The DFT-based （density fimctional theory） ab initio quantum mechanical methods have been applied to study the basicity of the nitrogen-containing compounds in petroleum. The results have indicated that there is a di...The DFT-based （density fimctional theory） ab initio quantum mechanical methods have been applied to study the basicity of the nitrogen-containing compounds in petroleum. The results have indicated that there is a distinct relationship between the protonation energy of nitrogen-containing compounds and their basicity. The more negative the protonation energy, the stronger the basicity is. It has been also found that aliphatic amines are more basic than pyridines or aromatic amines, and all these compounds are more basic than pyrroles. The addition of the aromatic rings can influence the basicity of anilines, while the 5- and 6-membered heterocyclic compounds function differently. The solvent properties may affect the basicity of these nitrogen-containing compounds.展开更多
The adsorptive denitrogenation from fuels over three metal-organic frameworks(MIL-96(Al),MIL-53(Al)and MIL-101(Cr))was studied by batch adsorption experiments.Four nitrogen-containing compounds(NCCs)pyridine,pyrrole,q...The adsorptive denitrogenation from fuels over three metal-organic frameworks(MIL-96(Al),MIL-53(Al)and MIL-101(Cr))was studied by batch adsorption experiments.Four nitrogen-containing compounds(NCCs)pyridine,pyrrole,quinoline and indole were used as model NCCs in fuels to study the adsorption mechanism.The physicochemical properties of the adsorbents were characterized by XRD,N2physical adsorption,FT-IR spectrum and Hammett indicator method.The metal-organic frameworks(MOFs),especially the MIL-101(Cr)containing Lewis acid sites as well as high specific surface area,can adsorb large quantities of NCCs from fuels.In addition,the adsorptive capacity over MIL-101(Cr)will be different for NCCs with different basicity.The stronger basicity of the NCC is,the more it can be absorbed over MIL-101(Cr).Furthermore,pore size and shape also affect the adsorption capacity for a given adsorbate,which can be proved by the adsorption over MIL-53(Al)and MIL-96(Al).The pseudo-second-order kinetic model and Langmuir equation can be used to describe kinetics and thermodynamics of the adsorption process,respectively.Finally,the regeneration of the used adsorbent has been conducted successfully by just washing it with ethanol.展开更多
To elucidate the effects of Fe_(2)O_(3) on nitrogen transformation during sludge pyrolysis,thermogravimetry coupled with mass spectrometry(TG-MS)was used to investigate the influences of Fe_(2)O_(3) on the pyrolysis c...To elucidate the effects of Fe_(2)O_(3) on nitrogen transformation during sludge pyrolysis,thermogravimetry coupled with mass spectrometry(TG-MS)was used to investigate the influences of Fe_(2)O_(3) on the pyrolysis characteristics and the release of important gaseous NO_(x) precursors such as HCN and NH_(3) during pyrolysis of three typical amino acids in urban sludge.The results show that after Fe_(2)O_(3) addition,the total weight loss rate of the three amino acids and the initial decomposition temperature of proline are reduced.The release amounts of NH_(3),HCN,CH_(3)CN,and HNCO from these three representative amino acids—glumatic,arginine,and proline,decrease in the order of arginine,glutamic,proline.The generation of Fe-N complexes,reduces the generation of NH_(3),HCN,CH_(3)CN,and HNCO while the catalysis effects of Fe_(2)O_(3) on the formation of H and H2 play a promoting role in the generation of NH_(3),HCN,CH_(3)CN,and HNCO.The results would provide an experimental and theoretical basis for subsequent research on the NOx precursor formation mechanisms during pyrolysis or combustion of Fe-containing sludge or sludge with additives containing Fe.展开更多
Nitrogen-containing organic compounds(NOCs)may potentially contribute to aqueous secondary organic aerosols,yet the different formation of NOCs in aerosol particles and cloud droplets remains unclear.With the in-situ ...Nitrogen-containing organic compounds(NOCs)may potentially contribute to aqueous secondary organic aerosols,yet the different formation of NOCs in aerosol particles and cloud droplets remains unclear.With the in-situ measurements performed at a mountain site(1690 m a.s.l.)in southern China,we investigated the formation of NOCs in the cloud droplets and the cloud-free particles,based on their mixing state information of NOCscontaining particles by single particle mass spectrometry.The relative abundance of NOCs in the cloud-free particles was significantly higher than those in cloud residual(cloud RES)particles.NOCs were highly correlated with carbonyl compounds(including glyoxalate and methylglyoxal)in the cloud-free particles,however,limited correlation was observed for cloud RES particles.Analysis of their mixing state and temporal variations highlights that NOCs was mainly formed from the carbonyl compounds and ammonium in the cloud-free particles,rather than in the cloud RES particles.The results support that the formation of NOCs from carbonyl compounds is facilitated in concentrated solutions in wet aerosols,rather than cloud droplets.In addition,we have identified the transport of biomass burning particles that facilitate the formation of NOCs,and that the observed NOCs is most likely contributed to the light absorption.These findings have implications for the evaluation of NOCs formation and their contribution to light absorption.展开更多
Chili fermentation is one of the most important processes in the production of Pixian Douban(PXDB),which determines the flavor and product quality of PXDB.However,the maturity of fermented chili mainly depends on empi...Chili fermentation is one of the most important processes in the production of Pixian Douban(PXDB),which determines the flavor and product quality of PXDB.However,the maturity of fermented chili mainly depends on empirical judgment,which can not satisfy the need for standardized production of PXDB.Therefore,this study aimed to investigate volatile and non-volatile substances during the maturation process and to find markers related to the maturity of fermented chili.Two-dimensional gas chromatography-mass spectrometry(GC×GC-MS)combined with multivariate statistical analysis and relative odor activity values(ROAV)analysis revealed that 2-methoxy-3-isobutyl pyrazine,linalool,3-(methylthio)propionaldehyde,myrcene,and decanal(ROAV≥1,VIP>1,P<0.05)were regarded as potentially active aromatic markers for differentiating fermentation time.Additionally,ultra-high performance liquid chromatography coupled with quadrupole time-of-flight mass spectrometry(UPLCQTOF-MS)combined with multivariate statistical analysis revealed that 25 compounds could serve as differentiated non-volatile compounds.The correlation of maturity-related physicochemical indicators with volatile and nonvolatile compounds revealed that four volatile compounds(2-methoxy-3-isobutylpyrazine,linalool,myrcene,and decanal)along with seven non-volatile compounds could serve as markers for evaluating the maturity of fermented chili.This study is expected to establish a standard for the determination of the maturity the fermented chili and lay the foundation for intelligent production of PXDB.展开更多
