The Fengcheng Formation is a crucial source rock and the primary reservoir for oil accumulation in the Mahu Sag.Crude oils are distributed throughout the Fengcheng Formation,ranging from the edge to the interior of th...The Fengcheng Formation is a crucial source rock and the primary reservoir for oil accumulation in the Mahu Sag.Crude oils are distributed throughout the Fengcheng Formation,ranging from the edge to the interior of the sag in the southern Mahu Sag.These crude oils originate from in-situ source rocks in shallowly buried areas and the inner deep sag.During migration,the crude oil from the inner deep sag affects the source rocks close to carrier beds,leading to changes in the organic geochemical characteristics of the source rocks.These changes might alter source rock evaluations and oil-source correlation.Based on data such as total organic carbon(TOC),Rock-Eval pyrolysis of source rocks,and gas chromatography-mass spectrometry(GC-MS)of the saturated fraction,and considering the geological characteristics of the study area,we define the identification characteristics of source rock affected by migrated hydrocarbons and establish the various patterns of influence that migrated hydrocarbons have on the source rock of the Fengcheng Formation in the southern Mahu Sag.The source rocks of the Fengcheng Formation are mostly fair to good,containing mainly Type II organic matter and being thermally mature enough to generate oil.Source rocks affected by migrated hydrocarbons exhibit relatively high hydrocarbon contents(S1/TOC>110 mg HC/g TOC,Extract/TOC>30%,HC:hydrocarbon),relatively low Rock-Eval Tmax values,and relatively high tricyclic terpane contents with a descending and mountain-shaped distribution.Furthermore,biomarker composition parameters indicate a higher thermal maturity than in-situ source rocks.Through a comparison of the extract biomarker fingerprints of adjacent reservoirs and mudstones in different boreholes,three types of influence patterns of migrated hydrocarbons are identified:the edge-influence of thin sandstone-thick mudstone,the mixed-influence of sandstone-mudstone interbedded,and the full-influence of thick sandstone-thin mudstone.This finding reminds us that the influence of migrated hydrocarbons must be considered when evaluating source rocks and conducting oil-source correlation.展开更多
Methane(CH_(4))as a substitute for other mineral fuels plays a crucial role in reducing energy consumption and preventing environmental pollution.The present study employs a solvothermal method to fabricate a porous f...Methane(CH_(4))as a substitute for other mineral fuels plays a crucial role in reducing energy consumption and preventing environmental pollution.The present study employs a solvothermal method to fabricate a porous framework Co-metal-organic framework(Co-MOF)containing two distinct secondary building units(SBUs):an anionic[Co_(2)(μ_(2)-OH)(COO)_(4)(H_(2)O)]and a neutral[CoN_(2)(COO)_(2)].Notably,within the anionic SBUs,the coordinated water molecules induce the generation of divergent unsaturated Co(Ⅱ)centers in the unidirectional porous channels,thereby creating open metal sites.The adsorption performance of Co-MOF towards pure component gases was systematically investigated.The results demonstrated that Co-MOF exhibits superior adsorption capacity for C_(2)-C_(3) hydrocarbons compared to CH_(4),which offers the potential for efficient adsorption and separation of CH_(4) from C_(2)-C_(3) hydrocarbons.The gas selectivity separation ratios of Co-MOF for C_(2)H_(6)/CH_(4) and C_(3)H_8/CH_(4) were calculated using the ideal adsorbed solution theory method at 273/298 K and 0.1 MPa.The results revealed that Co-MOF achieved remarkable equilibrium separation selectivity for CH_(4) and C_(2)-C_(3) hydrocarbon gases among non-modified MOFs,signifying the potential of the synthesized Co-MOF for efficient recovery and purification of CH_(4) from C_(2)-C_(3) hydrocarbons.Breakthrough experiments further demonstrate the ability of Co-MOF to purify methane from C_(2)-C_(3) hydrocarbons in practical gas separation scenarios.Additionally,molecular simulation calculations further substantiate the propensity of anionic SBUs to interact with C_(2)-C_(3) hydrocarbon compounds.This study provides a novel paradigm for the development of porous MOF materials in the application of gas mixture separation.展开更多
Objective To investigate changes in the urinary metabolite profiles of children exposed to polycyclic aromatic hydrocarbons(PAHs)during critical brain development and explore their potential link with the intestinal m...Objective To investigate changes in the urinary metabolite profiles of children exposed to polycyclic aromatic hydrocarbons(PAHs)during critical brain development and explore their potential link with the intestinal microbiota.Methods Liquid chromatography-tandem mass spectrometry was used to determine ten hydroxyl metabolites of PAHs(OH-PAHs)in 36-month-old children.Subsequently,37 children were categorized into low-and high-exposure groups based on the sum of the ten OH-PAHs.Ultra-high-performance liquid chromatography coupled with quadrupole time-of-flight mass spectrometry was used to identify non-targeted metabolites in the urine samples.Furthermore,fecal flora abundance was assessed by 16S rRNA gene sequencing using Illumina MiSeq.Results The concentrations of 21 metabolites were significantly higher in the high exposure group than in the low exposure group(variable importance for projection>1,P<0.05).Most of these metabolites were positively correlated with the hydroxyl metabolites of naphthalene,fluorine,and phenanthrene(r=0.336–0.531).The identified differential metabolites primarily belonged to pathways associated with inflammation or proinflammatory states,including amino acid,lipid,and nucleotide metabolism.Additionally,these distinct metabolites were significantly associated with specific intestinal flora abundances(r=0.34–0.55),which were mainly involved in neurodevelopment.Conclusion Higher PAH exposure in young children affected metabolic homeostasis,particularly that of certain gut microbiota-derived metabolites.Further investigation is needed to explore the potential influence of PAHs on the gut microbiota and their possible association with neurodevelopmental outcomes.展开更多
The electrochemical reduction of carbon dioxide offers a sound and economically viable technology for the electrification and decarbonization of the chemical and fuel industries.In this technology,an electrocatalytic ...The electrochemical reduction of carbon dioxide offers a sound and economically viable technology for the electrification and decarbonization of the chemical and fuel industries.In this technology,an electrocatalytic material and renewable energy-generated electricity drive the conversion of carbon dioxide into high-value chemicals and carbon-neutral fuels.Over the past few years,single-atom catalysts have been intensively studied as they could provide near-unity atom utilization and unique catalytic performance.Single-atom catalysts have become one of the state-of-the-art catalyst materials for the electrochemical reduction of carbon dioxide into carbon monoxide.However,it remains a challenge for single-atom catalysts to facilitate the efficient conversion of carbon dioxide into products beyond carbon monoxide.In this review,we summarize and present important findings and critical insights from studies on the electrochemical carbon dioxide reduction reaction into hydrocarbons and oxygenates using single-atom catalysts.It is hoped that this review gives a thorough recapitulation and analysis of the science behind the catalysis of carbon dioxide into more reduced products through singleatom catalysts so that it can be a guide for future research and development on catalysts with industry-ready performance for the electrochemical reduction of carbon dioxide into high-value chemicals and carbon-neutral fuels.展开更多
