Polybrominated biphenyl ethers(PBDEs)and polycyclic aromatic hydrocarbons(PAHs)are commonly detected contaminants at e-waste recycling sites.Against the conventional wisdom that PBDEs and PAHs are highly immobile and ...Polybrominated biphenyl ethers(PBDEs)and polycyclic aromatic hydrocarbons(PAHs)are commonly detected contaminants at e-waste recycling sites.Against the conventional wisdom that PBDEs and PAHs are highly immobile and persist primarily in shallowsurface soils,increasing evidence shows that these compounds can leach into the groundwater.Herein,we compare the leachabilities of PBDEs vs.PAHs from contaminated soils collected at an e-waste recycling site in Tianjin,China.Considerable amounts of BDE-209(0.3–2 ng/L)and phenanthrene(42–106 ng/L),the most abundant PBDE and PAH at the site,are detected in the effluents of columns packed with contaminated soils,with the specific concentrations varying with hydrodynamic and solution chemistry conditions.Interestingly,the leaching potential of BDE-209 appears to be closely related to the release of colloidal mineral particles,whereas the leachability of phenanthrene correlates well with the concentration of dissolved organic carbon in the effluent,but showing essentially no correlation with the concentration of mineral particles.The surprisingly different trends of the leachability observed between BDE-209 and phenanthrene is counterintuitive,as PBDEs and PAHs often co-exist at e-waste recycling sites(particularly at the sites wherein incineration is being practiced)and share many similarities in terms of physicochemical properties.One possible explanation is that due to its extremely low solubility,BDE-209 predominantly exists in free-phase(i.e.,as solid(nano)particles),whereas the more soluble phenanthrene is mainly sorbed to soil organic matter.Findings in this study underscore the need to better understand the mobility of highly hydrophobic organic contaminants at contaminated sites for improved risk management.展开更多
The associations of polycyclic aromatic hydrocarbon(PAH)exposure with serum uric acid(SUA)or hyperuricemia have been rarely assessed.We aimed to investigate the relationships between urinary PAH metabolites and SUA or...The associations of polycyclic aromatic hydrocarbon(PAH)exposure with serum uric acid(SUA)or hyperuricemia have been rarely assessed.We aimed to investigate the relationships between urinary PAH metabolites and SUA or hyperuricemia among US adults and to explore the mediating role of systemic inflammation in the associations.A total of 10,307 US adults were conducted to assess the associations of seven urinary hydroxy–PAH with SUA and hyperuricemia and evaluate the role of C-reactive protein(CRP),a biomarker of systemic inflammation,in such associations.Results showed that each 1-unit increase in ln-transformed 2-hydroxynaphthalene(2-OHNa),1-hydroxyphenanthrene(1-OHPh),2&3-hydroxyphenanthrene(2&3-OHPh)and total hydroxyphenanthrene(OHPh)was associated with a 1.68(95%confidence interval(CI):0.19 to 3.17),2.46(0.78 to 4.13),3.34(1.59 to 5.09),and 2.99(1.23 to 4.75)μmol/L increase in SUA,and a 8%(odds ratio(OR):1.08,1.02 to 1.15),9%(OR:1.09,1.02 to 1.18),13%(OR:1.13,1.05 to 1.22),and 12%(OR:1.12,95%CI:1.03,1.21)increase in hyperuricemia,respectively.Co-exposure of seven PAHs was positively associated with SUA and hyperuricemia,with 2&3-OHPh showing the highest weight(components weights:0.83 and 0.78,respectively).The CRP mediated 11.47%and 10.44%of the associations ofΣOHPh and 2&3-OHPh with SUA and mediated 8.60%and 8.62%in associations ofΣOHPh and 2&3-OHPh with hyperuricemia,respectively.In conclusion,internal levels of PAH metabolites were associated with elevated SUA levels and the increased risk of hyperuricemia among US adults,and CRP played a mediating role in the associations.展开更多
This study investigated environmental distribution and human exposure of polycyclic aromatic hydrocarbons(PAHs)and their derivatives in one Chinese petroleum refinery facility.It was found that,following with high con...This study investigated environmental distribution and human exposure of polycyclic aromatic hydrocarbons(PAHs)and their derivatives in one Chinese petroleum refinery facility.It was found that,following with high concentrations of 16 EPA PAHs(∑Parent-PAHs)in smelting subarea of studied petroleum refinery facility,total derivatives of PAHs[named as XPAHs,including nitro PAHs(NPAHs),chlorinated PAHs(Cl-PAHs),and brominated PAHs(Br-PAHs)]in gas(mean=1.57×10^(4)ng/m^(3)),total suspended particulate(TSP)(mean=4.33×10^(3) ng/m^(3))and soil(mean=4.37×10^(3) ng/g)in this subarea had 1.76-6.19 times higher levels than those from other subareas of this facility,surrounding residential areas and reference areas,indicating that petroleum refining processes would lead apparent derivation of PAHs.Especially,compared with those in residential and reference areas,gas samples in the petrochemical areas had higher∑NPAH/∑PAHs(mean=2.18),but lower∑Cl-PAH/∑PAHs(mean=1.43×10^(-1))and∑Br-PAH/∑PAHs ratios(mean=7.49×10^(-2)),indicating the richer nitrification of PAHs than chlorination during petrochemical process.The occupational exposure to PAHs and XPAHs in this petroleum refinery facility were 24-343 times higher than non-occupational exposure,and the ILCR(1.04×10^(-4))for petrochemical workers was considered to be potential high risk.Furthermore,one expanded high-resolution screening through GC Orbitrap/MS was performed for soils from petrochemical area,and another 35 PAHs were found,including alkyl-PAHs,phenyl-PAHs and other species,indicat-ing that profiles and risks of PAHs analogs in petrochemical areas deserve further expanded investigation.展开更多
Polycyclic aromatic hydrocarbons(PAHs)are of great concern because they threaten pri-mary productivity,but their specific effects on ecosystem functioning are scarce,hindering a comprehensive understanding of their ec...Polycyclic aromatic hydrocarbons(PAHs)are of great concern because they threaten pri-mary productivity,but their specific effects on ecosystem functioning are scarce,hindering a comprehensive understanding of their ecological risks,especially in eutrophicwaters.The present study was conducted by adding PAHs to four marine phytoplankton species and showed that naphthalene(Nap)and phenanthrene(Phe)induced both stimulatory and in-hibitory effects(>50%)on urea and NO_(3)−uptake by phytoplankton species.In addition,the apparent stimulative effects(>50%)for NH_(4)^(+)were also observed.Overall,38.9%of the sam-ples exhibited stimulation effects after 24 h exposure,which increased to 61.1%after 96 h exposure.This suggested the existence of a lag period,during which a tolerant cell popula-tion could adapt to PAHs.Significant positive correlations(P<0.01)between low and high concentrations of PAH individuals demonstrated that the mode of action for both pollutants on nitrogen uptake by phytoplankton was the same.Species-specific responses were also observed,with 19.0%of Thalassiosira sp.and 24.0%of Tetraselmis sp.exhibited inhibition effects greater than 50%,while 40.9%of Karlodinium veneficum and 27.3%of Rhodomonas salina demonstrated stimulation effects exceeding 50%,providing a unique perspective for exploring the harmful algal bloom of the mixotrophic K.veneficum,in addition to the original consideration of nutrients.The internal mechanisms may lie in differences in energy consumption between N-forms,exposure time and chemical concentrations,aswell as mor-phological characteristics and biochemical structures of the species,which require further investigation.展开更多
Rhizoremediation has emerged as a burgeoning approach for the removal of petroleum hydrocarbons(PHCs)from soil,with a primary emphasis on terrestrial plant systems.However,the mechanism of how soil microbiomes influen...Rhizoremediation has emerged as a burgeoning approach for the removal of petroleum hydrocarbons(PHCs)from soil,with a primary emphasis on terrestrial plant systems.However,the mechanism of how soil microbiomes influence the dissipation of PHCs within a hygrophyte planting system has yet to be fully elucidated.This work concentrated on the potential evolution of soil microbiomes and their effects on PHC dissipation within the Suaeda salsa(L.)Pall.planting system in a pot experiment.Two representative compounds,polycyclic aromatic hydrocarbons(PAHs)and n-alkanes,were used as target PHCs.The findings revealed a significant efficiency in the dissipation of PHCs in soil with Suaeda salsa cultivation,particularly with respect to n-alkanes.The high dissipation efficiency of PHCs was the synergistic result of root accumulation and microbial biodegradation.The key microbes involved in PHC dissipation were revealed,with the dominant phylum Proteobacteria and genus Salinimicrobium.The alterations in microbial diversity and abundance were closely associated with root exudation and PHC exposure.Significant differences in enzyme activities,an indicator of soil health and fertility,were observed between the rhizospheric and non-rhizospheric soils,which was attributed to root exudation.This study offers novel insights into the phytoremediation potential for Suaeda in PHC-contaminated soils and serves as a valuable scientific reference for the phytoremediation of such soils.展开更多