A trace analytical method based on solid-phase extraction gas chromatography-tandem mass spectrometry(SPE–GC–MS/MS)was developed for the rapid detection of 256 semi-volatile organic compounds(SVOCs),including 25 pol...A trace analytical method based on solid-phase extraction gas chromatography-tandem mass spectrometry(SPE–GC–MS/MS)was developed for the rapid detection of 256 semi-volatile organic compounds(SVOCs),including 25 polycyclic aromatic hydrocarbons(PAHs),70 polychlorinated biphenyls(PCBs),123 pesticides,20 phthalate esters(PAEs),4 organophosphate esters(OPEs),9 synthetic musks(SMs),and 5 UV filters(UVs)in water.No-tably,this method provided a decent linearity of calibration standards(R^(2)>0.999),excellent method limits of quantification(MLOQs)(0.12–11.41 ng/L),satisfactory matrix spiking recovery rates(60.4%–126%),and high precision(intra-day relative standard deviations(RSDs):1.0%–10.0%,inter-day RSDs:3.0%–15.0%,and inter-week RSDs:3.4%–15.7%),making it suitable for trace-level studies.Statistical analysis revealed that SVOCs with higher volatility exhibited enhanced recovery rates.Validation of the methodology involved analyzing SVOCs in real spring water and river water samples.Twenty-seven SVOCs were detected in spring water and 58 in river water,with an average concentration of 631.73 and 16,095 ng/L,respectively.Among the detected SVOCs,PAEs constituted the predominant proportion.This study underscored the presence of SVOCs contamination specifi-cally within the spring water,although SVOCs concentrations in river water were significantly greater than those found in spring water.In summary,this sensitive method based on SPE–GC–MS/MS was successfully developed and validated for the rapid analysis of a diverse array of 256 SVOCs at trace levels in water,including not only the traditional highly valued PAHs,PCBs,pesticides,and PAEs,but also the emerging OPEs,UVs,and SMs.展开更多
Endogenous hydrogen systems,consisting of metal–organic coordination catalysts and alcohols,have been widely applied for the transfer hydrogenation(TH)of biomass-derived carbonyl compounds in recent years.Metal-organ...Endogenous hydrogen systems,consisting of metal–organic coordination catalysts and alcohols,have been widely applied for the transfer hydrogenation(TH)of biomass-derived carbonyl compounds in recent years.Metal-organic coordination catalysts showed satisfactory ability of TH in the secondary alcohols,but most of them could not effectively employ the cheaper primary alcohols as hydrogen donors.Furthermore,they commonly contained high metal contents,which also led to low catalytic efficiency in significant measure.In this work,we constructed a novel magnesium single-atom catalyst(Mg-NC)with merely 0.37 wt%Mg by means of a combined self-assembly and pyrolysis strategy.The characterization results indicated that Mg was atomically dispersed and it was coordinated with four pyridinic-N in Mg-NC.Due to the obvious electron transfer from Mg to its coordinated pyridinic-N,Mg–N_(4)active centers displayed high Lewis acid-base strength with abundant content,which brought remarkable catalytic activity.When Mg-NC was used for the TH of 5-hydroxymethylfurfural(HMF)in ethanol(EtOH),2,5-bis(hydroxymethyl)furan(BHMF)yield was up to 96.3%with high productivity of 19.85 molBHMF mol_(Mg)^(−1)h^(−1)at 150°C for 5 h.More interestingly,the process of TH over Mg-NC in EtOH was proved to proceed via the hydrogen radical mechanism.Additionally,Mg-NC exhibited powerful catalytic universality;it could not only utilize other primary alcohols(such as n-propanol and n-butanol)as hydrogen donors,but also catalyze the TH of other carbonyl compounds(such as furfural,5-methylfurfural,benzaldehyde,cyclohexanone,and levulinic acid).Overall,this work offered some important clues and references to reinforce the hydrogen-supplying ability of primary alcohols in the TH of various biomass-derived carbonyl compounds to high-value fine chemicals.展开更多
Carbonyl compounds play a pivotal role in the formation of secondary pollutants such as O_(3) and SOA,signifi-cantly impacting air quality and human health.This study extended the observation period compared to previo...Carbonyl compounds play a pivotal role in the formation of secondary pollutants such as O_(3) and SOA,signifi-cantly impacting air quality and human health.This study extended the observation period compared to previous research,providing a long-term perspective on carbonyl compound variations and their environmental implica-tions.Atmospheric observations were conducted at Beijing(BJ)and Xianghe(XH)during the summer and winter months of 2018,2019,and 2023 to study the sources and impacts of carbonyl compounds in typical urban areas and peri‑urban areas.Notably,concentrations in the summer of 2023 increased compared to 2018 and 2019.The predominant carbonyl compounds—formaldehyde,acetaldehyde,and acetone—accounted for over 60%of the total.The mean values of OFP in BJ ranged from 18.55 to 58.61μg/m3,lower than those in XH(29.82 to 65.48μg/m3),with formaldehyde and acetaldehyde contributing over 80%of the total.SOAP exhibited a similar pattern,with values in XH(69.21 to 508.55μg/m3)significantly exceeding those in BJ(34.47 to 159.78μg/m3).The PMF model highlighted vehicle exhaust,secondary pollution,and biomass combustion as major sources of carbonyl compounds,emphasizing differences in source contributions between the two regions.This study’s com-parative analysis over different years and locations provides new insights into the dynamic changes in carbonyl compounds and their environmental importance.These results not only reinforce the importance of carbonyl compounds regulation but also offer a valuable reference for evaluating and refining emission control strategies during this period.展开更多
Many nitrogen-containing aromatic compounds （NACs）, such as nitrobenzene （NB）, 4-nitrophenol （4-NP）, aniline （AN）, and 2,4-dinitrophenol （2,4-DNP）, are environmentally hazardous, and their removal from conta...Many nitrogen-containing aromatic compounds （NACs）, such as nitrobenzene （NB）, 4-nitrophenol （4-NP）, aniline （AN）, and 2,4-dinitrophenol （2,4-DNP）, are environmentally hazardous, and their removal from contaminated water is one of the main challenges facing wastewater treatment plants. In this study, synthetic wastewater containing NB, 4-NP, 2,4-DNP, and AN at concentrations ranging from 50 to 180 mg/L was fed into a sequencing batch reactor （SBR）. Analyses of the SBR system indicated that it simultaneously removed more than 99% of the NACs at loading rates of 0.36 kg NB/（m^3·d）, 0.3 kg 4-NP/（m^3·d）, 0.25 kg AN/（m^3·d）, and 0.1 kg 2,4-DNP/（m^3·d）. Bacterial groups of Bacteriodetes, Candidate division TM7, α-Proteobacteria, and β-Proteobacteria were dominant in the clone libraries of 16S rRNA genes retrieved from the microbial communities in the SBR system. ＂Cycle tests＂ designed to alter feeding and aeration parameters of the SBR system demonstrated that the resident microbial biome of the SBR system responded rapidly to changing conditions. Consumption of O2 was concomitant with the apparent mineralization of NACs. Aromatic ring-cleaving dioxygenase activities suggested that （1） AN and NB were degraded via catechol 2,3-dioxygenase; （2） 4-NP was degraded via 1,2,4-benzentriol 1,2-dioxygenase; and （3） 2,4-DNP was degraded via an unresolved pathway.展开更多
In the last decade,shell biorefinery,a novel concept referring to the extraction of the main components of crustacean shells and the transformation of each component into valuable products,was proposed and has attract...In the last decade,shell biorefinery,a novel concept referring to the extraction of the main components of crustacean shells and the transformation of each component into valuable products,was proposed and has attracted increasing attentions.Chitin is one of main components of crustacean shells.Owing to the bio-fixed nitrogen element,chitin biomass has been regarded as a good candidate to produce nitrogen-containing chemicals.Among these,3-acetamido-5-acetylfuran(3A5AF)is an interesting furanic compound derived from the hydrolysis and sequential dehydration of chitin.Similar to cellulose-derived platform chemical 5-hydromethylfurfural(HMF),3A5AF is an emerging platform compound and also can be converted into various useful chemicals by oxidation,reduction,hydrolysis,substitution,and so on.This review showcases the recent advances in the synthesis of 3A5AF from chitin and N-acetyl glucosamine(NAG)employing various catalytic systems.The conversion of 3A5AF into valuable compounds was introduced then.There are still some challenges in this area,for example,the rational design of green and efficient catalytic systems for the synthesis of 3A5AF and its derivatives.The outlooks also were discussed at the end of the review.展开更多