Natural wax gelators have different compositions of compounds(hydrocarbons,wax esters,free fatty alcohols,and free fatty acids),which results in oleogels with varying properties.To maintain a consistent composition,th...Natural wax gelators have different compositions of compounds(hydrocarbons,wax esters,free fatty alcohols,and free fatty acids),which results in oleogels with varying properties.To maintain a consistent composition,the individual components can be added to the original wax gelator.The content of hydrocarbons and wax esters greatly affects the structuring process of liquid edible oils with waxes.The aim of this study was to evaluate the possibility of modifying the properties of beeswax as a gelling agent by adding hydrocarbons or monoesters to obtain oleogels with specific properties.Various tests were conducted to assess the changes in the oleogel properties,such as color,microstructure,oil-binding capacity,thermal and textural properties.The research results have shown that the addition of the studied fractions has led to a significant change in all properties of oleogels.The initial size of oleogel crystals(7.29±1.80μm)changed after adding fractions,varying from 5.28μm to 12.58μm with hydrocarbons and from 9.95μm to 30.41μm with wax esters.The addition of 30%–50% hydrocarbons decreased the ability of the oleogels to bind oil and made them less firm compared to samples with 10%-20% hydrocarbons.Adding 10%-20% monoesters increased the firmness of the oleogels,but this indicator decreased when their content was increased to 50%.The obtained data indicate that hydrocarbons and wax esters can be used for targeted correction of the gelling properties of beeswax.展开更多
Polycyclic aromatic hydrocarbons(PAHs)are typical persistent organic pollutants(POPs)that are commonly found in the environment.They are carcinogenic,teratogenic,mutagenic and biodegradable obviously.In this paper,the...Polycyclic aromatic hydrocarbons(PAHs)are typical persistent organic pollutants(POPs)that are commonly found in the environment.They are carcinogenic,teratogenic,mutagenic and biodegradable obviously.In this paper,the modified mussel shells were used to adsorb and remove anthracene.The results show that the adsorption removal rate of the mussel shells was higher after calcination at 600℃.5%H_(3)PO_(4) solution was more suitable for shell treatment than 3 mol/L ZnCl_(2) solution.As the dosage of the modified shells was 0.5 g/L,the adsorption reached a stable state,and the removal rate of PAHs was about 69.44%;the adsorption efficiency rose with the increase of time.It can be seen that as a new and cheap biological adsorbent,the modified shells can be used to remove PAHs from wastewater.展开更多
Based on the analysis of light hydrocarbon compositions of natural gas and regional comparison in combination with the chemical components and carbon isotopic compositions of methane,the indication of geochemical char...Based on the analysis of light hydrocarbon compositions of natural gas and regional comparison in combination with the chemical components and carbon isotopic compositions of methane,the indication of geochemical characteristics of light hydrocarbons on the migration features,dissolution and escape of natural gas from the Dongsheng gas field in the Ordos Basin is revealed,and the effect of migration on specific light hydrocarbon indexes is further discussed.The study indicates that,natural gas from the Lower Shihezi Formation(Pix)in the Dongsheng gas field displays higher iso-C5-7contents than n-C5-7contents,and the C6-7light hydrocarbons are composed of paraffins with extremely low aromatic contents(<0.4%),whereas the C7light hydrocarbons are dominated by methylcyclohexane,suggesting the characteristics of coal-derived gas with the influence by secondary alterations such as dissolution.The natural gas from the Dongsheng gas field has experienced free-phase migration from south to north and different degrees of dissolution after charging,and the gas in the Shiguhao area to the north of the Borjianghaizi fault has experienced apparent diffusion loss after accumulation.Long-distance migration in free phase results in the decrease of the relative contents of the methylcyclohexane in C7 light hydrocarbons and the toluene/n-heptane ratio,as well as the increase of the n-heptane/methylcyclohexane ratio and heptane values.The dissolution causes the increase of isoheptane values of the light hydrocarbons,whereas the diffusion loss of natural gas in the Shiguhao area results in the increase of n-C5-7contents compared to the iso-C5-7contents.展开更多
Catalytic pyrolysis of digestate to produce aromatic hydrocarbons can be combined with anaerobic fermentation to effectively transform and utilize all biomass components,which can achieve the meaningful purpose of tra...Catalytic pyrolysis of digestate to produce aromatic hydrocarbons can be combined with anaerobic fermentation to effectively transform and utilize all biomass components,which can achieve the meaningful purpose of transforming waste into high-value products.This study explored whether catalytic pyrolysis of digestate is feasible to prepare aromatic hydrocarbons by analyzing the thermogravimetric characteristics,pyrolysis characteristics,and catalytic pyrolysis characteristics of digestate.For digestate pyrolysis,an increase in temperature was found to elevate the CO,CH_4,and monocyclic aromatic hydrocarbon(benzene,toluene,and xylene;BTX)content,whereas it decreased the contents of phenols,acids,aldehydes,and other oxygenates.Furthermore,the catalytic pyrolysis process effectively inhibited the acids,phenols,and furans in the liquid,whereas the yield of BTX increased from 25.45%to 45.99%,and the selectivity of xylene was also increased from 10.32%to 28.72%after adding ZSM-5.ZSM-5 also inhibited the production of nitrogenous compounds.展开更多
Polycyclic aromatic hydrocarbons(PAHs)are one of the most important groups in oil,and re sponsible for major toxic and/or carcinogenic impact on humans and wildlife.It is important to understand the behavior of PAHs i...Polycyclic aromatic hydrocarbons(PAHs)are one of the most important groups in oil,and re sponsible for major toxic and/or carcinogenic impact on humans and wildlife.It is important to understand the behavior of PAHs in marine environment after an oil-spill incident.However,interaction between petroleum PAHs and microbial communities in a marine environment remains unclear.Therefore,a series of mesocosm experiments were conducted.in which water-accommodated fraction(WAF)of oil was generated to simulate an oil-spill scenario and to analyze the transport and behavior of marine oil spill containing PAHs with and without dispersants.Results indicate that the application of dispersant could increase the concentration of total PAHs in water column due mainly to significant increase in the concentration of highmolecular weight(HMW)PAHs at a lower removal rate.At the end of the 7-day experiment,significant amount of HMW PAHs were accumulated in sediment.In general,the application of dispersant did not increase the sediment uptake of PAHs but increased the PAHs concentration in water column.展开更多
Coriander(Coriandrum sativum L.)is recognized for its antioxidant property,as a kind of natural phenolic-rich ingredient.Polycyclic aromatic hydrocarbons(PAHs)present a class of heat-driven hazards in foods,especially...Coriander(Coriandrum sativum L.)is recognized for its antioxidant property,as a kind of natural phenolic-rich ingredient.Polycyclic aromatic hydrocarbons(PAHs)present a class of heat-driven hazards in foods,especially the processed meat.In this study,the effect of coriander root and leaf extract on the formation and inhibition of PAH8 in roasted duck wings was firstly investigated.Coriander root extract(CRE)and coriander leaf extract(CLE)with five concentration groups(200,400,600,800,1000 mg/L)were prepared respectively to marinate the duck wings.CRE marinade exhibited greater inhibitory effect on PAH8 formation in roasted duck wings that ranged from 65.0%-87.4%.The electron spin resonance study indicated a significantly positive correlation between PAH8 and free radical level,suggesting the participation of radicals in PAHs formation.Also,it was speculated that the inhibitory effect on PAH8 was related to the phenolic compounds identified in coriander marinades.CRE made greater inhibitory effect on the formation of PAH8 and could be considered as a kind of natural source to mitigate PAHs in heat-processed meat products.展开更多