Polycyclic compounds are widely found in natural products and drug molecules with important biological activities,which attracted the attention of many chemists.Phosphine-catalyzed nucleophilic addition is one of the ...Polycyclic compounds are widely found in natural products and drug molecules with important biological activities,which attracted the attention of many chemists.Phosphine-catalyzed nucleophilic addition is one of the most powerful tools for the construction of various cyclic compounds with the advantages of atom economy,mild reaction conditions and simplicity of operation.Allenolates,Morita−Baylis−Hillman(MBH)alcohols and their derivatives(MBHADs),electron-deficient olefins and alkynes are very efficient substrates in phosphine mediated annulations,which formed many phosphonium species such asβ-phosphonium enolates,β-phosphonium dienolates and vinyl phosphonium ylides as intermediates.This review describes the reactivities of these phosphonium zwitterions and summarizes the synthesis of polycycle compounds through phosphine-mediated intramolecular and intermolecular sequential annulations.Thus,a systematic summary of the research process based on the phosphine-mediated sequential annulations of allenolates,MBH alcohols and MBHADs,electron-deficient olefins and alkynes are presented in Chapters 2-6,respectively.展开更多
Hymoins A–C(1–3),three unusual polycyclic polyprenylated acylphloroglucinols(PPAPs)were isolated from the flowers of Hypericum monogynum.Hymoin A features the first intriguing 6/5/5/5/7 pentacyclic caged PPAP.Hymoin...Hymoins A–C(1–3),three unusual polycyclic polyprenylated acylphloroglucinols(PPAPs)were isolated from the flowers of Hypericum monogynum.Hymoin A features the first intriguing 6/5/5/5/7 pentacyclic caged PPAP.Hymoin B is characterized by an unprecedented rearranged 5/6/8 tricyclic ring system,while hymoin C represents the first rearranged PPAP with a fantastic spirocyclic 5/6/7 ring system.Their structures were established by extensive spectroscopic analysis,X-ray crystallography,and computational methods.The plausible biosynthetic routes for the compounds were also proposed.In oleic acid(OA)-induced HepG2 cells,all compounds exhibited significant lipid-lowering activity at the concentrations of 2–8μmol/L.Further mechanistic study implied that compound 1 exhibited excellent lipid-lowering activity in OA-induced HepG2 cells through inhibiting the proteins of free fatty acids synthesis and improving lipidolysis.展开更多
Size-fractionated particulate matter(PM_(2.5)and PM>_(2.5))was collected at a traffic site in Kanazawa,Japan in a seasonal sampling work in 2020.Nine polycyclic aromatic hydrocarbons(4-to 6-ring PAHs)were determine...Size-fractionated particulate matter(PM_(2.5)and PM>_(2.5))was collected at a traffic site in Kanazawa,Japan in a seasonal sampling work in 2020.Nine polycyclic aromatic hydrocarbons(4-to 6-ring PAHs)were determined in fine and coarse particles.The gas/particle partitioning coefficients(K_(p))of the PAHs were calculated from the supercooled liquid vapour pressure and octanol-air partitioning coefficient based on the relationships obtained in previous traffic pollution-related studies.Gaseous PAHs were estimated by K_(p) and the concentrations of PM and particulate PAHs.The concentrations of total PAHs were 32.5,320.1 and 5646.2 pg/m^(3) in the PM>_(2.5),PM_(2.5) and gas phases,respectively.Significant seasonal trends in PAHs were observed(particle phase:lowest in summer,gas phase:lowest in spring,particle and gas phase:lowest in spring).Compared to 2019,the total PAH concentrations(in particles)decreased in 2020,especially in spring and summer,which might be due to reduced traffic trips during the COVID-19 outbreak.The incremental lifetime cancer risk(ILCR)calculated from the toxic equivalent concentrations relative to benzo[a]pyrene(BaP_(eq))was lower than the acceptable limit issued by the US Environmental Protection Agency,indicating a low cancer risk in long-term exposure to current PAH levels.It is notable that gaseous PAHs considerably contributed to BaP_(eq) and ILCR(over 50%),which highlighted the significance of gaseous PAH monitoring for public health protection.This low-cost estimation method for gaseous PAHs can be expected to reliably and conveniently obtain PAH concentrations as a surrogate for traditional sampling in the future work.展开更多
Previous studies have reported a relationship between exposure to metals and polycyclic aromatic hydrocarbons(PAHs)and blood glucose levels,but whether the mechanisms are mediated by amino acids remains to be elucidat...Previous studies have reported a relationship between exposure to metals and polycyclic aromatic hydrocarbons(PAHs)and blood glucose levels,but whether the mechanisms are mediated by amino acids remains to be elucidated.We conducted a three-wave repeated measurement study involving 201 elderly individuals(aged≥50 years)from five communities in Beijing,China.We simultaneously measured eightmetals in both blood and urine,six monohydroxy PAHs in urine,and 23 amino acids in blood.Linear mixed-effects and sparse partial least squares models were used to evaluate the individual effects,and Bayesian kernel machine regression was employed to mixture effects.Mediation analysis was further used to explore whether amino acids mediators mediate the association.We observed significant associations of selenium and strontium with increased blood glucose.Additionally,blood copper,urinary nickel,as well as urinary 1+9 hydroxyphenanthrene,were associated with irregular blood glucose regulation.Moreover,we found that amino acids such as leucine,proline,and alanine may mediate the associations.This study is the first to investigate the effect of metals and PAHs on blood glucose homeostasis,while also exploring the mediating role of amino acids,offering new insights into the impact of metals and PAHs on blood glucose regulation.展开更多
Polycyclic aromatic hydrocarbons(PAHs)could be produced during the preparation of biochar,which may pose potential risks to the environment and human health.Existing research mainly focuses on the removal efficiency o...Polycyclic aromatic hydrocarbons(PAHs)could be produced during the preparation of biochar,which may pose potential risks to the environment and human health.Existing research mainly focuses on the removal efficiency of PAHs in biochar using different methods.Still,there are few reports on the removal mechanism of PAHs and the impact of treated biochar on plant growth.This study prepared biochar by pyrolysis of sewage sludge,pig manure,and distillers grains at 300,500,and 600℃,respectively.The prepared biochar was subjected to thermal treatment,water washing treatment,and hydrothermal treatment to investigate the removal mechanism of PAHs in biochar and evaluate its effect on plant growth.The results showed that the removal rates of PAHs in biochar by hydrothermal treatment,thermal treatment,and water washing were 36.79%-86.09%,80.00%-89.90%,and 19.15%-72.40%,respectively.Compared with thermal treatment and water washing treatments,the hydrothermal treatment is more effective.The removal rate of PAHs in sludge biochar with a pyrolysis temperature of 300℃ by hydrothermal treatment reached 86.09%under 80℃ for 2 h.The removal mechanisms of PAHs include weakening hydrophobic interaction and thermal desorption.The germination results indicate that treated biochar reduces malondialdehyde content in mung bean seedlings and increases superoxide dismutase,peroxidase,and catalase activities.Sludge biochar after hydrothermal treatment is more conducive to the growth of mung beans than pristine biochar.This study provides an effective pathway for the safe utilization of biochar.展开更多