In an earlier paper, the authors reported the solid and liquid phase equilibria in mix-tures of tetrachloromethane with oxygen-containing compounds. This note reports the solidand liquld phase equilibria for mixtures ...In an earlier paper, the authors reported the solid and liquid phase equilibria in mix-tures of tetrachloromethane with oxygen-containing compounds. This note reports the solidand liquld phase equilibria for mixtures of tetrachloromethane with nitrogen-containing com-pounds. The solid intermolecular compound forms in mixture of tetrachloromethane withbenzene, the intermolecular bonding in compound has been assumed to be charge transfer.The intermolecula compounds form easily in mixtures in which the electron density of thebenzene ring has been increased in the presence of electron-excluding substituents in展开更多
Evaluating the hydrocarbon generation potential of highly mature organic matter is a key and critically challenging area of research in petroleum geochemistry. To explore this issue, we used negative ion electrospray ...Evaluating the hydrocarbon generation potential of highly mature organic matter is a key and critically challenging area of research in petroleum geochemistry. To explore this issue, we used negative ion electrospray ionization-Fourier transform-ion cyclotron resonance-mass spectrometry to investigate the molecular evolution of N-containing compounds in Carboniferous-lower Permian source rocks with a range of maturities in the northwestern Junggar Basin, China. The N1compounds formed from on-fluorescent chlorophyll catabolites(NCCs), which record the characteristics of the residual soluble organic matter. These components remain in the source rocks after hydrocarbon generation and expulsion, and enable evaluation of the hydrocarbon generation potential. The newly defined indexes of molecular evolution, which are the polymerization index P1([DBE 18+DBE 15]/[DBE 12+DBE 9]_N1) and alkylation index R1(RC_(6–35)/RC_(0–5)), combined with the vitrinite reflectance(VR_(o)) and paleo-salinity index(β-carotane/n Cmax), can identify the factors that control the evolution of highly mature organic matter. The main factor for source rocks deposited in a weakly saline environment is the maturity, but for a highly saline environment both the maturity and salinity are key factors. The high salinity inhibits the molecular polymerization of organic matter and extends the oil generation peak. Given the differences in the bio-precursors in saline source rocks, we propose a new model for hydrocarbon generation that can be used to determine the oil generation potential of highly mature organic matter.展开更多
Furniture is identified as a vital volatile organic compound(VOC)emission source in the indoor environment.Leather has become the most common raw and auxiliary fabric material for upholstered furniture,particularly wi...Furniture is identified as a vital volatile organic compound(VOC)emission source in the indoor environment.Leather has become the most common raw and auxiliary fabric material for upholstered furniture,particularly with extensive consumption in sofas,due to its abundant resources and efficient functions.Despite being widely traded across the world,little research has been conducted on the VOCs released by leathermaterials and their health risk assessment in the indoor environment.Accordingly,this study investigated the VOC emissions of leather with different grades and the health risk of the inhalation exposure.Based on the ultra-fast gas phase electronic nose(EN)and GC-FID/Qtof,the substantial emissions of aliphatic aldehyde ketones(Aks),particularly hexanal,appear to be the cause of off-flavor in medium and low grade(MG and LG)sofa leathers.The health risk assessment indicated that leather materials barely pose non-carcinogenic and carcinogenic effects to residents.Given the abundance of VOC sources and the accumulation of health risks in the indoor environment,more stringent specifications concerning qualitative and quantitative content should be extended to provide VOC treatment basic for the manufacturing industry and obtain better indoor air quality.展开更多
Initial success has been achieved in Hong Kong in controlling primary air pollutants,but ambient ozone levels kept increasing during the past three decades.Volatile organic compounds(VOCs)are important for mitigating ...Initial success has been achieved in Hong Kong in controlling primary air pollutants,but ambient ozone levels kept increasing during the past three decades.Volatile organic compounds(VOCs)are important for mitigating ozone pollution as its major precursors.This study analyzed VOC characteristics of roadside,suburban,and rural sites in Hong Kong to investigate their compositions,concentrations,and source contributions.Herewe showthat the TVOC concentrations were 23.05±13.24,12.68±15.36,and 5.16±5.48 ppbv for roadside,suburban,and rural sites between May 2015 to June 2019,respectively.By using Positive Matrix Factorization(PMF)model,six sources were identified at the roadside site over five years:Liquefied petroleum gas(LPG)usage(33%–46%),gasoline evaporation(8%–31%),aged air mass(11%–28%),gasoline exhaust(5%–16%),diesel exhaust(2%–16%)and fuel filling(75–9%).Similarly,six sources were distinguished at the suburban site,including LPG usage(30%–33%),solvent usage(20%–26%),diesel exhaust(14%–26%),gasoline evaporation(8%–16%),aged air mass(4%–11%),and biogenic emissions(2%–5%).At the rural site,four sources were identified,including aged airmass(33%–51%),solvent usage(25%–30%),vehicular emissions(11%–28%),and biogenic emissions(6%–12%).The analysis further revealed that fuel filling and LPG usage were the primary contributors to OFP and OH reactivity at the roadside site,while solvent usage and biogenic emissions accounted for almost half of OFP and OH reactivity at the suburban and rural sites,respectively.These findings highlight the importance of identifying and characterizing VOC sources at different sites to help policymakers develop targeted measures for pollution mitigation in specific areas.展开更多
Organic-rich mudstones and shales,which hold significant potential for shale oil resources,characterize the first member of the Upper Cretaceous Qingshankou Formation(K_(2)qn~1)in the Sanzhao sag of the Songliao Basin...Organic-rich mudstones and shales,which hold significant potential for shale oil resources,characterize the first member of the Upper Cretaceous Qingshankou Formation(K_(2)qn~1)in the Sanzhao sag of the Songliao Basin,NE China.Focusing on 30 core samples obtained from the first shale oil parameter well,named SYY3 in the study area,we systematically analyzed the composition and stratigraphic distribution of the K_(2)qn~1 heteroatomic compounds using electrospray ionization Fourier transform-ion cyclotron resonance mass spectrometry(ESI FT-ICR MS),to assess their geological relevance to shale oil.The findings indicate that in the negative ion mode,the heteroatomic compounds predominantly consist of N_(1),N_(1)O_(1)-N_(1)O_(8),O_(1)-O_(8),O_(1)S_(1)-O_(6)S_(1);contrastingly,in the positive ion mode,they are primarily composed of N_(1)-N_(2),N_(1)O_(1)-N_(1)O_(4),N_(2)O_(1),O_(1)-O_(4),O_(1)S_(1)-O_(2)S_(1).Heteroatomic compound distributions vary significantly with depth in the negative ion mode,with minor variations in the positive ion mode.These distributions are categorized into three types based on the negative ion ratio((N_(1)+N_(1)O_(x))/O_(x)):TypeⅠ(>1.5),TypeⅡ(0.8-1.5),and TypeⅢ(<0.8);typesⅠandⅡgenerally exhibit a broader range of carbon numbers compared to TypeⅢ.The distribution of double bond equivalent(DBE)values across various sample types exhibits minimal variance,whereas that of carbon numbers shows substantial differences.Variations in heteroatomic compound compositions among the samples might have resulted from vertical sedimentary heterogeneity and differing biotic contributions.TypeⅢsamples show a decrease in total organic carbon(TOC)and free oil content(S_(1))compared to typesⅠandⅡ,but an increased oil saturation index(OSI),indicating a lower content of free oil but a higher proportion of movable oil.The reduced content of N-containing compounds implies lower paleolake productivity during deposition,leading to a reduction in TOC and S_(1).A lower TOC can enhance oil movability due to reduced oil adsorption,and the decreased presence of polar nitrogenous macromolecules with fewer highC-number heteroatomic compounds further promote shale oil movability.Additionally,the negative ion ratios of N1/N1O1and O2/O1 exhibit positive and negative correlations with the values of TOC,S_(1),and extractable organic matter(EOM),respectively,indicating that the salinity and redox conditions of the depositional water body are the primary controlling factors for both organic matter enrichment and shale oil accumulation.展开更多