The knowledge of the existence,distribution and fate of polycyclic aromatic hydrocarbons(PAHs)and substituted polycyclic aromatic hydrocarbons(SPAHs)in wastewater treatment plants(WWTPs)was vital for reducing their co...The knowledge of the existence,distribution and fate of polycyclic aromatic hydrocarbons(PAHs)and substituted polycyclic aromatic hydrocarbons(SPAHs)in wastewater treatment plants(WWTPs)was vital for reducing their concentrations entering the aquatic environment.The concentrations of 13 SPAHs and 16 PAHs were all determined in a WWTP with styrene butadiene rubber(SBR)in partnership with the moving bed biofilm reactor(MBBR)process.SPAHs presented a higher concentration lever than PAHs in nearly all samples.The total removal efficiencies of PAHs and SPAHs ranged from 64.0%to 71.36%and 78.4%to 79.7%,respectively.The total yearly loads of PAHs(43.0 kg)and SPAHs(73.0 kg)were mainly reduced by the primary and SBR/MBBR biological treatment stages.The tertiary treatment stage had a minor contribution to target compounds removal.According to a synthesis and improvement fate model,we found that the dominant processes changed as the chemical octanol water partition coefficient(K_(ow))increased.But the seasonal variations of experimental removal efficiencies were more obvious than that of predicted data.In the primary sedimentation tank,dissolution in the aqueous phase and sorption to sludge/particulate matter were controlling processes for the removal of PAHs and SPAHs.The sorption to sludge and biodegradation were the principal removal mechanisms during the SBR/MBBR biological treatment process.The contribution of volatilization to removal was always insignificant.Furthermore,the basic physicochemical properties and operating parameters influenced the fate of PAHs and SPAHs in the WWTP.展开更多
Low-carbon process for resource utilization of polycyclic aromatic hydrocarbons(PAHs)in zeolitecatalyzed processes,geared to carbon neutrality-a prominent trend throughout human activities,has been bottlenecked by the...Low-carbon process for resource utilization of polycyclic aromatic hydrocarbons(PAHs)in zeolitecatalyzed processes,geared to carbon neutrality-a prominent trend throughout human activities,has been bottlenecked by the lack of a complete mechanistic understanding of coking and decoking chemistry,involving the speciation and molecular evolution of PAHs,the plethora of which causes catalyst deactivation and forces regeneration,rendering significant CO_(2) emission.Herein,by exploiting the high-resolution matrix-assisted laser desorption/ionization Fourier-transform ion cyclotron resonance mass spectrometry(MALDI FT-ICR MS),we unveil the missing fingerprints of the mechanistic pathways for both formation and decomposition of cross-linked cage-passing PAHs for SAPO-34-catalyzed,industrially relevant methanol-to-olefins(MTO)as a model reaction.Notable is the molecule-resolved symmetrical signature:their speciation originates exclusively from the direct coupling of in-cage hydrocarbon pool(HCP)species,whereas water-promoted decomposition of cage-passing PAHs initiates with selective cracking of inter-cage local structures at 8-rings followed by deep aromatic steam reforming.Molecular deciphering the reversibly dynamic evolution trajectory(fate)of full-spectrum aromatic hydrocarbons and fulfilling the real-time quantitative carbon resource footprints advance the fundamental knowledge of deactivation and regeneration phenomena(decay and recovery motifs of autocatalysis)and disclose the underlying mechanisms of especially the chemistry of coking and decoking in zeolite catalysis.The positive yet divergent roles of water in these two processes are disentangled.These unprecedented insights ultimately lead us to a steam regeneration strategy with valuable CO and H_(2) as main products,negligible CO_(2) emission in steam reforming and full catalyst activity recovery,which further proves feasible in other important chemical processes,promising to be a sustainable and potent approach that contributes to carbon-neutral chemical industry.展开更多
Polycyclic aromatic hydrocarbons (PAHs) are strongly associated with agricultural, residential, transportation, industrial and petroleum activities. In this study, the presence of PAHs (polycyclic aromatic hydrocarbon...Polycyclic aromatic hydrocarbons (PAHs) are strongly associated with agricultural, residential, transportation, industrial and petroleum activities. In this study, the presence of PAHs (polycyclic aromatic hydrocarbons) was investigated in sediments of the ivory coastal zone (Toukouzou Hozalem-Assinie). The main objectives of this study were to determine the abundance and to predict the source of PAHs in the sediments. Gas chromatography-mass spectrometry (GC-MS) was used to analyze sixteen priority PAHs. Total PAHs concentrations were from 1.31 to 3992.68 mg/kg in sediment with an average concentration of (307.54 ± 16.10) mg/kg. Among all PAHs, Naphthalene (Nap = 332.72 mg/kg) and Phenanthrene (Phe = 41.75 mg/kg) were found in the highest concentration, whereas Benzo (k) Fluoranthene was found in the least concentration in the range of 0 - 0.85 mg/kg (mean 0.24 mg/kg). Bassam-Modeste Lagune (BML) sampling site was the site with the highest concentration of total PAHs (all 16 PAHs) compared to the others due to their location in a highly populated estuary area that receives commercial, tourism, port, petroleum and heavy industrial activities. Diagnostic ratios were used to determine the sources of PAHs and suggested that the PAH profile in the sediments was dominated by 2 and 3 ring PAHs. The patterns of PAH compounds in sediment indicated that contamination is from mixed sources, with a strong indication of petrogenic contamination potentially from spills of fuel, oil and industrial activities.展开更多
The geological characteristics and production practices of the major middle-and high-maturity shale oil exploration areas in China are analyzed.Combined with laboratory results,it is clear that three essential conditi...The geological characteristics and production practices of the major middle-and high-maturity shale oil exploration areas in China are analyzed.Combined with laboratory results,it is clear that three essential conditions,i.e.economic initial production,commercial cumulative oil production of single well,and large-scale recoverable reserves confirmed by the testing production,determine whether the continental shale oil can be put into large-scale commercial development.The quantity and quality of movable hydrocarbons are confirmed to be crucial to economic development of shale oil,and focuses in evaluation of shale oil enrichment area/interval.The evaluation indexes of movable hydrocarbon enrichment include:(1)the material basis for forming retained hydrocarbon,including TOC>2%(preferentially 3%-4%),and typeⅠ-Ⅱkerogens;(2)the mobility of retained hydrocarbon,which is closely related to the hydrocarbon composition and flow behaviors of light/heavy components,and can be evaluated from the perspectives of thermal maturity(Ro),gas-oil ratio(GOR),crude oil density,quality of hydrocarbon components,preservation conditions;and(3)the reservoir characteristics associated with the engineering reconstruction,including the main pore throat distribution zone,reservoir physical properties(including fractures),lamellation feature and diagenetic stage,etc.Accordingly,13 evaluation indexes in three categories and their reference values are established.The evaluation indicates that the light shale oil zones in the Gulong Sag of Songliao Basin have the most favorable enrichment conditions of movable hydrocarbons,followed by light oil and black oil zones,containing 20.8×10^(8) t light oil resources in reservoirs with R_(0)>1.2%,pressure coefficient greater than 1.4,effective porosity greater than 6%,crude oil density less than 0.82 g/cm^(3),and GOR>100 m/m^(3).The shale oil in the Gulong Sag can be explored and developed separately by the categories(resource sweet spot,engineering sweet spot,and tight oil sweet spot)depending on shale oil flowability.The Gulong Sag is the most promising area to achieve large-scale breakthrough and production of continental shale oil in China.展开更多
Catalytic hydrogenation of CO_(2) using renewable hydrogen not only reduces greenhouse gas emissions,but also provides industrial chemicals.Herein,a Co-Fe bimetallic catalyst was developed by a facile reactive ball-mi...Catalytic hydrogenation of CO_(2) using renewable hydrogen not only reduces greenhouse gas emissions,but also provides industrial chemicals.Herein,a Co-Fe bimetallic catalyst was developed by a facile reactive ball-milling method for highly active and selective hydrogenation of CO_(2) to value-added hydrocarbons.When reacted at 320℃,1.0 MPa and 9600 mL h^(-1) g_(cat)^(-1),the selectivity to light olefin(C_(2)^(=)-C_(4)^(=)) and C_(5)+ species achieves 57.3% and 22.3%,respectively,at a CO_(2) co nversion of 31.4%,which is superior to previous Fe-based catalysts.The CO_(2) activation can be promoted by the CoFe phase formed by reactive ball milling of the Fe-Co_(3)O_(4) mixture,and the in-situ Co_(2)C and Fe_(5)C_(2) formed during hydrogenation are beneficial for the C-C coupling reaction.The initial C-C coupling is related to the combination of CO species with the surface carbon of Fe/Co carbides,and the sustained C-C coupling is maintained by self-recovery of defective carbides.This new strategy contributes to the development of efficient catalysts for the hydrogenation of CO_(2) to value-added hydrocarbons.展开更多
