, and further provided information on morphology and composition of the micro/nano-plastic particles. This work is promising as it demonstrates that a wide range of recyclable nanostructures, in-laboratory built or commercial, can provide ultra-trace capability for quantification for both soluble polymers and insoluble plastics in air, water and soil. It may thereby produce key missing information to determine the fate of micro/nanoplastics in the environment, and their impacts on human health.

Black carbon (BC) is the most potent light-absorbing component of particulate matter and can have a significant warming impact. On-road vehicles are a major source of BC and a significant contributor to global warming. This paper establishes an updated inventory to quantify the mitigation potential of efforts to control BC emissions from on-road transportation in China. The total emissions of BC from on-road vehicles in China were 152.1 thousand tons in 2017. Heavy-duty diesel fleets accounted for a large percentage of emissions, whereas light-duty gasoline fleets presented a gradually increasing trend of emissions. Historically, comprehensive control policies for on-road vehicle emissions have achieved substantial BC reductions, with a 45% decrease in 2017 compared to 2000. With the implementation of stringent control policies and the development of advanced control technologies, BC emissions from the on-road sector may have a greater reduction potential in the future. By 2035, three various future scenarios representing different stringency levels of emission controls will reduce BC emissions by 58%, 90%, and 93% relative to 2017. The major benefits in reducing BC emissions result from more stringent emission standards and the accelerated retirement of older heavy-duty diesel vehicles. The shorter lifetime of BC than that of CO₂ implies that the mitigation of BC emissions would offer an important opportunity to contribute to alleviating global warming in the short term. Our assessment reveals that in 2035, the most stringent scenario, Scenario PC3, could deliver a CO₂-equivalent emission reduction on a 20-year scale of 234.2 (GWP₂₀₋yᵣ) million tons compared with the NAP Scenario, which is equivalent to reducing the oil consumption in China’s transportation sector by nearly 20% from a climate impact perspective.