Particulate matter(PM)can cause adverse health effects by overproducing reactive oxygen species(ROS).Although the ability of PM to induce ROS generation depends on its composi-tion and environmental factors.This study...Particulate matter(PM)can cause adverse health effects by overproducing reactive oxygen species(ROS).Although the ability of PM to induce ROS generation depends on its composi-tion and environmental factors.This study explores how photo-oxidation affects ROS gen-eration from aromatic compounds(ACs,including catechol(CAT),phthalic acid(PA),and 4,4-oxydibenzoic acid(4,4-OBA))and their mixtures with transition metals(TMs,includ-ing Fe(II),Mn(II),and Cu(II))using Fourier-transform infrared(FTIR)and Ultraviolet-visible spectroscopy(UV-Vis).Results showed that photo-oxidation facilitated ROS generation from ACs.CAT-Fe(II)/Cu(II)showed synergistic effects,but 4,4-OBA-Fe(II)/Cu(II)showed antag-onistic effects.ACs-Mn(II)and PA-Fe(II)/Cu(II)exhibited synergistic effects first and then showed antagonistic effects.The different interactions were due to complexation between ACs and TMs.The photo-oxidized ACs-TMs significantly enhanced ROS generation com-pared with ACs-TMs.The study suggested the photo-oxidation mechanism involved that the transfer ofπ-electrons from the ground to an excited state in benzene rings and func-tional groups,leading to the breakage and formation of chemical bonds or easierπ-electron transfer from ACs to TMs.The former could generate ROS directly or produce polymers that promoted ROS generation,while the latter promoted ROS generation by transferringπ-electrons to dissolved oxygen quickly.Our study revealed that both interactions among components and photo-oxidation significantly influenced ROS generation.Future studies should integrate broader atmospheric factors and PM components to fully assess oxidative potential and health impacts.展开更多
VOCs(Volatile organic compounds)exert a vital role in ozone and secondary organic aerosol production,necessitating investigations into their concentration,chemical characteristics,and source apportionment for the effe...VOCs(Volatile organic compounds)exert a vital role in ozone and secondary organic aerosol production,necessitating investigations into their concentration,chemical characteristics,and source apportionment for the effective implementation of measures aimed at preventing and controlling atmospheric pollution.FromJuly to October 2020,onlinemonitoringwas conducted in the main urban area of Shijiazhuang to collect data on VOCs and analyze their concentrations and reactivity.Additionally,the PMF(positive matrix factorization)method was utilized to identify the VOCs sources.Results indicated that the TVOCs(total VOCs)concentration was(96.7±63.4μg/m^3),with alkanes exhibiting the highest concentration of(36.1±26.4μg/m^3),followed by OVOCs(16.4±14.4μg/m^3).The key active components were alkenes and aromatics,among which xylene,propylene,toluene,propionaldehyde,acetaldehyde,ethylene,and styrene played crucial roles as reactive species.The sources derived from PMF analysis encompassed vehicle emissions,solvent and coating sources,combustion sources,industrial emissions sources,as well as plant sources,the contribution of which were 37.80%,27.93%,16.57%,15.24%,and 2.46%,respectively.Hence,reducing vehicular exhaust emissions and encouraging neighboring industries to adopt low-volatile organic solvents and coatings should be prioritized to mitigate VOCs levels.展开更多
The organic compound composition ofwastewater,serves as a crucial indicator for the operational performance of activated sludge processes and has a major influence on the development of filamentous bulking in activate...The organic compound composition ofwastewater,serves as a crucial indicator for the operational performance of activated sludge processes and has a major influence on the development of filamentous bulking in activated sludge.This study focused on the impact of typical soluble and slowly-biodegradable organic compounds,investigating the pathways through which these substrates affect the occurrence of filamentous bulking in systems operated under both high-and low-oxygen conditions.Results showed that slowly-biodegradable organic compounds lead to a concentrated distribution of microorganisms within flocs,with inward growth of filamentous bacteria.Both Tween-80 and granular starch treated systems exhibited a significant increase in protein content.The glucose system,utilizing soluble substrates,exhibited a markedly higher total polysaccharide content.Microbial communities in the Tween-80 and granular starch treated systems were characterized by a higher abundance of bacteria known to enhance sludge flocculation and settling,such as Competibacter,Xanthomonadaceae and Zoogloea.These findings are of high significance for controlling the operational performance and stability of activated sludge systems,deepening our understanding and providing a novel perspective for the improvement of wastewater treatment processes.展开更多
Peptic ulcer(PU)is characterized by inflammation,necrosis,and erosion of the gastrointestinal mucosa caused by various pathogenic factors,leading to ulcer formation.The stomach and duodenum are the most commonly affec...Peptic ulcer(PU)is characterized by inflammation,necrosis,and erosion of the gastrointestinal mucosa caused by various pathogenic factors,leading to ulcer formation.The stomach and duodenum are the most commonly affected sites.Bletilla striata,a traditional Chinese medicinal herb,contains diverse chemical constituents and exhibits multiple pharmacological effects.As a key component in various traditional Chinese medicine compound formulations,it has demonstrated notable clinical efficacy.Moreover,it has a solid research foundation and broad application prospects in the treatment of gastrointestinal diseases.This paper systematically elaborates on the clinical efficacy and mechanisms of action of Bletilla striata in the treatment of PUs,drawing from ancient medical literature and traditional formula applications to provide support for clinical use.展开更多
Emission characteristics of biogenic volatile organic compounds(BVOCs)from dominant tree species in the subtropical pristine forests of China are extremely limited.Here we conducted in situ field measurements of BVOCs...Emission characteristics of biogenic volatile organic compounds(BVOCs)from dominant tree species in the subtropical pristine forests of China are extremely limited.Here we conducted in situ field measurements of BVOCs emissions from representative mature evergreen trees by using dynamic branch enclosures at four altitude gradients(600-1690ma.s.l.)in the Nanling Mountains of southern China.Composition characteristics as well as seasonal and altitudinal variations were analyzed.Standardized emission rates and canopyscale emission factors were then calculated.Results showed that BVOCs emission intensities in the wet season were generally higher than those in the dry season.Monoterpenes were the dominant BVOCs emitted from most broad-leaved trees,accounting for over 70%of the total.Schima superba,Yushania basihirsuta and Altingia chinensis had relatively high emission intensities and secondary pollutant formation potentials.The localized emission factors of isoprene were comparable to the defaults in the Model of Emissions of Gases and Aerosols fromNature(MEGAN),while emission factors of monoterpenes and sesquiterpenes were 2 to 58 times of those in the model.Our results can be used to update the current BVOCs emission inventory in MEGAN,thereby reducing the uncertainties of BVOCs emission estimations in forested regions of southern China.展开更多
基金supported by the"973"project envisaged in the State Key Basic R&D Program(2006CB202505).