Three kerogen samples(JJZG-1,JJZG-2 and JJZG-3)isolated from the Permian Lucaogou shales of varying biodegradation levels(BLs≈0,3 and 7,respectively)were subjected to sequential stepwise pyrolysis combined with on-li...Three kerogen samples(JJZG-1,JJZG-2 and JJZG-3)isolated from the Permian Lucaogou shales of varying biodegradation levels(BLs≈0,3 and 7,respectively)were subjected to sequential stepwise pyrolysis combined with on-line detection of gas chromatography-mass spectrometry(GC-MS).Occluded fractions(bitumenⅡ)released at low-temperature steps(≥410℃)show consistent biodegradative signatures with that reported for solvent-extracted fractions(bitumenⅠ)of the original shales,e.g.,broad range of abundant n-alkanes,isoprenoids and regular hopanes for the non-biodegraded JJZG-1;trace n-alkanes and abundant hopanes for the moderately biodegraded JJZG-2;and no n-alkanes but still prominent hopanes including the microbially produced 25-nohopanes for the severely biodegraded JJZG-3.This consistency between bitumenⅡand bitumenⅠfractions indicates the biodegradability of the kerogenoccluded bitumenⅡwith limited protection from host kerogen.A minor level of protection was suggested by the trace distribution of n-alkanes in the bitumenⅡof JJZG-2,whereas the bitumenⅠhad no nalkanes.The kerogen itself was more resistant to biodegradation as reflected by the persistence of high abundances of both n-alkanes and hopanes in the high temperature(≥460℃)products of all three kerogen samples.However,the relative abundances of these product groups did show some evidence of biodegradation alteration,e.g.,ratios of n-C_(15)alkene/C_(27)hop-17(21)-ene at 510℃pyrolysis decreased by order of magnitude from the non-biodegraded(JJZG-1=27.4)to highly biodegraded(0.3 for JJZG-3)samples.The reduced biodegradation impact on the kerogen fraction(Cf.bitumen fractions)was also evident by the absence of 25-norhopanes in the high-temperature analysis of the JJZG-3 kerogen.展开更多
The influence of origin, depositional environment and thermal maturity of organic matter on the occurrence of aromatic hydrocarbons in source rocks from the central and northwestern Niger Delta was investigated. Eight...The influence of origin, depositional environment and thermal maturity of organic matter on the occurrence of aromatic hydrocarbons in source rocks from the central and northwestern Niger Delta was investigated. Eighty two source rock samples from four oil wells in the central and northwestern Niger Delta were analyzed for the aromatic hydrocarbon content using gas chromatography-mass spectrometry (GC-MS). The results of analysis of aromatic hydrocarbon fractions of the source rock extracts show the presence of many classes of aromatic hydrocarbons, which include naphthalenes, phenanthrenes, biphenyls, dibenzothiophenes and fluorenes. Trimethylnaphthalene (TMN) is the most abundant among the naphthalenes while dimethylphenanthrene (DMP) is the most abundant among the phenanthrenes. Among the biphenyls, 3-methylbiphenyl (3 MB) is the most abundant while 4-methyldibenzothiophene (4MDBT) is the most abundant among the dibenzothiphenes. Only two fluorenes were detected, and fluorene is more in abundance than 1-methylfluorene (1 MF). Depositional environment indicators of aromatic hydrocarbon organic matter reveal that the organic materials in the source rocks in these wells were deposited in marine-to-swamp depositional environments under reducing to suboxic conditions. Thermal maturity indicators calculated from the abundance of the aromatic hydrocarbons indicate that the source rock samples are thermally mature. Most of the source rocks are at the peak of oil window while a few at the early oil window. Source rocks from wells GB, OP and OT in the central Niger Delta are thermally more mature than those from well AW in the northwestern Niger Delta.展开更多
Despite the upsurge in hydrocarbon exploration in the Lake Albert Rift Basin(LARB)over the past three decades,systematic characterization of hydrocarbon compositions remains lacking,leading to uncertainties in source ...Despite the upsurge in hydrocarbon exploration in the Lake Albert Rift Basin(LARB)over the past three decades,systematic characterization of hydrocarbon compositions remains lacking,leading to uncertainties in source rock and oil generation determination.We characterized crude oil compositions and oil sand samples in the northern and southern subbasins of LARB.The relative abundance of normal and branched linear alkanes,hopanes,steranes,and aromatic hydrocarbon suggest that northern and southern hydrocarbons were deposited in anoxic to suboxic lacustrine environments and share similar biological source compositions(i.e.,a mixture of plants and aquatic algae and bacteria).Relative to southern samples,northern samples show more negative δ^(13)C values for oils,saturates and aromatics,indicating longer migration paths,and exhibit higher MPI-1,DNR-1 and 4-/1-MDBT ratios,indicating higher maturity.Between the two possible sets of source rocks(upper Miocene and Jurassic strata),the positive δ^(13)C values of saturated hydrocarbons(average=-20.5‰)suggest that the upper Miocene lacustrine shale is the most likely candidate.Oleanane index(<5% in our samples)does not exclude either source rock possibility,and C_(28)/C_(29) regular sterane(average=0.63)may be biased by high terrestrial inputs in a lacustrine setting.Together,our data show that northern and southern oils originate from the same source rocks but different oil kitchens.Given the similar geochemical characteristics of southern and northern oils,previous exploration successes in the northern subbasin likely suggest similar potential in the southern sector,while other elements influencing exploration success must be also evaluated.展开更多
The contents and distribution of 20 polycyclic aromatic hydrocarbons (PAHs) and heterocyclic aromatic hydrocarbons (HAHs) were investigated in 16 soil profiles of Beijing and Tianjin region. Transport of high mole...The contents and distribution of 20 polycyclic aromatic hydrocarbons (PAHs) and heterocyclic aromatic hydrocarbons (HAHs) were investigated in 16 soil profiles of Beijing and Tianjin region. Transport of high molecular weight PAHs (HMWPAHs) and the correlation between total organic carbon (TOC) and their concentrations were also discussed. The results indicated that highly contaminated sites were located at urban or wastewater irrigation areas and pollutants mainly accumulated in topsoil (〈 40 cm), with a sharp content decrease at the vertical boundary of 30-40 cm. Total PAHs/HAHs concentrations in soils from Tianjin were markedly greater than those from Beijing. Even the contents at bottoms of soil profiles in Tianjin were higher than those in topsoils of Beijing soil profile. HMWPAHs dominated the PAH profiles, exhibiting a uniform distribution of pyrogenic origin between topsoils and deep layers. Furthermore, the percentages of HMWPAHs remained relative constant with the depth of soil profiles, which were consistent with the distribution of particulate matter-associated PAHs in the local atmospheric environments. Therefore, HMWPAHs transport with particulates might be the predominant source found in soil profiles.展开更多
Based on the systematic study of aromatic hydrocarbons in over 100 crude oil samples collected from the Tabei and Tazhong uplifts in the Tarim Basin,the western depression area in the Qaidam Basin and the Tabei depres...Based on the systematic study of aromatic hydrocarbons in over 100 crude oil samples collected from the Tabei and Tazhong uplifts in the Tarim Basin,the western depression area in the Qaidam Basin and the Tabei depression in the Turpan Basin,the geochemical characteristics of the marine(Tarim Basin),saline lacustrine(Qaidam Basin),and swamp(Turpan Basin) oils were investigated.The marine oils from the Tarim basin are characterized by relatively low abundance of diaromatic hydrocarbons such as biphenyl and naphthalene,and relatively high abundance of triaromatic hydrocarbons including phenanthrene,dibenzothiophene and fluorene.In contrast,the swamp oils from the Turpan Basin are dominated by the highest relative abundance of diaromatic hydrocarbons and the lowest relative abundance of triaromatic hydrocarbons in all the oil samples in this study.The relative abundance of diaromatic and triaromatic hydrocarbons in the saline lacustrine oils from Qaidam Basin is between that in Tarim oils and Turpan oils.Aromatic parameters based on the isomer distributions of dimethylnaphthalenes(DMN),trimethylnaphthalenes(TMN),tetramethylnaphthalenes(TeMN) and methylphenanthrenes(MP),i.e.,1,2,5-trimethylnaphthalene(TMN)/1,3,6-TMN ratio,1,2,7-TMN/1,3,7TMN ratio,(2,6-+2,7-)-dimethylnaphthalenes(DMN)/1,6-DMN ratio,1,3,7-TMN/(1,2,5-+1,3,7-)TMN,1,3,6,7-TeMN/(1,3,6,7-+1,2,5,6-+1,2,3,5-)-TeMN ratio and MP index,may reflect the diversity of organic source input,thermal maturity and depositional environments.In addition,the dibenzothiophenes(DBTs)/fluorenes(Fs) and dibenzofurans(DBFs)/Fs ratios were found to the very useful and effective in determining genetic types of crude oils for the marine,saline lacustrine,and swamp depositional environments,and for oil-oil correlations.展开更多