Objective To investigate the association of various polycyclic aromatic hydrocarbon(PAH)metabolites with diverse subtypes of cardiovascular disease(CVD)risk.Methods A novel predicting risk of cardiovascular disease EV...Objective To investigate the association of various polycyclic aromatic hydrocarbon(PAH)metabolites with diverse subtypes of cardiovascular disease(CVD)risk.Methods A novel predicting risk of cardiovascular disease EVENTs PREVENT equation was used to estimate the 10-year diverse subtypes of CVD risk,and their associations with PAH metabolites were analyzed using multiple logistic regression models,the weighted quantile sum(WQS)model,the quantile g-computation(qgcomp)model,and a stratified analysis of subgroups.Results For this study,six thousand seven hundred and forty-five participants were selected,and significant positive associations were observed between PAHs,naphthalene(NAP),and fluorene(FLU),and the risks of total CVD,atherosclerotic cardiovascular disease(ASCVD),and heart failure(HF).NAP and FLU were the primary contributors to the effects of PAH mixtures,and their associations with total CVD,ASCVD,and HF risk were significant in younger participants(30≤age<50 years);however,the associations of phenanthrene(PHEN)with ASCVD,HF,coronary heart disease(CHD),and stroke were dominant in aging participants(age≥50 years).Notably,pyrene(PYR)was negatively associated with the risk of ASCVD,HF,CHD,and stroke.Similarly,negative associations of PYR with the four CVD subtypes were noticeable in aging participants.Conclusion Different PAHs metabolites had different impacts on each CVD subtype among different age groups.Notably,the protective effects of PYR on ASCVD,HF,CHD,and stroke were noticeable in aging individuals.展开更多
High-energy-density(HED)fuel(e.g.widely used JP-10 and RJ-4),featuring compact 3D polycyclic structure with high strain,is of critical importance for volume-limited military aircraft,since their high density and combu...High-energy-density(HED)fuel(e.g.widely used JP-10 and RJ-4),featuring compact 3D polycyclic structure with high strain,is of critical importance for volume-limited military aircraft,since their high density and combustion heat can provide more propulsion energy.To reduce the reliance on petroleum source,it is highly desirable to develop renewable alternatives for the production of strained polycyclic HED fuel,but which remains a big challenge because of the inaccessibility caused by the high strain,We herein demonstrate a three-step catalytic route towards highly strained C_(17)and C_(18)spirofuel with biomass feedstocks.The process includes catalytic aldol condensation of renewable cyclohexanone/cyclopentanone with benzaldehyde,catalytic spiro Diels-Alder(D-A)reaction of aldol adduct with isoprene,and catalytic hydrodeoxygenation.The key spiro D-A reaction is enabled by the catalysis of heterogeneous Lewis acidic ionic liquid.The chloroaluminate IL,formed by benign urea and AICl3,exhibits good catalytic performance and reusability for this step.An eventual hydrodeoxygenation(HDO)over Pd/C and H-Y produces strained tricyclic spirofuel with density>0.93 g/mL,combustion heat>41 MJ/L and freezing point<-40℃,which are better than the properties of tactical fuel RJ-4.Therefore,it is anticipated that the as-prepared renewable fuels have the potential to replace traditional petroleum-derived HED fuels.展开更多
Multiple active components in steel slags can optimize soil texture and catalyze the thermal desorption of refractory organic pollutants,especially polycyclic aromatic hydrocarbons(PAHs).In this study,a safety and ris...Multiple active components in steel slags can optimize soil texture and catalyze the thermal desorption of refractory organic pollutants,especially polycyclic aromatic hydrocarbons(PAHs).In this study,a safety and risk assessment was conducted on toxic metals present in collected steel slags,and the refining slag with a high content of free-CaO from the XG iron and steel plant(XGRS)was selected and used to regulate the plasticity index(PI)of clay soils.For the clay soil with high liquid limit and high plasticity(CH),the PI reduced from 34.3%to 24.8%with steel slags at an addition ratio of 10%(mass percent),and for the clay soil with low liquid limit(CL),the PI decreased from 22.8%to 16.5%,resulting in silt soil with optimal thermal properties.The thermal removal efficiency of PAHs in CH decreased from 81.9%to 74.0%at 350℃ as the soil water content increased from 0 to 150 g kg^(-1),due to the hydration and swelling of clay minerals and the heat loss associated with dehydroxylation and dehydration.The efficiency further decreased to 68.7%using 2%(mass percent)CaO as an additive due to the delayed dehydr(oxyl)ation of clay minerals and enhanced aromatization of soil organic matter.In contrast,addition of 2%high-content titania-bearing slag(HTBS)enhanced the removal efficiency of high-ring PAHs,with the efficiency increasing for 5-ring from 52.6%to 59.7%and for 6-ring from 76.6%to 81.8%.This is due to the presence of amorphous TiO_(2) and crystalline CaTiO_(3) in HTBS,which can degrade water to produce reactive oxygen species.The 2%XGRS addition facilitated the complete removal of PAHs by air-supplemented lattice oxygen,leading to the oxidation of C–C bonds in CH to C–O,C=O,and O–C=O functional groups.This study provides valuable insights into the use of additives to enhance the thermal remediation of PAH-contaminated clay soils via activating oxygen species and oxidizing C–C bonds in organo-mineral complexes within clay soils.展开更多
Anemia is still prevalent among low and middle-income countries,posing serious family and social burdens.However,scarce studies provided evidence for real-world exposure to polycyclic aromatic hydrocarbons(PAHs)and an...Anemia is still prevalent among low and middle-income countries,posing serious family and social burdens.However,scarce studies provided evidence for real-world exposure to polycyclic aromatic hydrocarbons(PAHs)and anemia among pregnant women,as well as involved biological mechanisms.So,we conducted this study including 1717 late pregnant women fromZunyi Birth Cohort and collected urine samples for PAHs metabolites detection.Logistic regression and restricted cubic spline regression were used to examine exposuredisease risks and dose-response relationships.We conducted Bayesian kernel machine regression,weighted quantile sum regression,and quantile g-computation regression to fit the joint impacts of multiple PAHs in the real-world scenario on hypocalcemia and anemia.Results showed single exposure to 2-OHNap,2-OHFlu,9-OHFlu,1-OHPhe,2-OHPhe,3-OHPhe,and 1-OHPyr(all P-trend<0.05)increased the risks of hypocalcemia and anemia.Moreover,PAHs mixture was significantly related to higher risks of hypocalcemia and anemia,with 3-OHPhe and 1-OHPyr identified as their major drivers,respectively.Importantly,hypocalcemia served as a significant biological mechanism responsible for PAHs and anemia.Our findings suggest that individual and joint exposure to PAHs during late pregnancy elevate the anemia risk,and calcium supplementation might be a low-cost intervention target for reducing the PAHs-related impairment on anemia for pregnant women.展开更多
There have been reports of potential health risks for people from hydrophobic organic pollutants,such as polycyclic aromatic hydrocarbons(PAHs),polychlorinated hydrocarbons(PCHs),and organophosphate flame retardants(O...There have been reports of potential health risks for people from hydrophobic organic pollutants,such as polycyclic aromatic hydrocarbons(PAHs),polychlorinated hydrocarbons(PCHs),and organophosphate flame retardants(OPFRs).When a contaminated site is used for residential housing or public utility and recreation areas,the soil-bound organic pollutantsmight pose a threat to human health.In this study,we investigated the contamination profiles and potential risks to human health of 15 PAHs,6 PCHs,and 12 OPFRs in soils from four contaminated sites in China.We used an in vitro method to determine the oral bioaccessibility of soil pollutants.Total PAHswere found at concentrations ranging from26.4 ng/g to 987 ng/g.PCHs(0.27-14.3 ng/g)and OPFRs(6.30-310 ng/g)were detected,but at low levels compared to earlier reports.The levels of PAHs,PCHs,and OPFRs released from contaminated soils into simulated gastrointestinal fluids ranged from 1.74%to 91.0%,2.51%to 39.6%,and 1.37%to 96.9%,respectively.Based on both spiked and unspiked samples,we found that the oral bioaccessibility of pollutantswas correlated with their logKow andmolecularweight,and the total organic carbon content and pH of soils.PAHs in 13 out of 38 contaminated soil samples posed potential high risks to children.When considering oral bioaccessibility,nine soils still posed potential risks,while the risks in the remaining soils became negligible.The contribution of this paper is that it corrects the health risk of soil-bound organic pollutants by detecting bioaccessibility in actual soils from different contaminated sites.展开更多