文摘The DFT-based （density fimctional theory） ab initio quantum mechanical methods have been applied to study the basicity of the nitrogen-containing compounds in petroleum. The results have indicated that there is a distinct relationship between the protonation energy of nitrogen-containing compounds and their basicity. The more negative the protonation energy, the stronger the basicity is. It has been also found that aliphatic amines are more basic than pyridines or aromatic amines, and all these compounds are more basic than pyrroles. The addition of the aromatic rings can influence the basicity of anilines, while the 5- and 6-membered heterocyclic compounds function differently. The solvent properties may affect the basicity of these nitrogen-containing compounds.
基金supported by the Program for New Century Excellent Talents in University (NCET-04-0270)National Basic Research Program of China (2011CB201301)
文摘The adsorptive denitrogenation from fuels over three metal-organic frameworks(MIL-96(Al),MIL-53(Al)and MIL-101(Cr))was studied by batch adsorption experiments.Four nitrogen-containing compounds(NCCs)pyridine,pyrrole,quinoline and indole were used as model NCCs in fuels to study the adsorption mechanism.The physicochemical properties of the adsorbents were characterized by XRD,N2physical adsorption,FT-IR spectrum and Hammett indicator method.The metal-organic frameworks(MOFs),especially the MIL-101(Cr)containing Lewis acid sites as well as high specific surface area,can adsorb large quantities of NCCs from fuels.In addition,the adsorptive capacity over MIL-101(Cr)will be different for NCCs with different basicity.The stronger basicity of the NCC is,the more it can be absorbed over MIL-101(Cr).Furthermore,pore size and shape also affect the adsorption capacity for a given adsorbate,which can be proved by the adsorption over MIL-53(Al)and MIL-96(Al).The pseudo-second-order kinetic model and Langmuir equation can be used to describe kinetics and thermodynamics of the adsorption process,respectively.Finally,the regeneration of the used adsorbent has been conducted successfully by just washing it with ethanol.
文摘To elucidate the effects of Fe_(2)O_(3) on nitrogen transformation during sludge pyrolysis,thermogravimetry coupled with mass spectrometry(TG-MS)was used to investigate the influences of Fe_(2)O_(3) on the pyrolysis characteristics and the release of important gaseous NO_(x) precursors such as HCN and NH_(3) during pyrolysis of three typical amino acids in urban sludge.The results show that after Fe_(2)O_(3) addition,the total weight loss rate of the three amino acids and the initial decomposition temperature of proline are reduced.The release amounts of NH_(3),HCN,CH_(3)CN,and HNCO from these three representative amino acids—glumatic,arginine,and proline,decrease in the order of arginine,glutamic,proline.The generation of Fe-N complexes,reduces the generation of NH_(3),HCN,CH_(3)CN,and HNCO while the catalysis effects of Fe_(2)O_(3) on the formation of H and H2 play a promoting role in the generation of NH_(3),HCN,CH_(3)CN,and HNCO.The results would provide an experimental and theoretical basis for subsequent research on the NOx precursor formation mechanisms during pyrolysis or combustion of Fe-containing sludge or sludge with additives containing Fe.
基金supported by the National Key Research and Development Program of China(No.2022YFC3701103)the National Natural Science Foundation of China(No.42222705)+1 种基金the Youth Innovation Promotion Association CAS(No.2021354)Guangdong Foundation for Program of Science and Technology Research(No.2023B1212060049).
文摘Nitrogen-containing organic compounds(NOCs)may potentially contribute to aqueous secondary organic aerosols,yet the different formation of NOCs in aerosol particles and cloud droplets remains unclear.With the in-situ measurements performed at a mountain site(1690 m a.s.l.)in southern China,we investigated the formation of NOCs in the cloud droplets and the cloud-free particles,based on their mixing state information of NOCscontaining particles by single particle mass spectrometry.The relative abundance of NOCs in the cloud-free particles was significantly higher than those in cloud residual(cloud RES)particles.NOCs were highly correlated with carbonyl compounds(including glyoxalate and methylglyoxal)in the cloud-free particles,however,limited correlation was observed for cloud RES particles.Analysis of their mixing state and temporal variations highlights that NOCs was mainly formed from the carbonyl compounds and ammonium in the cloud-free particles,rather than in the cloud RES particles.The results support that the formation of NOCs from carbonyl compounds is facilitated in concentrated solutions in wet aerosols,rather than cloud droplets.In addition,we have identified the transport of biomass burning particles that facilitate the formation of NOCs,and that the observed NOCs is most likely contributed to the light absorption.These findings have implications for the evaluation of NOCs formation and their contribution to light absorption.
基金supported by the Sichuan Provincial Department of Science and Technology(2024ZHCG0086)the Chongqing Science and Technology Commission(cstc2021jscx-cylhX0014).
文摘Chili fermentation is one of the most important processes in the production of Pixian Douban(PXDB),which determines the flavor and product quality of PXDB.However,the maturity of fermented chili mainly depends on empirical judgment,which can not satisfy the need for standardized production of PXDB.Therefore,this study aimed to investigate volatile and non-volatile substances during the maturation process and to find markers related to the maturity of fermented chili.Two-dimensional gas chromatography-mass spectrometry(GC×GC-MS)combined with multivariate statistical analysis and relative odor activity values(ROAV)analysis revealed that 2-methoxy-3-isobutyl pyrazine,linalool,3-(methylthio)propionaldehyde,myrcene,and decanal(ROAV≥1,VIP>1,P<0.05)were regarded as potentially active aromatic markers for differentiating fermentation time.Additionally,ultra-high performance liquid chromatography coupled with quadrupole time-of-flight mass spectrometry(UPLCQTOF-MS)combined with multivariate statistical analysis revealed that 25 compounds could serve as differentiated non-volatile compounds.The correlation of maturity-related physicochemical indicators with volatile and nonvolatile compounds revealed that four volatile compounds(2-methoxy-3-isobutylpyrazine,linalool,myrcene,and decanal)along with seven non-volatile compounds could serve as markers for evaluating the maturity of fermented chili.This study is expected to establish a standard for the determination of the maturity the fermented chili and lay the foundation for intelligent production of PXDB.
基金supported by the National Natural Science Foundation of China(No.51939009)Shenzhen Science and Technology Program(Nos.JCYJ20241202125905008 and GXWD20201231165807007-20200810165349001).
文摘A trace analytical method based on solid-phase extraction gas chromatography-tandem mass spectrometry(SPE–GC–MS/MS)was developed for the rapid detection of 256 semi-volatile organic compounds(SVOCs),including 25 polycyclic aromatic hydrocarbons(PAHs),70 polychlorinated biphenyls(PCBs),123 pesticides,20 phthalate esters(PAEs),4 organophosphate esters(OPEs),9 synthetic musks(SMs),and 5 UV filters(UVs)in water.No-tably,this method provided a decent linearity of calibration standards(R^(2)>0.999),excellent method limits of quantification(MLOQs)(0.12–11.41 ng/L),satisfactory matrix spiking recovery rates(60.4%–126%),and high precision(intra-day relative standard deviations(RSDs):1.0%–10.0%,inter-day RSDs:3.0%–15.0%,and inter-week RSDs:3.4%–15.7%),making it suitable for trace-level studies.Statistical analysis revealed that SVOCs with higher volatility exhibited enhanced recovery rates.Validation of the methodology involved analyzing SVOCs in real spring water and river water samples.Twenty-seven SVOCs were detected in spring water and 58 in river water,with an average concentration of 631.73 and 16,095 ng/L,respectively.Among the detected SVOCs,PAEs constituted the predominant proportion.This study underscored the presence of SVOCs contamination specifi-cally within the spring water,although SVOCs concentrations in river water were significantly greater than those found in spring water.In summary,this sensitive method based on SPE–GC–MS/MS was successfully developed and validated for the rapid analysis of a diverse array of 256 SVOCs at trace levels in water,including not only the traditional highly valued PAHs,PCBs,pesticides,and PAEs,but also the emerging OPEs,UVs,and SMs.