文摘The Fengcheng Formation is a crucial source rock and the primary reservoir for oil accumulation in the Mahu Sag.Crude oils are distributed throughout the Fengcheng Formation,ranging from the edge to the interior of the sag in the southern Mahu Sag.These crude oils originate from in-situ source rocks in shallowly buried areas and the inner deep sag.During migration,the crude oil from the inner deep sag affects the source rocks close to carrier beds,leading to changes in the organic geochemical characteristics of the source rocks.These changes might alter source rock evaluations and oil-source correlation.Based on data such as total organic carbon(TOC),Rock-Eval pyrolysis of source rocks,and gas chromatography-mass spectrometry(GC-MS)of the saturated fraction,and considering the geological characteristics of the study area,we define the identification characteristics of source rock affected by migrated hydrocarbons and establish the various patterns of influence that migrated hydrocarbons have on the source rock of the Fengcheng Formation in the southern Mahu Sag.The source rocks of the Fengcheng Formation are mostly fair to good,containing mainly Type II organic matter and being thermally mature enough to generate oil.Source rocks affected by migrated hydrocarbons exhibit relatively high hydrocarbon contents(S1/TOC>110 mg HC/g TOC,Extract/TOC>30%,HC:hydrocarbon),relatively low Rock-Eval Tmax values,and relatively high tricyclic terpane contents with a descending and mountain-shaped distribution.Furthermore,biomarker composition parameters indicate a higher thermal maturity than in-situ source rocks.Through a comparison of the extract biomarker fingerprints of adjacent reservoirs and mudstones in different boreholes,three types of influence patterns of migrated hydrocarbons are identified:the edge-influence of thin sandstone-thick mudstone,the mixed-influence of sandstone-mudstone interbedded,and the full-influence of thick sandstone-thin mudstone.This finding reminds us that the influence of migrated hydrocarbons must be considered when evaluating source rocks and conducting oil-source correlation.
基金supported by the National Natural Science Foundation of China(21401099)the Natural Science Foundation of Shanxi Province(202203021212331)+3 种基金Science and Technology Innovation Project of Colleges and Universities of Shanxi Province(2022L532)the National Natural Science Foundation of Anhui Province(2008085MB32 and KJ2021ZD0073)Natural Science Foundation of Shandong Province(ZR2021QB159)supported by the Talent Program Foundation of Dezhou University(2021xjrc102)。
文摘Methane(CH_(4))as a substitute for other mineral fuels plays a crucial role in reducing energy consumption and preventing environmental pollution.The present study employs a solvothermal method to fabricate a porous framework Co-metal-organic framework(Co-MOF)containing two distinct secondary building units(SBUs):an anionic[Co_(2)(μ_(2)-OH)(COO)_(4)(H_(2)O)]and a neutral[CoN_(2)(COO)_(2)].Notably,within the anionic SBUs,the coordinated water molecules induce the generation of divergent unsaturated Co(Ⅱ)centers in the unidirectional porous channels,thereby creating open metal sites.The adsorption performance of Co-MOF towards pure component gases was systematically investigated.The results demonstrated that Co-MOF exhibits superior adsorption capacity for C_(2)-C_(3) hydrocarbons compared to CH_(4),which offers the potential for efficient adsorption and separation of CH_(4) from C_(2)-C_(3) hydrocarbons.The gas selectivity separation ratios of Co-MOF for C_(2)H_(6)/CH_(4) and C_(3)H_8/CH_(4) were calculated using the ideal adsorbed solution theory method at 273/298 K and 0.1 MPa.The results revealed that Co-MOF achieved remarkable equilibrium separation selectivity for CH_(4) and C_(2)-C_(3) hydrocarbon gases among non-modified MOFs,signifying the potential of the synthesized Co-MOF for efficient recovery and purification of CH_(4) from C_(2)-C_(3) hydrocarbons.Breakthrough experiments further demonstrate the ability of Co-MOF to purify methane from C_(2)-C_(3) hydrocarbons in practical gas separation scenarios.Additionally,molecular simulation calculations further substantiate the propensity of anionic SBUs to interact with C_(2)-C_(3) hydrocarbon compounds.This study provides a novel paradigm for the development of porous MOF materials in the application of gas mixture separation.
基金partly supported by grants from the National Natural Science Foundation of China(No:81372955)BiosTime Maternal and Infant Nutrition and Health Research Fund(2017FYH008)+1 种基金the Projects of Medical and Health Technology Development Program in Shandong Province(No:2016WS0309)Qingdao Outstanding Health Professional Development Fund(2020-2022,2022-2024)。
文摘Objective To investigate changes in the urinary metabolite profiles of children exposed to polycyclic aromatic hydrocarbons(PAHs)during critical brain development and explore their potential link with the intestinal microbiota.Methods Liquid chromatography-tandem mass spectrometry was used to determine ten hydroxyl metabolites of PAHs(OH-PAHs)in 36-month-old children.Subsequently,37 children were categorized into low-and high-exposure groups based on the sum of the ten OH-PAHs.Ultra-high-performance liquid chromatography coupled with quadrupole time-of-flight mass spectrometry was used to identify non-targeted metabolites in the urine samples.Furthermore,fecal flora abundance was assessed by 16S rRNA gene sequencing using Illumina MiSeq.Results The concentrations of 21 metabolites were significantly higher in the high exposure group than in the low exposure group(variable importance for projection>1,P<0.05).Most of these metabolites were positively correlated with the hydroxyl metabolites of naphthalene,fluorine,and phenanthrene(r=0.336–0.531).The identified differential metabolites primarily belonged to pathways associated with inflammation or proinflammatory states,including amino acid,lipid,and nucleotide metabolism.Additionally,these distinct metabolites were significantly associated with specific intestinal flora abundances(r=0.34–0.55),which were mainly involved in neurodevelopment.Conclusion Higher PAH exposure in young children affected metabolic homeostasis,particularly that of certain gut microbiota-derived metabolites.Further investigation is needed to explore the potential influence of PAHs on the gut microbiota and their possible association with neurodevelopmental outcomes.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIP)(NRF,2021R1C1C1013953,2022K1A4A7A04094394,2022K1A4A7A04095890)。
文摘The electrochemical reduction of carbon dioxide offers a sound and economically viable technology for the electrification and decarbonization of the chemical and fuel industries.In this technology,an electrocatalytic material and renewable energy-generated electricity drive the conversion of carbon dioxide into high-value chemicals and carbon-neutral fuels.Over the past few years,single-atom catalysts have been intensively studied as they could provide near-unity atom utilization and unique catalytic performance.Single-atom catalysts have become one of the state-of-the-art catalyst materials for the electrochemical reduction of carbon dioxide into carbon monoxide.However,it remains a challenge for single-atom catalysts to facilitate the efficient conversion of carbon dioxide into products beyond carbon monoxide.In this review,we summarize and present important findings and critical insights from studies on the electrochemical carbon dioxide reduction reaction into hydrocarbons and oxygenates using single-atom catalysts.It is hoped that this review gives a thorough recapitulation and analysis of the science behind the catalysis of carbon dioxide into more reduced products through singleatom catalysts so that it can be a guide for future research and development on catalysts with industry-ready performance for the electrochemical reduction of carbon dioxide into high-value chemicals and carbon-neutral fuels.
基金supported by the Russian Science Foundation under grant(Project No.19-16-00113).