The Yellow River Delta(YRD)is rich in oil,natural gas,and land resources.With the expansion of an important oil production base in North China,the increased discharge of Polycyclic aromatic hydrocarbons(PAHs)and alkyl...The Yellow River Delta(YRD)is rich in oil,natural gas,and land resources.With the expansion of an important oil production base in North China,the increased discharge of Polycyclic aromatic hydrocarbons(PAHs)and alkylated/nitrated/oxygenated PAHs(APAHs/NPAHs/OPAHs)into the Yellow River poses a potential risk to the aquatic ecosystem and human health.A total of 42 samples were gathered from trunk streams and tributaries within the YRD region during the wet and dry seasons,and 19 PAHs,5 APAHs,16 NPAHs,and 7 OPAHswere measured.The concentrations of ƩPAHs,ƩAPAHs,ƩNPAHs and ƩOPAHs ranged between 29 and 620 ng/L,6.9–81 ng/L,0.64–9.0 ng/L,and 7.2–81 ng/L in water,respectively,and 27–420 ng/g,5.1–130 ng/g,0.19–1.8 ng/g and 3.9–51 ng/g in sediment,respectively.The oil extraction activities resulted in an increased presence of middle-high molecular weight PAHs and APAHs in sediment,and port activities had a notable influence on the proportion of 1-methylpyrene in both water and sediment.The fugacity fraction analysis suggested that sediment was a secondary source of OPAHs,while benzo[k]fluoranthene,benzo[e]pyrene,benzo[a]pyrene,and 5-methylchrysene migrated from water to sediment.The main contributors to PAHs,APAHs,NPAHs,and OPAHs in water and sediment were combustion and petroleum sources.Compared to water,sediment displayed a heightened ecological risk associated with PAHs,APAHs,NPAHs,and OPAHs.Adults residing in the YRD region were at higher risk of cancer than children,which deserves special attention.展开更多
Objective Exposure to polycyclic aromatic hydrocarbons(PAHs)or metal(loid)s individually has been associated with neural tube defects(NTDs).However,the impacts of PAH and metal(loid)co-exposure and potential interacti...Objective Exposure to polycyclic aromatic hydrocarbons(PAHs)or metal(loid)s individually has been associated with neural tube defects(NTDs).However,the impacts of PAH and metal(loid)co-exposure and potential interaction effects on NTD risk remain unclear.We conducted a case-control study in China among population with a high prevalence of NTDs to investigate the combined effects of PAH and metal(loid)exposures on the risk of NTD.Methods Cases included 80 women who gave birth to offspring with NTDs,whereas controls were 50 women who delivered infants with no congenital malformations.We analyzed the levels of placental PAHs using gas chromatography and mass spectrometry,PAH-DNA adducts with 32P-post-labeling method,and metal(loid)s with an inductively coupled plasma mass spectrometer.Unconditional logistic regression was employed to estimate the associations between individual exposures and NTDs.Least absolute shrinkage and selection operator(LASSO)penalized regression models were used to select a subset of exposures,while additive interaction models were used to identify interaction effects.Results In the single-exposure models,we found that eight PAHs,PAH-DNA adducts,and 28 metal(loid)s were associated with NTDs.Pyrene,selenium,molybdenum,cadmium,uranium,and rubidium were selected through LASSO regression and were statistically associated with NTDs in the multiple-exposure models.Women with high levels of pyrene and molybdenum or pyrene and selenium exhibited significantly increased risk of having offspring with NTDs,indicating that these combinations may have synergistic effects on the risk of NTDs.Conclusion Our findings suggest that individual PAHs and metal(loid)s,as well as their interactions,may be associated with the risk of NTDs,which warrants further investigation.展开更多
Hepatic ischemia/reperfusion injury(IRI)remains a critical complication contributing to graft dysfunction following liver surgery.As part of an ongoing search for hepatoprotective natural products,five previously unre...Hepatic ischemia/reperfusion injury(IRI)remains a critical complication contributing to graft dysfunction following liver surgery.As part of an ongoing search for hepatoprotective natural products,five previously unreported homoadamantane-type polycyclic polyprenylated acylphloroglucinols(PPAPs),named hyperhomanoons A-E(1-5),and one known analog,hypersampsone O(6),were isolated from Hypericum patulum.Among these,compound 6 demonstrated potent protective effects against CoCl_(2)-induced hypoxic injury in hepatocytes.Furthermore,in a murine model of hepatic IRI induced by vascular occlusion,pretreatment with 6 markedly alleviated liver damage and reduced hepatocyte apoptosis.This study is the first to identify PPAPs as promising scaffolds for the development of therapeutic agents targeting hepatic IRI,underscoring their potential as lead compounds in drug discovery efforts for ischemic liver diseases.展开更多
The concentrations of polycyclic aromatic hydrocarbons(PAHs),their sources and toxic equivalent(TEQ)in soil,suspended matter and bottom sediments in the Fatala River Basin ecosystem were obtained for the fi rst time t...The concentrations of polycyclic aromatic hydrocarbons(PAHs),their sources and toxic equivalent(TEQ)in soil,suspended matter and bottom sediments in the Fatala River Basin ecosystem were obtained for the fi rst time to our knowledge.Determination of 14 PAHs(ΣPAHs)was carried out using high-performance liquid chromatography.TheΣPAH content in soil ranged from 13 to 50,920(Me=820)ng/g.The composition of PAHs(high proportion of low-molecular-weight compounds and values of individual PAHs ratios)refl ected the signifi cant oil pollution of soil.Contaminated soil was localated in the central part of the Fatala River Basin.The median benzo(a)pyrene toxic equivalent of soil at the study site was 1.08(range,0.05 to 53.16)ngTEQ/g,showing generally low soil toxicity.TheΣPAH content in suspended matter was in the range of 33 to 1316(Me=309)ng/L.TheΣPAH content in bottom sediments ranged from 36 to 6943(Me=478)ng/L,corresponding to clean and moderately contaminated sediments.TheΣPAH content in bottom sediments depended on the anthropogenic impact on the Fatala River Basin territory and the bottom sediment features.Bottom sediments and suspended matter had a low toxic equivalent.展开更多
High molecular weight polycyclic aromatic hydrocarbons(HMW-PAHs)pose significant environmental challenges due to their complex structures and persistent toxicity,and are difficult to be degraded by bacteria.Fungi,howe...High molecular weight polycyclic aromatic hydrocarbons(HMW-PAHs)pose significant environmental challenges due to their complex structures and persistent toxicity,and are difficult to be degraded by bacteria.Fungi,however,possess the ability to overcome these challenges,primarily through various enzymes with broad substrate specificity,including cytochrome P450(CYP450),laccase,manganese peroxidase,lignin peroxidase.As a result,the development of efficient fungal strains capable of degrading HMW-PAHs is essential for advancing bioremediation strategies.In this study,Aspergillus fumigatus Z5 was isolated from a contaminated site and demonstrated a remarkable ability to degrade the highly recalcitrant benzo[a]pyrene,achieving a degradation rate of 75.43%.Transcriptomic analysis revealed significant upregulation of 34 CYP450 genes.Among these genes,CYP3A4(gene 8840)showed strong binding affinity for benzo[a]pyrene,as confirmed by molecular docking studies,indicating its key role in the biodegradable process.Furthermore,the metabolic network analysis showed that the electron transfer required for CYP450-mediated oxidative reactions enhanced mitochondrial oxidative phosphorylation and subsequently energy metabolism in A.fumigatus Z5.This metabolic coordination likely facilitates the complete degradation of benzo[a]pyrene.Our study illuminates the fundamental roles of CYP450 from A.fumigatus Z5 in benzo[a]pyrene degradation and provides novel insight into designing and implementing enhanced bioremediation strategies.展开更多
基金supported by the National Key Research and Development Program of China(No.2019YFC1804202)the National Natural Science Foundation of China(Nos.22020102004 and 22125603)+1 种基金Tianjin Municipal Science and Technology Bureau(No.21JCZDJC00280)the Fundamental Research Funds for the Central Universities,and the Ministry of Education of China(No.T2017002).