基金financially supported by the National Natural Science Foundation of China(U22A20421)the Qinglan Project of Jiangsu Province,the 533 Talent Program of Huaian City,and the College Students’Innovative Entrepreneurial Training Plan Program of Jiangsu Province(X202510323027).
文摘Endogenous hydrogen systems,consisting of metal–organic coordination catalysts and alcohols,have been widely applied for the transfer hydrogenation(TH)of biomass-derived carbonyl compounds in recent years.Metal-organic coordination catalysts showed satisfactory ability of TH in the secondary alcohols,but most of them could not effectively employ the cheaper primary alcohols as hydrogen donors.Furthermore,they commonly contained high metal contents,which also led to low catalytic efficiency in significant measure.In this work,we constructed a novel magnesium single-atom catalyst(Mg-NC)with merely 0.37 wt%Mg by means of a combined self-assembly and pyrolysis strategy.The characterization results indicated that Mg was atomically dispersed and it was coordinated with four pyridinic-N in Mg-NC.Due to the obvious electron transfer from Mg to its coordinated pyridinic-N,Mg–N_(4)active centers displayed high Lewis acid-base strength with abundant content,which brought remarkable catalytic activity.When Mg-NC was used for the TH of 5-hydroxymethylfurfural(HMF)in ethanol(EtOH),2,5-bis(hydroxymethyl)furan(BHMF)yield was up to 96.3%with high productivity of 19.85 molBHMF mol_(Mg)^(−1)h^(−1)at 150°C for 5 h.More interestingly,the process of TH over Mg-NC in EtOH was proved to proceed via the hydrogen radical mechanism.Additionally,Mg-NC exhibited powerful catalytic universality;it could not only utilize other primary alcohols(such as n-propanol and n-butanol)as hydrogen donors,but also catalyze the TH of other carbonyl compounds(such as furfural,5-methylfurfural,benzaldehyde,cyclohexanone,and levulinic acid).Overall,this work offered some important clues and references to reinforce the hydrogen-supplying ability of primary alcohols in the TH of various biomass-derived carbonyl compounds to high-value fine chemicals.
基金supported by the National Natural Science Foundation of China(Nos.41905108 and 42130704).
文摘Carbonyl compounds play a pivotal role in the formation of secondary pollutants such as O_(3) and SOA,signifi-cantly impacting air quality and human health.This study extended the observation period compared to previous research,providing a long-term perspective on carbonyl compound variations and their environmental implica-tions.Atmospheric observations were conducted at Beijing(BJ)and Xianghe(XH)during the summer and winter months of 2018,2019,and 2023 to study the sources and impacts of carbonyl compounds in typical urban areas and peri‑urban areas.Notably,concentrations in the summer of 2023 increased compared to 2018 and 2019.The predominant carbonyl compounds—formaldehyde,acetaldehyde,and acetone—accounted for over 60%of the total.The mean values of OFP in BJ ranged from 18.55 to 58.61μg/m3,lower than those in XH(29.82 to 65.48μg/m3),with formaldehyde and acetaldehyde contributing over 80%of the total.SOAP exhibited a similar pattern,with values in XH(69.21 to 508.55μg/m3)significantly exceeding those in BJ(34.47 to 159.78μg/m3).The PMF model highlighted vehicle exhaust,secondary pollution,and biomass combustion as major sources of carbonyl compounds,emphasizing differences in source contributions between the two regions.This study’s com-parative analysis over different years and locations provides new insights into the dynamic changes in carbonyl compounds and their environmental importance.These results not only reinforce the importance of carbonyl compounds regulation but also offer a valuable reference for evaluating and refining emission control strategies during this period.
基金Project supported by the Pilot Project of Knowledge Innovation Program of Chinese Academy of Sciences (No. KZCX2-YW-G-009)the National Natural Science Foundation of China (No. 20577067, 30230010).
文摘Many nitrogen-containing aromatic compounds （NACs）, such as nitrobenzene （NB）, 4-nitrophenol （4-NP）, aniline （AN）, and 2,4-dinitrophenol （2,4-DNP）, are environmentally hazardous, and their removal from contaminated water is one of the main challenges facing wastewater treatment plants. In this study, synthetic wastewater containing NB, 4-NP, 2,4-DNP, and AN at concentrations ranging from 50 to 180 mg/L was fed into a sequencing batch reactor （SBR）. Analyses of the SBR system indicated that it simultaneously removed more than 99% of the NACs at loading rates of 0.36 kg NB/（m^3·d）, 0.3 kg 4-NP/（m^3·d）, 0.25 kg AN/（m^3·d）, and 0.1 kg 2,4-DNP/（m^3·d）. Bacterial groups of Bacteriodetes, Candidate division TM7, α-Proteobacteria, and β-Proteobacteria were dominant in the clone libraries of 16S rRNA genes retrieved from the microbial communities in the SBR system. ＂Cycle tests＂ designed to alter feeding and aeration parameters of the SBR system demonstrated that the resident microbial biome of the SBR system responded rapidly to changing conditions. Consumption of O2 was concomitant with the apparent mineralization of NACs. Aromatic ring-cleaving dioxygenase activities suggested that （1） AN and NB were degraded via catechol 2,3-dioxygenase; （2） 4-NP was degraded via 1,2,4-benzentriol 1,2-dioxygenase; and （3） 2,4-DNP was degraded via an unresolved pathway.
基金support of the National Natural Science Foundation of China(22408032)the Science and Technology Research Program of Chongqing Municipal Education Commission(KJQN202000826 and KJQN202300836)+2 种基金Research Start-up Funding project of Chongqing Technology and Business University(1856011)Science and Technology Project of Chongqing Technology and Business University(2152027)Graduate Innovative Research Project from Chongqing Technology and Business University(yjscxx2024-284-29).
文摘In the last decade,shell biorefinery,a novel concept referring to the extraction of the main components of crustacean shells and the transformation of each component into valuable products,was proposed and has attracted increasing attentions.Chitin is one of main components of crustacean shells.Owing to the bio-fixed nitrogen element,chitin biomass has been regarded as a good candidate to produce nitrogen-containing chemicals.Among these,3-acetamido-5-acetylfuran(3A5AF)is an interesting furanic compound derived from the hydrolysis and sequential dehydration of chitin.Similar to cellulose-derived platform chemical 5-hydromethylfurfural(HMF),3A5AF is an emerging platform compound and also can be converted into various useful chemicals by oxidation,reduction,hydrolysis,substitution,and so on.This review showcases the recent advances in the synthesis of 3A5AF from chitin and N-acetyl glucosamine(NAG)employing various catalytic systems.The conversion of 3A5AF into valuable compounds was introduced then.There are still some challenges in this area,for example,the rational design of green and efficient catalytic systems for the synthesis of 3A5AF and its derivatives.The outlooks also were discussed at the end of the review.