文摘Natural wax gelators have different compositions of compounds(hydrocarbons,wax esters,free fatty alcohols,and free fatty acids),which results in oleogels with varying properties.To maintain a consistent composition,the individual components can be added to the original wax gelator.The content of hydrocarbons and wax esters greatly affects the structuring process of liquid edible oils with waxes.The aim of this study was to evaluate the possibility of modifying the properties of beeswax as a gelling agent by adding hydrocarbons or monoesters to obtain oleogels with specific properties.Various tests were conducted to assess the changes in the oleogel properties,such as color,microstructure,oil-binding capacity,thermal and textural properties.The research results have shown that the addition of the studied fractions has led to a significant change in all properties of oleogels.The initial size of oleogel crystals(7.29±1.80μm)changed after adding fractions,varying from 5.28μm to 12.58μm with hydrocarbons and from 9.95μm to 30.41μm with wax esters.The addition of 30%–50% hydrocarbons decreased the ability of the oleogels to bind oil and made them less firm compared to samples with 10%-20% hydrocarbons.Adding 10%-20% monoesters increased the firmness of the oleogels,but this indicator decreased when their content was increased to 50%.The obtained data indicate that hydrocarbons and wax esters can be used for targeted correction of the gelling properties of beeswax.
基金the Technology Research Project(LGF22D060003)Zhoushan Municipal Science and Technology Cooperation(Active Design)Project(2023C13015).
文摘Polycyclic aromatic hydrocarbons(PAHs)are typical persistent organic pollutants(POPs)that are commonly found in the environment.They are carcinogenic,teratogenic,mutagenic and biodegradable obviously.In this paper,the modified mussel shells were used to adsorb and remove anthracene.The results show that the adsorption removal rate of the mussel shells was higher after calcination at 600℃.5%H_(3)PO_(4) solution was more suitable for shell treatment than 3 mol/L ZnCl_(2) solution.As the dosage of the modified shells was 0.5 g/L,the adsorption reached a stable state,and the removal rate of PAHs was about 69.44%;the adsorption efficiency rose with the increase of time.It can be seen that as a new and cheap biological adsorbent,the modified shells can be used to remove PAHs from wastewater.
基金Supported by the National Natural Science Foundation of China(42172149,U2244209)Sinopec Science and Technology Research Project(P23230,P22132)。
文摘Based on the analysis of light hydrocarbon compositions of natural gas and regional comparison in combination with the chemical components and carbon isotopic compositions of methane,the indication of geochemical characteristics of light hydrocarbons on the migration features,dissolution and escape of natural gas from the Dongsheng gas field in the Ordos Basin is revealed,and the effect of migration on specific light hydrocarbon indexes is further discussed.The study indicates that,natural gas from the Lower Shihezi Formation(Pix)in the Dongsheng gas field displays higher iso-C5-7contents than n-C5-7contents,and the C6-7light hydrocarbons are composed of paraffins with extremely low aromatic contents(<0.4%),whereas the C7light hydrocarbons are dominated by methylcyclohexane,suggesting the characteristics of coal-derived gas with the influence by secondary alterations such as dissolution.The natural gas from the Dongsheng gas field has experienced free-phase migration from south to north and different degrees of dissolution after charging,and the gas in the Shiguhao area to the north of the Borjianghaizi fault has experienced apparent diffusion loss after accumulation.Long-distance migration in free phase results in the decrease of the relative contents of the methylcyclohexane in C7 light hydrocarbons and the toluene/n-heptane ratio,as well as the increase of the n-heptane/methylcyclohexane ratio and heptane values.The dissolution causes the increase of isoheptane values of the light hydrocarbons,whereas the diffusion loss of natural gas in the Shiguhao area results in the increase of n-C5-7contents compared to the iso-C5-7contents.
基金partially funded by the GTCLC-NEG project,which received funding from the European Union’s Horizon 2020 Research and Innovation Programme under the Marie Sklodowska-Curie Grant Agreement (101018756)the Brisk 2 European project (731101)for funding this project.The project acronym was B2PB-SIN2-1001,and the project title was“Optimization of catalytic pyrolysis of digestate and sewage sludge.”。
文摘Catalytic pyrolysis of digestate to produce aromatic hydrocarbons can be combined with anaerobic fermentation to effectively transform and utilize all biomass components,which can achieve the meaningful purpose of transforming waste into high-value products.This study explored whether catalytic pyrolysis of digestate is feasible to prepare aromatic hydrocarbons by analyzing the thermogravimetric characteristics,pyrolysis characteristics,and catalytic pyrolysis characteristics of digestate.For digestate pyrolysis,an increase in temperature was found to elevate the CO,CH_4,and monocyclic aromatic hydrocarbon(benzene,toluene,and xylene;BTX)content,whereas it decreased the contents of phenols,acids,aldehydes,and other oxygenates.Furthermore,the catalytic pyrolysis process effectively inhibited the acids,phenols,and furans in the liquid,whereas the yield of BTX increased from 25.45%to 45.99%,and the selectivity of xylene was also increased from 10.32%to 28.72%after adding ZSM-5.ZSM-5 also inhibited the production of nitrogenous compounds.
文摘Polycyclic aromatic hydrocarbons(PAHs)are one of the most important groups in oil,and re sponsible for major toxic and/or carcinogenic impact on humans and wildlife.It is important to understand the behavior of PAHs in marine environment after an oil-spill incident.However,interaction between petroleum PAHs and microbial communities in a marine environment remains unclear.Therefore,a series of mesocosm experiments were conducted.in which water-accommodated fraction(WAF)of oil was generated to simulate an oil-spill scenario and to analyze the transport and behavior of marine oil spill containing PAHs with and without dispersants.Results indicate that the application of dispersant could increase the concentration of total PAHs in water column due mainly to significant increase in the concentration of highmolecular weight(HMW)PAHs at a lower removal rate.At the end of the 7-day experiment,significant amount of HMW PAHs were accumulated in sediment.In general,the application of dispersant did not increase the sediment uptake of PAHs but increased the PAHs concentration in water column.
基金funded by the National Key R&D Program of China(2016YFD040040303).
文摘Coriander(Coriandrum sativum L.)is recognized for its antioxidant property,as a kind of natural phenolic-rich ingredient.Polycyclic aromatic hydrocarbons(PAHs)present a class of heat-driven hazards in foods,especially the processed meat.In this study,the effect of coriander root and leaf extract on the formation and inhibition of PAH8 in roasted duck wings was firstly investigated.Coriander root extract(CRE)and coriander leaf extract(CLE)with five concentration groups(200,400,600,800,1000 mg/L)were prepared respectively to marinate the duck wings.CRE marinade exhibited greater inhibitory effect on PAH8 formation in roasted duck wings that ranged from 65.0%-87.4%.The electron spin resonance study indicated a significantly positive correlation between PAH8 and free radical level,suggesting the participation of radicals in PAHs formation.Also,it was speculated that the inhibitory effect on PAH8 was related to the phenolic compounds identified in coriander marinades.CRE made greater inhibitory effect on the formation of PAH8 and could be considered as a kind of natural source to mitigate PAHs in heat-processed meat products.
基金This work was supported by the National Natural Science Foundation of China(No.51979255).
文摘The knowledge of the existence,distribution and fate of polycyclic aromatic hydrocarbons(PAHs)and substituted polycyclic aromatic hydrocarbons(SPAHs)in wastewater treatment plants(WWTPs)was vital for reducing their concentrations entering the aquatic environment.The concentrations of 13 SPAHs and 16 PAHs were all determined in a WWTP with styrene butadiene rubber(SBR)in partnership with the moving bed biofilm reactor(MBBR)process.SPAHs presented a higher concentration lever than PAHs in nearly all samples.The total removal efficiencies of PAHs and SPAHs ranged from 64.0%to 71.36%and 78.4%to 79.7%,respectively.The total yearly loads of PAHs(43.0 kg)and SPAHs(73.0 kg)were mainly reduced by the primary and SBR/MBBR biological treatment stages.The tertiary treatment stage had a minor contribution to target compounds removal.According to a synthesis and improvement fate model,we found that the dominant processes changed as the chemical octanol water partition coefficient(K_(ow))increased.But the seasonal variations of experimental removal efficiencies were more obvious than that of predicted data.In the primary sedimentation tank,dissolution in the aqueous phase and sorption to sludge/particulate matter were controlling processes for the removal of PAHs and SPAHs.The sorption to sludge and biodegradation were the principal removal mechanisms during the SBR/MBBR biological treatment process.The contribution of volatilization to removal was always insignificant.Furthermore,the basic physicochemical properties and operating parameters influenced the fate of PAHs and SPAHs in the WWTP.