文摘Polybrominated biphenyl ethers(PBDEs)and polycyclic aromatic hydrocarbons(PAHs)are commonly detected contaminants at e-waste recycling sites.Against the conventional wisdom that PBDEs and PAHs are highly immobile and persist primarily in shallowsurface soils,increasing evidence shows that these compounds can leach into the groundwater.Herein,we compare the leachabilities of PBDEs vs.PAHs from contaminated soils collected at an e-waste recycling site in Tianjin,China.Considerable amounts of BDE-209(0.3–2 ng/L)and phenanthrene(42–106 ng/L),the most abundant PBDE and PAH at the site,are detected in the effluents of columns packed with contaminated soils,with the specific concentrations varying with hydrodynamic and solution chemistry conditions.Interestingly,the leaching potential of BDE-209 appears to be closely related to the release of colloidal mineral particles,whereas the leachability of phenanthrene correlates well with the concentration of dissolved organic carbon in the effluent,but showing essentially no correlation with the concentration of mineral particles.The surprisingly different trends of the leachability observed between BDE-209 and phenanthrene is counterintuitive,as PBDEs and PAHs often co-exist at e-waste recycling sites(particularly at the sites wherein incineration is being practiced)and share many similarities in terms of physicochemical properties.One possible explanation is that due to its extremely low solubility,BDE-209 predominantly exists in free-phase(i.e.,as solid(nano)particles),whereas the more soluble phenanthrene is mainly sorbed to soil organic matter.Findings in this study underscore the need to better understand the mobility of highly hydrophobic organic contaminants at contaminated sites for improved risk management.
基金supported by the Key Program of National Natural Science Foundation of China(No.82241088)the Natural Science Foundation of Hubei Province(No.2022CFB813).
文摘The associations of polycyclic aromatic hydrocarbon(PAH)exposure with serum uric acid(SUA)or hyperuricemia have been rarely assessed.We aimed to investigate the relationships between urinary PAH metabolites and SUA or hyperuricemia among US adults and to explore the mediating role of systemic inflammation in the associations.A total of 10,307 US adults were conducted to assess the associations of seven urinary hydroxy–PAH with SUA and hyperuricemia and evaluate the role of C-reactive protein(CRP),a biomarker of systemic inflammation,in such associations.Results showed that each 1-unit increase in ln-transformed 2-hydroxynaphthalene(2-OHNa),1-hydroxyphenanthrene(1-OHPh),2&3-hydroxyphenanthrene(2&3-OHPh)and total hydroxyphenanthrene(OHPh)was associated with a 1.68(95%confidence interval(CI):0.19 to 3.17),2.46(0.78 to 4.13),3.34(1.59 to 5.09),and 2.99(1.23 to 4.75)μmol/L increase in SUA,and a 8%(odds ratio(OR):1.08,1.02 to 1.15),9%(OR:1.09,1.02 to 1.18),13%(OR:1.13,1.05 to 1.22),and 12%(OR:1.12,95%CI:1.03,1.21)increase in hyperuricemia,respectively.Co-exposure of seven PAHs was positively associated with SUA and hyperuricemia,with 2&3-OHPh showing the highest weight(components weights:0.83 and 0.78,respectively).The CRP mediated 11.47%and 10.44%of the associations ofΣOHPh and 2&3-OHPh with SUA and mediated 8.60%and 8.62%in associations ofΣOHPh and 2&3-OHPh with hyperuricemia,respectively.In conclusion,internal levels of PAH metabolites were associated with elevated SUA levels and the increased risk of hyperuricemia among US adults,and CRP played a mediating role in the associations.
基金supported by the National Key Research and Development Program of China(No.2019YFC1804501)the National Natural Science Foundation of China(Nos.22036007 and 22122611)+1 种基金the Natural Science Foundation of Shandong Province(No.ZR2020ME228)the Introduction and Cultivation Plan for Young Innovative Talents of Colleges and Universities.
文摘This study investigated environmental distribution and human exposure of polycyclic aromatic hydrocarbons(PAHs)and their derivatives in one Chinese petroleum refinery facility.It was found that,following with high concentrations of 16 EPA PAHs(∑Parent-PAHs)in smelting subarea of studied petroleum refinery facility,total derivatives of PAHs[named as XPAHs,including nitro PAHs(NPAHs),chlorinated PAHs(Cl-PAHs),and brominated PAHs(Br-PAHs)]in gas(mean=1.57×10^(4)ng/m^(3)),total suspended particulate(TSP)(mean=4.33×10^(3) ng/m^(3))and soil(mean=4.37×10^(3) ng/g)in this subarea had 1.76-6.19 times higher levels than those from other subareas of this facility,surrounding residential areas and reference areas,indicating that petroleum refining processes would lead apparent derivation of PAHs.Especially,compared with those in residential and reference areas,gas samples in the petrochemical areas had higher∑NPAH/∑PAHs(mean=2.18),but lower∑Cl-PAH/∑PAHs(mean=1.43×10^(-1))and∑Br-PAH/∑PAHs ratios(mean=7.49×10^(-2)),indicating the richer nitrification of PAHs than chlorination during petrochemical process.The occupational exposure to PAHs and XPAHs in this petroleum refinery facility were 24-343 times higher than non-occupational exposure,and the ILCR(1.04×10^(-4))for petrochemical workers was considered to be potential high risk.Furthermore,one expanded high-resolution screening through GC Orbitrap/MS was performed for soils from petrochemical area,and another 35 PAHs were found,including alkyl-PAHs,phenyl-PAHs and other species,indicat-ing that profiles and risks of PAHs analogs in petrochemical areas deserve further expanded investigation.
基金supported by the National Natural Science Foundation of China(No.42277404)the State Environmental Protection Key Laboratory of Aquatic Ecosystem Health in the Middle and Lower Reaches of Yangtze River(No.AEHKF2023004)+2 种基金the National Key Research and Development Programof China(No.2022YFC3202703)the International Collaboration Program of Chinese Academy of Sciences(Nos.SAJC202403,067GJHZ2023034MI)the Autonomous Deployment Project of Key Laboratory of Lake andWatershed Science for Water Security(No.NKL2023-KP01).
文摘Polycyclic aromatic hydrocarbons(PAHs)are of great concern because they threaten pri-mary productivity,but their specific effects on ecosystem functioning are scarce,hindering a comprehensive understanding of their ecological risks,especially in eutrophicwaters.The present study was conducted by adding PAHs to four marine phytoplankton species and showed that naphthalene(Nap)and phenanthrene(Phe)induced both stimulatory and in-hibitory effects(>50%)on urea and NO_(3)−uptake by phytoplankton species.In addition,the apparent stimulative effects(>50%)for NH_(4)^(+)were also observed.Overall,38.9%of the sam-ples exhibited stimulation effects after 24 h exposure,which increased to 61.1%after 96 h exposure.This suggested the existence of a lag period,during which a tolerant cell popula-tion could adapt to PAHs.Significant positive correlations(P<0.01)between low and high concentrations of PAH individuals demonstrated that the mode of action for both pollutants on nitrogen uptake by phytoplankton was the same.Species-specific responses were also observed,with 19.0%of Thalassiosira sp.and 24.0%of Tetraselmis sp.exhibited inhibition effects greater than 50%,while 40.9%of Karlodinium veneficum and 27.3%of Rhodomonas salina demonstrated stimulation effects exceeding 50%,providing a unique perspective for exploring the harmful algal bloom of the mixotrophic K.veneficum,in addition to the original consideration of nutrients.The internal mechanisms may lie in differences in energy consumption between N-forms,exposure time and chemical concentrations,aswell as mor-phological characteristics and biochemical structures of the species,which require further investigation.
基金financially supported by the National Natural Science Foundation of China(Nos.22176025 and 22136007)the National Key Research and Development Program of China(No.2022YFC3701404)the Petro China Innovation Foundation(No.D2019-5007-0502)。
文摘Rhizoremediation has emerged as a burgeoning approach for the removal of petroleum hydrocarbons(PHCs)from soil,with a primary emphasis on terrestrial plant systems.However,the mechanism of how soil microbiomes influence the dissipation of PHCs within a hygrophyte planting system has yet to be fully elucidated.This work concentrated on the potential evolution of soil microbiomes and their effects on PHC dissipation within the Suaeda salsa(L.)Pall.planting system in a pot experiment.Two representative compounds,polycyclic aromatic hydrocarbons(PAHs)and n-alkanes,were used as target PHCs.The findings revealed a significant efficiency in the dissipation of PHCs in soil with Suaeda salsa cultivation,particularly with respect to n-alkanes.The high dissipation efficiency of PHCs was the synergistic result of root accumulation and microbial biodegradation.The key microbes involved in PHC dissipation were revealed,with the dominant phylum Proteobacteria and genus Salinimicrobium.The alterations in microbial diversity and abundance were closely associated with root exudation and PHC exposure.Significant differences in enzyme activities,an indicator of soil health and fertility,were observed between the rhizospheric and non-rhizospheric soils,which was attributed to root exudation.This study offers novel insights into the phytoremediation potential for Suaeda in PHC-contaminated soils and serves as a valuable scientific reference for the phytoremediation of such soils.