文摘In an earlier paper, the authors reported the solid and liquid phase equilibria in mix-tures of tetrachloromethane with oxygen-containing compounds. This note reports the solidand liquld phase equilibria for mixtures of tetrachloromethane with nitrogen-containing com-pounds. The solid intermolecular compound forms in mixture of tetrachloromethane withbenzene, the intermolecular bonding in compound has been assumed to be charge transfer.The intermolecula compounds form easily in mixtures in which the electron density of thebenzene ring has been increased in the presence of electron-excluding substituents in
基金supported by the National Natural Science Foundation of China(Grant Nos.42230808 and 42102148)China Postdoctoral Science Foundation(Grant No.2021M691497)。
文摘Evaluating the hydrocarbon generation potential of highly mature organic matter is a key and critically challenging area of research in petroleum geochemistry. To explore this issue, we used negative ion electrospray ionization-Fourier transform-ion cyclotron resonance-mass spectrometry to investigate the molecular evolution of N-containing compounds in Carboniferous-lower Permian source rocks with a range of maturities in the northwestern Junggar Basin, China. The N1compounds formed from on-fluorescent chlorophyll catabolites(NCCs), which record the characteristics of the residual soluble organic matter. These components remain in the source rocks after hydrocarbon generation and expulsion, and enable evaluation of the hydrocarbon generation potential. The newly defined indexes of molecular evolution, which are the polymerization index P1([DBE 18+DBE 15]/[DBE 12+DBE 9]_N1) and alkylation index R1(RC_(6–35)/RC_(0–5)), combined with the vitrinite reflectance(VR_(o)) and paleo-salinity index(β-carotane/n Cmax), can identify the factors that control the evolution of highly mature organic matter. The main factor for source rocks deposited in a weakly saline environment is the maturity, but for a highly saline environment both the maturity and salinity are key factors. The high salinity inhibits the molecular polymerization of organic matter and extends the oil generation peak. Given the differences in the bio-precursors in saline source rocks, we propose a new model for hydrocarbon generation that can be used to determine the oil generation potential of highly mature organic matter.
基金supported by the National Key Research and Development Program of China (No.2019YFC1904501).
文摘Furniture is identified as a vital volatile organic compound(VOC)emission source in the indoor environment.Leather has become the most common raw and auxiliary fabric material for upholstered furniture,particularly with extensive consumption in sofas,due to its abundant resources and efficient functions.Despite being widely traded across the world,little research has been conducted on the VOCs released by leathermaterials and their health risk assessment in the indoor environment.Accordingly,this study investigated the VOC emissions of leather with different grades and the health risk of the inhalation exposure.Based on the ultra-fast gas phase electronic nose(EN)and GC-FID/Qtof,the substantial emissions of aliphatic aldehyde ketones(Aks),particularly hexanal,appear to be the cause of off-flavor in medium and low grade(MG and LG)sofa leathers.The health risk assessment indicated that leather materials barely pose non-carcinogenic and carcinogenic effects to residents.Given the abundance of VOC sources and the accumulation of health risks in the indoor environment,more stringent specifications concerning qualitative and quantitative content should be extended to provide VOC treatment basic for the manufacturing industry and obtain better indoor air quality.
基金supported by Hong Kong Environment Protection Department(Quotation Ref.18-06532)Hong Kong Innovation and Technology Fund(ITS/193/20FP)Hong Kong Research Grants Council(No.26304921).
文摘Initial success has been achieved in Hong Kong in controlling primary air pollutants,but ambient ozone levels kept increasing during the past three decades.Volatile organic compounds(VOCs)are important for mitigating ozone pollution as its major precursors.This study analyzed VOC characteristics of roadside,suburban,and rural sites in Hong Kong to investigate their compositions,concentrations,and source contributions.Herewe showthat the TVOC concentrations were 23.05±13.24,12.68±15.36,and 5.16±5.48 ppbv for roadside,suburban,and rural sites between May 2015 to June 2019,respectively.By using Positive Matrix Factorization(PMF)model,six sources were identified at the roadside site over five years:Liquefied petroleum gas(LPG)usage(33%–46%),gasoline evaporation(8%–31%),aged air mass(11%–28%),gasoline exhaust(5%–16%),diesel exhaust(2%–16%)and fuel filling(75–9%).Similarly,six sources were distinguished at the suburban site,including LPG usage(30%–33%),solvent usage(20%–26%),diesel exhaust(14%–26%),gasoline evaporation(8%–16%),aged air mass(4%–11%),and biogenic emissions(2%–5%).At the rural site,four sources were identified,including aged airmass(33%–51%),solvent usage(25%–30%),vehicular emissions(11%–28%),and biogenic emissions(6%–12%).The analysis further revealed that fuel filling and LPG usage were the primary contributors to OFP and OH reactivity at the roadside site,while solvent usage and biogenic emissions accounted for almost half of OFP and OH reactivity at the suburban and rural sites,respectively.These findings highlight the importance of identifying and characterizing VOC sources at different sites to help policymakers develop targeted measures for pollution mitigation in specific areas.
基金jointly funded by the National Natural Science Foundation of China(Grant Nos.42072178 and U2244207)the funding project of Northeast Geological S&T Innovation Center of China Geological Survey(Grant No.QCJJ2022-37)Geological Survey Project of China Geological Survey(Grant Nos.DD20190114,DD20230022,and DD20240045)。
文摘Organic-rich mudstones and shales,which hold significant potential for shale oil resources,characterize the first member of the Upper Cretaceous Qingshankou Formation(K_(2)qn~1)in the Sanzhao sag of the Songliao Basin,NE China.Focusing on 30 core samples obtained from the first shale oil parameter well,named SYY3 in the study area,we systematically analyzed the composition and stratigraphic distribution of the K_(2)qn~1 heteroatomic compounds using electrospray ionization Fourier transform-ion cyclotron resonance mass spectrometry(ESI FT-ICR MS),to assess their geological relevance to shale oil.The findings indicate that in the negative ion mode,the heteroatomic compounds predominantly consist of N_(1),N_(1)O_(1)-N_(1)O_(8),O_(1)-O_(8),O_(1)S_(1)-O_(6)S_(1);contrastingly,in the positive ion mode,they are primarily composed of N_(1)-N_(2),N_(1)O_(1)-N_(1)O_(4),N_(2)O_(1),O_(1)-O_(4),O_(1)S_(1)-O_(2)S_(1).Heteroatomic compound distributions vary significantly with depth in the negative ion mode,with minor variations in the positive ion mode.These distributions are categorized into three types based on the negative ion ratio((N_(1)+N_(1)O_(x))/O_(x)):TypeⅠ(>1.5),TypeⅡ(0.8-1.5),and TypeⅢ(<0.8);typesⅠandⅡgenerally exhibit a broader range of carbon numbers compared to TypeⅢ.The distribution of double bond equivalent(DBE)values across various sample types exhibits minimal variance,whereas that of carbon numbers shows substantial differences.Variations in heteroatomic compound compositions among the samples might have resulted from vertical sedimentary heterogeneity and differing biotic contributions.TypeⅢsamples show a decrease in total organic carbon(TOC)and free oil content(S_(1))compared to typesⅠandⅡ,but an increased oil saturation index(OSI),indicating a lower content of free oil but a higher proportion of movable oil.The reduced content of N-containing compounds implies lower paleolake productivity during deposition,leading to a reduction in TOC and S_(1).A lower TOC can enhance oil movability due to reduced oil adsorption,and the decreased presence of polar nitrogenous macromolecules with fewer highC-number heteroatomic compounds further promote shale oil movability.Additionally,the negative ion ratios of N1/N1O1and O2/O1 exhibit positive and negative correlations with the values of TOC,S_(1),and extractable organic matter(EOM),respectively,indicating that the salinity and redox conditions of the depositional water body are the primary controlling factors for both organic matter enrichment and shale oil accumulation.