基金financial support from the National Natural Science Foundation of China(21991092,21991090,22022202,21972142,21902153,21974138)the Chinese Academy of Sciences(QYZDY-SSW-SC024)the Dalian Institute of Chemical Physics(DICP I201926,DICP I201947)。
文摘Low-carbon process for resource utilization of polycyclic aromatic hydrocarbons(PAHs)in zeolitecatalyzed processes,geared to carbon neutrality-a prominent trend throughout human activities,has been bottlenecked by the lack of a complete mechanistic understanding of coking and decoking chemistry,involving the speciation and molecular evolution of PAHs,the plethora of which causes catalyst deactivation and forces regeneration,rendering significant CO_(2) emission.Herein,by exploiting the high-resolution matrix-assisted laser desorption/ionization Fourier-transform ion cyclotron resonance mass spectrometry(MALDI FT-ICR MS),we unveil the missing fingerprints of the mechanistic pathways for both formation and decomposition of cross-linked cage-passing PAHs for SAPO-34-catalyzed,industrially relevant methanol-to-olefins(MTO)as a model reaction.Notable is the molecule-resolved symmetrical signature:their speciation originates exclusively from the direct coupling of in-cage hydrocarbon pool(HCP)species,whereas water-promoted decomposition of cage-passing PAHs initiates with selective cracking of inter-cage local structures at 8-rings followed by deep aromatic steam reforming.Molecular deciphering the reversibly dynamic evolution trajectory(fate)of full-spectrum aromatic hydrocarbons and fulfilling the real-time quantitative carbon resource footprints advance the fundamental knowledge of deactivation and regeneration phenomena(decay and recovery motifs of autocatalysis)and disclose the underlying mechanisms of especially the chemistry of coking and decoking in zeolite catalysis.The positive yet divergent roles of water in these two processes are disentangled.These unprecedented insights ultimately lead us to a steam regeneration strategy with valuable CO and H_(2) as main products,negligible CO_(2) emission in steam reforming and full catalyst activity recovery,which further proves feasible in other important chemical processes,promising to be a sustainable and potent approach that contributes to carbon-neutral chemical industry.
文摘Polycyclic aromatic hydrocarbons (PAHs) are strongly associated with agricultural, residential, transportation, industrial and petroleum activities. In this study, the presence of PAHs (polycyclic aromatic hydrocarbons) was investigated in sediments of the ivory coastal zone (Toukouzou Hozalem-Assinie). The main objectives of this study were to determine the abundance and to predict the source of PAHs in the sediments. Gas chromatography-mass spectrometry (GC-MS) was used to analyze sixteen priority PAHs. Total PAHs concentrations were from 1.31 to 3992.68 mg/kg in sediment with an average concentration of (307.54 ± 16.10) mg/kg. Among all PAHs, Naphthalene (Nap = 332.72 mg/kg) and Phenanthrene (Phe = 41.75 mg/kg) were found in the highest concentration, whereas Benzo (k) Fluoranthene was found in the least concentration in the range of 0 - 0.85 mg/kg (mean 0.24 mg/kg). Bassam-Modeste Lagune (BML) sampling site was the site with the highest concentration of total PAHs (all 16 PAHs) compared to the others due to their location in a highly populated estuary area that receives commercial, tourism, port, petroleum and heavy industrial activities. Diagnostic ratios were used to determine the sources of PAHs and suggested that the PAH profile in the sediments was dominated by 2 and 3 ring PAHs. The patterns of PAH compounds in sediment indicated that contamination is from mixed sources, with a strong indication of petrogenic contamination potentially from spills of fuel, oil and industrial activities.
基金Supported by the National Natural Science Foundation of China(U22B6004)the PetroChina Research Institute of Petroleum Exploration&Development Project(2022yjcq03).
文摘The geological characteristics and production practices of the major middle-and high-maturity shale oil exploration areas in China are analyzed.Combined with laboratory results,it is clear that three essential conditions,i.e.economic initial production,commercial cumulative oil production of single well,and large-scale recoverable reserves confirmed by the testing production,determine whether the continental shale oil can be put into large-scale commercial development.The quantity and quality of movable hydrocarbons are confirmed to be crucial to economic development of shale oil,and focuses in evaluation of shale oil enrichment area/interval.The evaluation indexes of movable hydrocarbon enrichment include:(1)the material basis for forming retained hydrocarbon,including TOC>2%(preferentially 3%-4%),and typeⅠ-Ⅱkerogens;(2)the mobility of retained hydrocarbon,which is closely related to the hydrocarbon composition and flow behaviors of light/heavy components,and can be evaluated from the perspectives of thermal maturity(Ro),gas-oil ratio(GOR),crude oil density,quality of hydrocarbon components,preservation conditions;and(3)the reservoir characteristics associated with the engineering reconstruction,including the main pore throat distribution zone,reservoir physical properties(including fractures),lamellation feature and diagenetic stage,etc.Accordingly,13 evaluation indexes in three categories and their reference values are established.The evaluation indicates that the light shale oil zones in the Gulong Sag of Songliao Basin have the most favorable enrichment conditions of movable hydrocarbons,followed by light oil and black oil zones,containing 20.8×10^(8) t light oil resources in reservoirs with R_(0)>1.2%,pressure coefficient greater than 1.4,effective porosity greater than 6%,crude oil density less than 0.82 g/cm^(3),and GOR>100 m/m^(3).The shale oil in the Gulong Sag can be explored and developed separately by the categories(resource sweet spot,engineering sweet spot,and tight oil sweet spot)depending on shale oil flowability.The Gulong Sag is the most promising area to achieve large-scale breakthrough and production of continental shale oil in China.
基金supported by the National Natural Science Foundation of China (22008098, 21978156, 42002040)the Program for Innovative Research Team (in Science and Technology) in University of Henan Province (21IRTSTHN004)+1 种基金the Program for Science & Technology Innovation Talents in Universities of Henan Province (22HASTIT008)the Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering (2022-K34)。
文摘Catalytic hydrogenation of CO_(2) using renewable hydrogen not only reduces greenhouse gas emissions,but also provides industrial chemicals.Herein,a Co-Fe bimetallic catalyst was developed by a facile reactive ball-milling method for highly active and selective hydrogenation of CO_(2) to value-added hydrocarbons.When reacted at 320℃,1.0 MPa and 9600 mL h^(-1) g_(cat)^(-1),the selectivity to light olefin(C_(2)^(=)-C_(4)^(=)) and C_(5)+ species achieves 57.3% and 22.3%,respectively,at a CO_(2) co nversion of 31.4%,which is superior to previous Fe-based catalysts.The CO_(2) activation can be promoted by the CoFe phase formed by reactive ball milling of the Fe-Co_(3)O_(4) mixture,and the in-situ Co_(2)C and Fe_(5)C_(2) formed during hydrogenation are beneficial for the C-C coupling reaction.The initial C-C coupling is related to the combination of CO species with the surface carbon of Fe/Co carbides,and the sustained C-C coupling is maintained by self-recovery of defective carbides.This new strategy contributes to the development of efficient catalysts for the hydrogenation of CO_(2) to value-added hydrocarbons.
基金supported by the National Natural Science Foundation of China(grants No.41972163 and 42173055).