基金the National Natural Science Foundation of China(Nos.22171147 and 21871148)for the financial support。
文摘Polycyclic compounds are widely found in natural products and drug molecules with important biological activities,which attracted the attention of many chemists.Phosphine-catalyzed nucleophilic addition is one of the most powerful tools for the construction of various cyclic compounds with the advantages of atom economy,mild reaction conditions and simplicity of operation.Allenolates,Morita−Baylis−Hillman(MBH)alcohols and their derivatives(MBHADs),electron-deficient olefins and alkynes are very efficient substrates in phosphine mediated annulations,which formed many phosphonium species such asβ-phosphonium enolates,β-phosphonium dienolates and vinyl phosphonium ylides as intermediates.This review describes the reactivities of these phosphonium zwitterions and summarizes the synthesis of polycycle compounds through phosphine-mediated intramolecular and intermolecular sequential annulations.Thus,a systematic summary of the research process based on the phosphine-mediated sequential annulations of allenolates,MBH alcohols and MBHADs,electron-deficient olefins and alkynes are presented in Chapters 2-6,respectively.
基金financially supported by the National Natural Science Foundation of China(Nos.32270413,82060631,82160808,and 82360035)the Science and Technology Department of Guizhou Province(Nos.QKHJC 2020–1Z076,QKHJC-ZK[2023]YB156,QKHJC-ZK[2021]YB569,and QKHPTRC[2020]5008)+4 种基金Excellent Young Talents Plan of Guizhou Medical University(2023,No.106)the 13thbatch of outstanding young scientific and technological talents in Guizhou Province(No.QKHPTRC[2021]5633)Guizhou Science and Technology Innovation Talent Team(No.QKHPTRC–CXTD[2022]007)High-level Innovative Talents in Guizhou Province(Thousand Levels of Talent for Chunmao Yuan in 2018)the project of State Key Laboratory of Functions and Applications of Medicinal Plants,Guizhou Medical University(Nos.FAMP202102K and QJJ[2023]113)。
文摘Hymoins A–C(1–3),three unusual polycyclic polyprenylated acylphloroglucinols(PPAPs)were isolated from the flowers of Hypericum monogynum.Hymoin A features the first intriguing 6/5/5/5/7 pentacyclic caged PPAP.Hymoin B is characterized by an unprecedented rearranged 5/6/8 tricyclic ring system,while hymoin C represents the first rearranged PPAP with a fantastic spirocyclic 5/6/7 ring system.Their structures were established by extensive spectroscopic analysis,X-ray crystallography,and computational methods.The plausible biosynthetic routes for the compounds were also proposed.In oleic acid(OA)-induced HepG2 cells,all compounds exhibited significant lipid-lowering activity at the concentrations of 2–8μmol/L.Further mechanistic study implied that compound 1 exhibited excellent lipid-lowering activity in OA-induced HepG2 cells through inhibiting the proteins of free fatty acids synthesis and improving lipidolysis.
基金supported by the Bilateral Open Partnership Joint Research Projects of the Japan Society for the Promotion of Science,Japan(No.JPJSBP120219914)the CHOZEN Project of Kanazawa University,Japan(2019)the Cooperative Research Programs of Institute of Nature and Environmental Technology,Kanazawa University,Japan(22002,22013,22007)。
文摘Size-fractionated particulate matter(PM_(2.5)and PM>_(2.5))was collected at a traffic site in Kanazawa,Japan in a seasonal sampling work in 2020.Nine polycyclic aromatic hydrocarbons(4-to 6-ring PAHs)were determined in fine and coarse particles.The gas/particle partitioning coefficients(K_(p))of the PAHs were calculated from the supercooled liquid vapour pressure and octanol-air partitioning coefficient based on the relationships obtained in previous traffic pollution-related studies.Gaseous PAHs were estimated by K_(p) and the concentrations of PM and particulate PAHs.The concentrations of total PAHs were 32.5,320.1 and 5646.2 pg/m^(3) in the PM>_(2.5),PM_(2.5) and gas phases,respectively.Significant seasonal trends in PAHs were observed(particle phase:lowest in summer,gas phase:lowest in spring,particle and gas phase:lowest in spring).Compared to 2019,the total PAH concentrations(in particles)decreased in 2020,especially in spring and summer,which might be due to reduced traffic trips during the COVID-19 outbreak.The incremental lifetime cancer risk(ILCR)calculated from the toxic equivalent concentrations relative to benzo[a]pyrene(BaP_(eq))was lower than the acceptable limit issued by the US Environmental Protection Agency,indicating a low cancer risk in long-term exposure to current PAH levels.It is notable that gaseous PAHs considerably contributed to BaP_(eq) and ILCR(over 50%),which highlighted the significance of gaseous PAH monitoring for public health protection.This low-cost estimation method for gaseous PAHs can be expected to reliably and conveniently obtain PAH concentrations as a surrogate for traditional sampling in the future work.
基金supported by the Noncommunicable Chronic Diseases-National Science and Technology Major Project(No.2023ZD0513200)the National Natural Science Foundation of China(Nos.82404278 and 82404365)China Postdoctoral Science Foundation(Nos.2023M730317 and 2023T160066).
文摘Previous studies have reported a relationship between exposure to metals and polycyclic aromatic hydrocarbons(PAHs)and blood glucose levels,but whether the mechanisms are mediated by amino acids remains to be elucidated.We conducted a three-wave repeated measurement study involving 201 elderly individuals(aged≥50 years)from five communities in Beijing,China.We simultaneously measured eightmetals in both blood and urine,six monohydroxy PAHs in urine,and 23 amino acids in blood.Linear mixed-effects and sparse partial least squares models were used to evaluate the individual effects,and Bayesian kernel machine regression was employed to mixture effects.Mediation analysis was further used to explore whether amino acids mediators mediate the association.We observed significant associations of selenium and strontium with increased blood glucose.Additionally,blood copper,urinary nickel,as well as urinary 1+9 hydroxyphenanthrene,were associated with irregular blood glucose regulation.Moreover,we found that amino acids such as leucine,proline,and alanine may mediate the associations.This study is the first to investigate the effect of metals and PAHs on blood glucose homeostasis,while also exploring the mediating role of amino acids,offering new insights into the impact of metals and PAHs on blood glucose regulation.
基金supported by the National Natural Science Foundation of China(No.41977297)the Special Fund for Outstanding Youth Talents of Science and Technology of Guizhou Province(No.YQK[2023]014)+1 种基金the Key Project of Science and Technology Department of Guizhou Province(No.ZK(2022)016)the Foreign Expert Project of the Ministry of Science and Technology(No.Y20240039)。
文摘Polycyclic aromatic hydrocarbons(PAHs)could be produced during the preparation of biochar,which may pose potential risks to the environment and human health.Existing research mainly focuses on the removal efficiency of PAHs in biochar using different methods.Still,there are few reports on the removal mechanism of PAHs and the impact of treated biochar on plant growth.This study prepared biochar by pyrolysis of sewage sludge,pig manure,and distillers grains at 300,500,and 600℃,respectively.The prepared biochar was subjected to thermal treatment,water washing treatment,and hydrothermal treatment to investigate the removal mechanism of PAHs in biochar and evaluate its effect on plant growth.The results showed that the removal rates of PAHs in biochar by hydrothermal treatment,thermal treatment,and water washing were 36.79%-86.09%,80.00%-89.90%,and 19.15%-72.40%,respectively.Compared with thermal treatment and water washing treatments,the hydrothermal treatment is more effective.The removal rate of PAHs in sludge biochar with a pyrolysis temperature of 300℃ by hydrothermal treatment reached 86.09%under 80℃ for 2 h.The removal mechanisms of PAHs include weakening hydrophobic interaction and thermal desorption.The germination results indicate that treated biochar reduces malondialdehyde content in mung bean seedlings and increases superoxide dismutase,peroxidase,and catalase activities.Sludge biochar after hydrothermal treatment is more conducive to the growth of mung beans than pristine biochar.This study provides an effective pathway for the safe utilization of biochar.