基金supported by the Weiqiao-UCAS Special Projects on Low-Carbon Technology Development(No.GYY-DTFZ-2022-007)the Fundamental Research Funds for the Central Universities(No.E0E48927×2)the National Natural Science Foundation of China(No.21677145).
文摘Particulate matter(PM)can cause adverse health effects by overproducing reactive oxygen species(ROS).Although the ability of PM to induce ROS generation depends on its composi-tion and environmental factors.This study explores how photo-oxidation affects ROS gen-eration from aromatic compounds(ACs,including catechol(CAT),phthalic acid(PA),and 4,4-oxydibenzoic acid(4,4-OBA))and their mixtures with transition metals(TMs,includ-ing Fe(II),Mn(II),and Cu(II))using Fourier-transform infrared(FTIR)and Ultraviolet-visible spectroscopy(UV-Vis).Results showed that photo-oxidation facilitated ROS generation from ACs.CAT-Fe(II)/Cu(II)showed synergistic effects,but 4,4-OBA-Fe(II)/Cu(II)showed antag-onistic effects.ACs-Mn(II)and PA-Fe(II)/Cu(II)exhibited synergistic effects first and then showed antagonistic effects.The different interactions were due to complexation between ACs and TMs.The photo-oxidized ACs-TMs significantly enhanced ROS generation com-pared with ACs-TMs.The study suggested the photo-oxidation mechanism involved that the transfer ofπ-electrons from the ground to an excited state in benzene rings and func-tional groups,leading to the breakage and formation of chemical bonds or easierπ-electron transfer from ACs to TMs.The former could generate ROS directly or produce polymers that promoted ROS generation,while the latter promoted ROS generation by transferringπ-electrons to dissolved oxygen quickly.Our study revealed that both interactions among components and photo-oxidation significantly influenced ROS generation.Future studies should integrate broader atmospheric factors and PM components to fully assess oxidative potential and health impacts.
基金supported by the Natural Science Foundation of Hebei Province(Nos.D2019106042,D2020304038,and D2021106002)the National Natural Science Foundation of China(No.22276099)+1 种基金the State Environmental Protection Key Laboratory of Formation and Prevention of Urban Air Pollution Complex(No.2021080544)the Environmental Monitoring Research Foundation of Jiangsu Province(No.2211).
文摘VOCs(Volatile organic compounds)exert a vital role in ozone and secondary organic aerosol production,necessitating investigations into their concentration,chemical characteristics,and source apportionment for the effective implementation of measures aimed at preventing and controlling atmospheric pollution.FromJuly to October 2020,onlinemonitoringwas conducted in the main urban area of Shijiazhuang to collect data on VOCs and analyze their concentrations and reactivity.Additionally,the PMF(positive matrix factorization)method was utilized to identify the VOCs sources.Results indicated that the TVOCs(total VOCs)concentration was(96.7±63.4μg/m^3),with alkanes exhibiting the highest concentration of(36.1±26.4μg/m^3),followed by OVOCs(16.4±14.4μg/m^3).The key active components were alkenes and aromatics,among which xylene,propylene,toluene,propionaldehyde,acetaldehyde,ethylene,and styrene played crucial roles as reactive species.The sources derived from PMF analysis encompassed vehicle emissions,solvent and coating sources,combustion sources,industrial emissions sources,as well as plant sources,the contribution of which were 37.80%,27.93%,16.57%,15.24%,and 2.46%,respectively.Hence,reducing vehicular exhaust emissions and encouraging neighboring industries to adopt low-volatile organic solvents and coatings should be prioritized to mitigate VOCs levels.
基金supported by the Opening Project of National Engineering Laboratory for Advanced Municipal Wastewater Treatment and Reuse Technology,and the National Natural Science Foundation of China(No.52270017).
文摘The organic compound composition ofwastewater,serves as a crucial indicator for the operational performance of activated sludge processes and has a major influence on the development of filamentous bulking in activated sludge.This study focused on the impact of typical soluble and slowly-biodegradable organic compounds,investigating the pathways through which these substrates affect the occurrence of filamentous bulking in systems operated under both high-and low-oxygen conditions.Results showed that slowly-biodegradable organic compounds lead to a concentrated distribution of microorganisms within flocs,with inward growth of filamentous bacteria.Both Tween-80 and granular starch treated systems exhibited a significant increase in protein content.The glucose system,utilizing soluble substrates,exhibited a markedly higher total polysaccharide content.Microbial communities in the Tween-80 and granular starch treated systems were characterized by a higher abundance of bacteria known to enhance sludge flocculation and settling,such as Competibacter,Xanthomonadaceae and Zoogloea.These findings are of high significance for controlling the operational performance and stability of activated sludge systems,deepening our understanding and providing a novel perspective for the improvement of wastewater treatment processes.
基金Supported by National Science and Technology Major Project,No.2024ZD0521002The Innovation Team Project of Traditional Chinese Medicine of Liaoning Province,No.LNZYYCXTD-CCCX-003+1 种基金General Program of the National Natural Science Foundation of China,No.82074296Construction Project of Inheritance Studios of Famous Chinese Medicine Experts in China,No.[2022]No.75.
文摘Peptic ulcer(PU)is characterized by inflammation,necrosis,and erosion of the gastrointestinal mucosa caused by various pathogenic factors,leading to ulcer formation.The stomach and duodenum are the most commonly affected sites.Bletilla striata,a traditional Chinese medicinal herb,contains diverse chemical constituents and exhibits multiple pharmacological effects.As a key component in various traditional Chinese medicine compound formulations,it has demonstrated notable clinical efficacy.Moreover,it has a solid research foundation and broad application prospects in the treatment of gastrointestinal diseases.This paper systematically elaborates on the clinical efficacy and mechanisms of action of Bletilla striata in the treatment of PUs,drawing from ancient medical literature and traditional formula applications to provide support for clinical use.
基金supported by the National Natural Science Foundation of China (NSFC)Projects (Nos.42205105,42121004,and 42077190)the Science and Technology Project of Shaoguan (No.210811164532141)+3 种基金the National Key R&D Program of China (2022YFC3700604)the Science and Technology Program of Guangzhou City (No.202201010400)the Fundamental Research Funds for the Central Universities (No.21622319)the Research Center of Low Carbon Economy for Guangzhou Region (No.22JNZS50).
文摘Emission characteristics of biogenic volatile organic compounds(BVOCs)from dominant tree species in the subtropical pristine forests of China are extremely limited.Here we conducted in situ field measurements of BVOCs emissions from representative mature evergreen trees by using dynamic branch enclosures at four altitude gradients(600-1690ma.s.l.)in the Nanling Mountains of southern China.Composition characteristics as well as seasonal and altitudinal variations were analyzed.Standardized emission rates and canopyscale emission factors were then calculated.Results showed that BVOCs emission intensities in the wet season were generally higher than those in the dry season.Monoterpenes were the dominant BVOCs emitted from most broad-leaved trees,accounting for over 70%of the total.Schima superba,Yushania basihirsuta and Altingia chinensis had relatively high emission intensities and secondary pollutant formation potentials.The localized emission factors of isoprene were comparable to the defaults in the Model of Emissions of Gases and Aerosols fromNature(MEGAN),while emission factors of monoterpenes and sesquiterpenes were 2 to 58 times of those in the model.Our results can be used to update the current BVOCs emission inventory in MEGAN,thereby reducing the uncertainties of BVOCs emission estimations in forested regions of southern China.