文摘Three kerogen samples(JJZG-1,JJZG-2 and JJZG-3)isolated from the Permian Lucaogou shales of varying biodegradation levels(BLs≈0,3 and 7,respectively)were subjected to sequential stepwise pyrolysis combined with on-line detection of gas chromatography-mass spectrometry(GC-MS).Occluded fractions(bitumenⅡ)released at low-temperature steps(≥410℃)show consistent biodegradative signatures with that reported for solvent-extracted fractions(bitumenⅠ)of the original shales,e.g.,broad range of abundant n-alkanes,isoprenoids and regular hopanes for the non-biodegraded JJZG-1;trace n-alkanes and abundant hopanes for the moderately biodegraded JJZG-2;and no n-alkanes but still prominent hopanes including the microbially produced 25-nohopanes for the severely biodegraded JJZG-3.This consistency between bitumenⅡand bitumenⅠfractions indicates the biodegradability of the kerogenoccluded bitumenⅡwith limited protection from host kerogen.A minor level of protection was suggested by the trace distribution of n-alkanes in the bitumenⅡof JJZG-2,whereas the bitumenⅠhad no nalkanes.The kerogen itself was more resistant to biodegradation as reflected by the persistence of high abundances of both n-alkanes and hopanes in the high temperature(≥460℃)products of all three kerogen samples.However,the relative abundances of these product groups did show some evidence of biodegradation alteration,e.g.,ratios of n-C_(15)alkene/C_(27)hop-17(21)-ene at 510℃pyrolysis decreased by order of magnitude from the non-biodegraded(JJZG-1=27.4)to highly biodegraded(0.3 for JJZG-3)samples.The reduced biodegradation impact on the kerogen fraction(Cf.bitumen fractions)was also evident by the absence of 25-norhopanes in the high-temperature analysis of the JJZG-3 kerogen.
文摘The influence of origin, depositional environment and thermal maturity of organic matter on the occurrence of aromatic hydrocarbons in source rocks from the central and northwestern Niger Delta was investigated. Eighty two source rock samples from four oil wells in the central and northwestern Niger Delta were analyzed for the aromatic hydrocarbon content using gas chromatography-mass spectrometry (GC-MS). The results of analysis of aromatic hydrocarbon fractions of the source rock extracts show the presence of many classes of aromatic hydrocarbons, which include naphthalenes, phenanthrenes, biphenyls, dibenzothiophenes and fluorenes. Trimethylnaphthalene (TMN) is the most abundant among the naphthalenes while dimethylphenanthrene (DMP) is the most abundant among the phenanthrenes. Among the biphenyls, 3-methylbiphenyl (3 MB) is the most abundant while 4-methyldibenzothiophene (4MDBT) is the most abundant among the dibenzothiphenes. Only two fluorenes were detected, and fluorene is more in abundance than 1-methylfluorene (1 MF). Depositional environment indicators of aromatic hydrocarbon organic matter reveal that the organic materials in the source rocks in these wells were deposited in marine-to-swamp depositional environments under reducing to suboxic conditions. Thermal maturity indicators calculated from the abundance of the aromatic hydrocarbons indicate that the source rock samples are thermally mature. Most of the source rocks are at the peak of oil window while a few at the early oil window. Source rocks from wells GB, OP and OT in the central Niger Delta are thermally more mature than those from well AW in the northwestern Niger Delta.
基金funded by National Natural Science Foundation of China(Grant No.42072149)support of US National Science Foundation grant(Grant No.EAR-1255724)。
文摘Despite the upsurge in hydrocarbon exploration in the Lake Albert Rift Basin(LARB)over the past three decades,systematic characterization of hydrocarbon compositions remains lacking,leading to uncertainties in source rock and oil generation determination.We characterized crude oil compositions and oil sand samples in the northern and southern subbasins of LARB.The relative abundance of normal and branched linear alkanes,hopanes,steranes,and aromatic hydrocarbon suggest that northern and southern hydrocarbons were deposited in anoxic to suboxic lacustrine environments and share similar biological source compositions(i.e.,a mixture of plants and aquatic algae and bacteria).Relative to southern samples,northern samples show more negative δ^(13)C values for oils,saturates and aromatics,indicating longer migration paths,and exhibit higher MPI-1,DNR-1 and 4-/1-MDBT ratios,indicating higher maturity.Between the two possible sets of source rocks(upper Miocene and Jurassic strata),the positive δ^(13)C values of saturated hydrocarbons(average=-20.5‰)suggest that the upper Miocene lacustrine shale is the most likely candidate.Oleanane index(<5% in our samples)does not exclude either source rock possibility,and C_(28)/C_(29) regular sterane(average=0.63)may be biased by high terrestrial inputs in a lacustrine setting.Together,our data show that northern and southern oils originate from the same source rocks but different oil kitchens.Given the similar geochemical characteristics of southern and northern oils,previous exploration successes in the northern subbasin likely suggest similar potential in the southern sector,while other elements influencing exploration success must be also evaluated.
基金supported by the National NaturalScience Foundation of China (No. 40473045)
文摘The contents and distribution of 20 polycyclic aromatic hydrocarbons (PAHs) and heterocyclic aromatic hydrocarbons (HAHs) were investigated in 16 soil profiles of Beijing and Tianjin region. Transport of high molecular weight PAHs (HMWPAHs) and the correlation between total organic carbon (TOC) and their concentrations were also discussed. The results indicated that highly contaminated sites were located at urban or wastewater irrigation areas and pollutants mainly accumulated in topsoil (〈 40 cm), with a sharp content decrease at the vertical boundary of 30-40 cm. Total PAHs/HAHs concentrations in soils from Tianjin were markedly greater than those from Beijing. Even the contents at bottoms of soil profiles in Tianjin were higher than those in topsoils of Beijing soil profile. HMWPAHs dominated the PAH profiles, exhibiting a uniform distribution of pyrogenic origin between topsoils and deep layers. Furthermore, the percentages of HMWPAHs remained relative constant with the depth of soil profiles, which were consistent with the distribution of particulate matter-associated PAHs in the local atmospheric environments. Therefore, HMWPAHs transport with particulates might be the predominant source found in soil profiles.
基金funded by the National Natural Science Foundation of China (Grant No. 40973041)
文摘Based on the systematic study of aromatic hydrocarbons in over 100 crude oil samples collected from the Tabei and Tazhong uplifts in the Tarim Basin,the western depression area in the Qaidam Basin and the Tabei depression in the Turpan Basin,the geochemical characteristics of the marine(Tarim Basin),saline lacustrine(Qaidam Basin),and swamp(Turpan Basin) oils were investigated.The marine oils from the Tarim basin are characterized by relatively low abundance of diaromatic hydrocarbons such as biphenyl and naphthalene,and relatively high abundance of triaromatic hydrocarbons including phenanthrene,dibenzothiophene and fluorene.In contrast,the swamp oils from the Turpan Basin are dominated by the highest relative abundance of diaromatic hydrocarbons and the lowest relative abundance of triaromatic hydrocarbons in all the oil samples in this study.The relative abundance of diaromatic and triaromatic hydrocarbons in the saline lacustrine oils from Qaidam Basin is between that in Tarim oils and Turpan oils.Aromatic parameters based on the isomer distributions of dimethylnaphthalenes(DMN),trimethylnaphthalenes(TMN),tetramethylnaphthalenes(TeMN) and methylphenanthrenes(MP),i.e.,1,2,5-trimethylnaphthalene(TMN)/1,3,6-TMN ratio,1,2,7-TMN/1,3,7TMN ratio,(2,6-+2,7-)-dimethylnaphthalenes(DMN)/1,6-DMN ratio,1,3,7-TMN/(1,2,5-+1,3,7-)TMN,1,3,6,7-TeMN/(1,3,6,7-+1,2,5,6-+1,2,3,5-)-TeMN ratio and MP index,may reflect the diversity of organic source input,thermal maturity and depositional environments.In addition,the dibenzothiophenes(DBTs)/fluorenes(Fs) and dibenzofurans(DBFs)/Fs ratios were found to the very useful and effective in determining genetic types of crude oils for the marine,saline lacustrine,and swamp depositional environments,and for oil-oil correlations.