基金the technology projects entrusted by enterprises and institutions(2022KJ000803)the Beijing Natural Science Foundation(No.7242184)the project that Study on the role of ASGR1 in regulating chaperone mediated autophagy involved in methyl tert-butyl ether–induced hepatic lipotoxicity(XSKY2024).
文摘Objective To investigate the association of various polycyclic aromatic hydrocarbon(PAH)metabolites with diverse subtypes of cardiovascular disease(CVD)risk.Methods A novel predicting risk of cardiovascular disease EVENTs PREVENT equation was used to estimate the 10-year diverse subtypes of CVD risk,and their associations with PAH metabolites were analyzed using multiple logistic regression models,the weighted quantile sum(WQS)model,the quantile g-computation(qgcomp)model,and a stratified analysis of subgroups.Results For this study,six thousand seven hundred and forty-five participants were selected,and significant positive associations were observed between PAHs,naphthalene(NAP),and fluorene(FLU),and the risks of total CVD,atherosclerotic cardiovascular disease(ASCVD),and heart failure(HF).NAP and FLU were the primary contributors to the effects of PAH mixtures,and their associations with total CVD,ASCVD,and HF risk were significant in younger participants(30≤age<50 years);however,the associations of phenanthrene(PHEN)with ASCVD,HF,coronary heart disease(CHD),and stroke were dominant in aging participants(age≥50 years).Notably,pyrene(PYR)was negatively associated with the risk of ASCVD,HF,CHD,and stroke.Similarly,negative associations of PYR with the four CVD subtypes were noticeable in aging participants.Conclusion Different PAHs metabolites had different impacts on each CVD subtype among different age groups.Notably,the protective effects of PYR on ASCVD,HF,CHD,and stroke were noticeable in aging individuals.
基金supported by the Fundamental Research Funds for the Central Universities(2023QN1009)Xuzhou Basic Research Project(KC23018)+1 种基金China University of Mining and Technology(CUMT)Open Sharing Fund for Large-scale Instruments and Equipment(DYGX-2024-34)Priority Academic Program Development of Jiangsu Higher Education Institutions.
文摘High-energy-density(HED)fuel(e.g.widely used JP-10 and RJ-4),featuring compact 3D polycyclic structure with high strain,is of critical importance for volume-limited military aircraft,since their high density and combustion heat can provide more propulsion energy.To reduce the reliance on petroleum source,it is highly desirable to develop renewable alternatives for the production of strained polycyclic HED fuel,but which remains a big challenge because of the inaccessibility caused by the high strain,We herein demonstrate a three-step catalytic route towards highly strained C_(17)and C_(18)spirofuel with biomass feedstocks.The process includes catalytic aldol condensation of renewable cyclohexanone/cyclopentanone with benzaldehyde,catalytic spiro Diels-Alder(D-A)reaction of aldol adduct with isoprene,and catalytic hydrodeoxygenation.The key spiro D-A reaction is enabled by the catalysis of heterogeneous Lewis acidic ionic liquid.The chloroaluminate IL,formed by benign urea and AICl3,exhibits good catalytic performance and reusability for this step.An eventual hydrodeoxygenation(HDO)over Pd/C and H-Y produces strained tricyclic spirofuel with density>0.93 g/mL,combustion heat>41 MJ/L and freezing point<-40℃,which are better than the properties of tactical fuel RJ-4.Therefore,it is anticipated that the as-prepared renewable fuels have the potential to replace traditional petroleum-derived HED fuels.
基金sponsored by the National Key R&D Program of China(No.2018YFC1802101)the National Natural Science Foundation of China(No.52170149)。
文摘Multiple active components in steel slags can optimize soil texture and catalyze the thermal desorption of refractory organic pollutants,especially polycyclic aromatic hydrocarbons(PAHs).In this study,a safety and risk assessment was conducted on toxic metals present in collected steel slags,and the refining slag with a high content of free-CaO from the XG iron and steel plant(XGRS)was selected and used to regulate the plasticity index(PI)of clay soils.For the clay soil with high liquid limit and high plasticity(CH),the PI reduced from 34.3%to 24.8%with steel slags at an addition ratio of 10%(mass percent),and for the clay soil with low liquid limit(CL),the PI decreased from 22.8%to 16.5%,resulting in silt soil with optimal thermal properties.The thermal removal efficiency of PAHs in CH decreased from 81.9%to 74.0%at 350℃ as the soil water content increased from 0 to 150 g kg^(-1),due to the hydration and swelling of clay minerals and the heat loss associated with dehydroxylation and dehydration.The efficiency further decreased to 68.7%using 2%(mass percent)CaO as an additive due to the delayed dehydr(oxyl)ation of clay minerals and enhanced aromatization of soil organic matter.In contrast,addition of 2%high-content titania-bearing slag(HTBS)enhanced the removal efficiency of high-ring PAHs,with the efficiency increasing for 5-ring from 52.6%to 59.7%and for 6-ring from 76.6%to 81.8%.This is due to the presence of amorphous TiO_(2) and crystalline CaTiO_(3) in HTBS,which can degrade water to produce reactive oxygen species.The 2%XGRS addition facilitated the complete removal of PAHs by air-supplemented lattice oxygen,leading to the oxidation of C–C bonds in CH to C–O,C=O,and O–C=O functional groups.This study provides valuable insights into the use of additives to enhance the thermal remediation of PAH-contaminated clay soils via activating oxygen species and oxidizing C–C bonds in organo-mineral complexes within clay soils.
基金supported by the Science&Technology Program of Guizhou Province(Nos.QKHPTRC-GCC[2022]039-1,QKHPTRC-CXTD[2022]014,and QKHHBZ[2020]3002)the Scientific Research Programof Guizhou Provincial Department of Education(No.QJJ[2023]019).
文摘Anemia is still prevalent among low and middle-income countries,posing serious family and social burdens.However,scarce studies provided evidence for real-world exposure to polycyclic aromatic hydrocarbons(PAHs)and anemia among pregnant women,as well as involved biological mechanisms.So,we conducted this study including 1717 late pregnant women fromZunyi Birth Cohort and collected urine samples for PAHs metabolites detection.Logistic regression and restricted cubic spline regression were used to examine exposuredisease risks and dose-response relationships.We conducted Bayesian kernel machine regression,weighted quantile sum regression,and quantile g-computation regression to fit the joint impacts of multiple PAHs in the real-world scenario on hypocalcemia and anemia.Results showed single exposure to 2-OHNap,2-OHFlu,9-OHFlu,1-OHPhe,2-OHPhe,3-OHPhe,and 1-OHPyr(all P-trend<0.05)increased the risks of hypocalcemia and anemia.Moreover,PAHs mixture was significantly related to higher risks of hypocalcemia and anemia,with 3-OHPhe and 1-OHPyr identified as their major drivers,respectively.Importantly,hypocalcemia served as a significant biological mechanism responsible for PAHs and anemia.Our findings suggest that individual and joint exposure to PAHs during late pregnancy elevate the anemia risk,and calcium supplementation might be a low-cost intervention target for reducing the PAHs-related impairment on anemia for pregnant women.
基金supported by the National Key Research and Development Program of China(No.2019YFC1804604)Basic and Applied Basic Research Foundation of Guangdong Province(No.2021A1515010018).
文摘There have been reports of potential health risks for people from hydrophobic organic pollutants,such as polycyclic aromatic hydrocarbons(PAHs),polychlorinated hydrocarbons(PCHs),and organophosphate flame retardants(OPFRs).When a contaminated site is used for residential housing or public utility and recreation areas,the soil-bound organic pollutantsmight pose a threat to human health.In this study,we investigated the contamination profiles and potential risks to human health of 15 PAHs,6 PCHs,and 12 OPFRs in soils from four contaminated sites in China.We used an in vitro method to determine the oral bioaccessibility of soil pollutants.Total PAHswere found at concentrations ranging from26.4 ng/g to 987 ng/g.PCHs(0.27-14.3 ng/g)and OPFRs(6.30-310 ng/g)were detected,but at low levels compared to earlier reports.The levels of PAHs,PCHs,and OPFRs released from contaminated soils into simulated gastrointestinal fluids ranged from 1.74%to 91.0%,2.51%to 39.6%,and 1.37%to 96.9%,respectively.Based on both spiked and unspiked samples,we found that the oral bioaccessibility of pollutantswas correlated with their logKow andmolecularweight,and the total organic carbon content and pH of soils.PAHs in 13 out of 38 contaminated soil samples posed potential high risks to children.When considering oral bioaccessibility,nine soils still posed potential risks,while the risks in the remaining soils became negligible.The contribution of this paper is that it corrects the health risk of soil-bound organic pollutants by detecting bioaccessibility in actual soils from different contaminated sites.
基金supported by the Natural Science Foundation of Qingdao(No.23-2-1-224-zyyd-jch).
文摘The Yellow River Delta(YRD)is rich in oil,natural gas,and land resources.With the expansion of an important oil production base in North China,the increased discharge of Polycyclic aromatic hydrocarbons(PAHs)and alkylated/nitrated/oxygenated PAHs(APAHs/NPAHs/OPAHs)into the Yellow River poses a potential risk to the aquatic ecosystem and human health.A total of 42 samples were gathered from trunk streams and tributaries within the YRD region during the wet and dry seasons,and 19 PAHs,5 APAHs,16 NPAHs,and 7 OPAHswere measured.The concentrations of ƩPAHs,ƩAPAHs,ƩNPAHs and ƩOPAHs ranged between 29 and 620 ng/L,6.9–81 ng/L,0.64–9.0 ng/L,and 7.2–81 ng/L in water,respectively,and 27–420 ng/g,5.1–130 ng/g,0.19–1.8 ng/g and 3.9–51 ng/g in sediment,respectively.The oil extraction activities resulted in an increased presence of middle-high molecular weight PAHs and APAHs in sediment,and port activities had a notable influence on the proportion of 1-methylpyrene in both water and sediment.The fugacity fraction analysis suggested that sediment was a secondary source of OPAHs,while benzo[k]fluoranthene,benzo[e]pyrene,benzo[a]pyrene,and 5-methylchrysene migrated from water to sediment.The main contributors to PAHs,APAHs,NPAHs,and OPAHs in water and sediment were combustion and petroleum sources.Compared to water,sediment displayed a heightened ecological risk associated with PAHs,APAHs,NPAHs,and OPAHs.Adults residing in the YRD region were at higher risk of cancer than children,which deserves special attention.
基金supported by the National Key Research and Development Program,Ministry of Science and Technology of the People's Republic of China(Grant No.2021YFC2701001)the National Natural Science Foundation of China(Grant No.81973056).
文摘Objective Exposure to polycyclic aromatic hydrocarbons(PAHs)or metal(loid)s individually has been associated with neural tube defects(NTDs).However,the impacts of PAH and metal(loid)co-exposure and potential interaction effects on NTD risk remain unclear.We conducted a case-control study in China among population with a high prevalence of NTDs to investigate the combined effects of PAH and metal(loid)exposures on the risk of NTD.Methods Cases included 80 women who gave birth to offspring with NTDs,whereas controls were 50 women who delivered infants with no congenital malformations.We analyzed the levels of placental PAHs using gas chromatography and mass spectrometry,PAH-DNA adducts with 32P-post-labeling method,and metal(loid)s with an inductively coupled plasma mass spectrometer.Unconditional logistic regression was employed to estimate the associations between individual exposures and NTDs.Least absolute shrinkage and selection operator(LASSO)penalized regression models were used to select a subset of exposures,while additive interaction models were used to identify interaction effects.Results In the single-exposure models,we found that eight PAHs,PAH-DNA adducts,and 28 metal(loid)s were associated with NTDs.Pyrene,selenium,molybdenum,cadmium,uranium,and rubidium were selected through LASSO regression and were statistically associated with NTDs in the multiple-exposure models.Women with high levels of pyrene and molybdenum or pyrene and selenium exhibited significantly increased risk of having offspring with NTDs,indicating that these combinations may have synergistic effects on the risk of NTDs.Conclusion Our findings suggest that individual PAHs and metal(loid)s,as well as their interactions,may be associated with the risk of NTDs,which warrants further investigation.
基金supported by the National Natural Science Foundation for Distinguished Young Scholars(No.81725021)the National Natural Science Foundation of China(Nos.82003633 and 82173705)。
文摘Hepatic ischemia/reperfusion injury(IRI)remains a critical complication contributing to graft dysfunction following liver surgery.As part of an ongoing search for hepatoprotective natural products,five previously unreported homoadamantane-type polycyclic polyprenylated acylphloroglucinols(PPAPs),named hyperhomanoons A-E(1-5),and one known analog,hypersampsone O(6),were isolated from Hypericum patulum.Among these,compound 6 demonstrated potent protective effects against CoCl_(2)-induced hypoxic injury in hepatocytes.Furthermore,in a murine model of hepatic IRI induced by vascular occlusion,pretreatment with 6 markedly alleviated liver damage and reduced hepatocyte apoptosis.This study is the first to identify PPAPs as promising scaffolds for the development of therapeutic agents targeting hepatic IRI,underscoring their potential as lead compounds in drug discovery efforts for ischemic liver diseases.
基金support of the Project of the Russian Federation represented by the Ministry of Science and Higher Education of the Russian Federation:assistance in the form of grants in accordance with paragraph 4 of article 78.1 of the Budget Code of the Russian Federation(agreement No.075-15-2023-592 on subject No.13.2251.21.0216)CEREMAC-G own research fund and a Support special fi nancier of the Ministry of Higher Education,Scientifi c Research and Innovation(MESRSI)of the Republic of Guinea.
文摘The concentrations of polycyclic aromatic hydrocarbons(PAHs),their sources and toxic equivalent(TEQ)in soil,suspended matter and bottom sediments in the Fatala River Basin ecosystem were obtained for the fi rst time to our knowledge.Determination of 14 PAHs(ΣPAHs)was carried out using high-performance liquid chromatography.TheΣPAH content in soil ranged from 13 to 50,920(Me=820)ng/g.The composition of PAHs(high proportion of low-molecular-weight compounds and values of individual PAHs ratios)refl ected the signifi cant oil pollution of soil.Contaminated soil was localated in the central part of the Fatala River Basin.The median benzo(a)pyrene toxic equivalent of soil at the study site was 1.08(range,0.05 to 53.16)ngTEQ/g,showing generally low soil toxicity.TheΣPAH content in suspended matter was in the range of 33 to 1316(Me=309)ng/L.TheΣPAH content in bottom sediments ranged from 36 to 6943(Me=478)ng/L,corresponding to clean and moderately contaminated sediments.TheΣPAH content in bottom sediments depended on the anthropogenic impact on the Fatala River Basin territory and the bottom sediment features.Bottom sediments and suspended matter had a low toxic equivalent.
基金supported by the National Key R&D Program of China(No.2021YFC1808902)the National Natural Science Foundation of China(No.31770152)+1 种基金Shaanxi Fundamental Science Research Project for Chemistry&Biology(No.22JHZ008)the Natural Science Foundation of Gansu Province of China(No.23JRRM738).
文摘High molecular weight polycyclic aromatic hydrocarbons(HMW-PAHs)pose significant environmental challenges due to their complex structures and persistent toxicity,and are difficult to be degraded by bacteria.Fungi,however,possess the ability to overcome these challenges,primarily through various enzymes with broad substrate specificity,including cytochrome P450(CYP450),laccase,manganese peroxidase,lignin peroxidase.As a result,the development of efficient fungal strains capable of degrading HMW-PAHs is essential for advancing bioremediation strategies.In this study,Aspergillus fumigatus Z5 was isolated from a contaminated site and demonstrated a remarkable ability to degrade the highly recalcitrant benzo[a]pyrene,achieving a degradation rate of 75.43%.Transcriptomic analysis revealed significant upregulation of 34 CYP450 genes.Among these genes,CYP3A4(gene 8840)showed strong binding affinity for benzo[a]pyrene,as confirmed by molecular docking studies,indicating its key role in the biodegradable process.Furthermore,the metabolic network analysis showed that the electron transfer required for CYP450-mediated oxidative reactions enhanced mitochondrial oxidative phosphorylation and subsequently energy metabolism in A.fumigatus Z5.This metabolic coordination likely facilitates the complete degradation of benzo[a]pyrene.Our study illuminates the fundamental roles of CYP450 from A.fumigatus Z5 in benzo[a]pyrene degradation and provides novel insight into designing and implementing enhanced bioremediation strategies.
