An innovative classification system for ranking the biological effects of marine aromatic hydrocarbons based on fish embryotoxicity

Petroleum hydrocarbon pollution is a global concern,particularly in coastal environments.Polycyclic aromatic hydrocarbons(PAHs) are regarded as the most toxic components of petroleum hydrocarbons.In this study,the biomonitoring and ranking effects of petroleum hydrocarbons and PAHs on the marine fish model Oryzias melastigma embryos were determined in the Jiulong River Estuary(JRE) and its adjacent waters in China.The results showed that the levels of petroleum hydrocarbons from almost all sites met the primary standard for marine seawater quality,and the concentrations of the 16 priority PAHs in the surface seawater were lower compared with those in other coastal areas worldwide.A new fish expert system based on the embryotoxicity of O.melastigma(OME-FES) was developed and applied in the field to evaluate the biological effects of petroleum hydrocarbons and PAHs.The selected physiological index and molecular indicators in OME-FES were appropriate biomarkers for indicating the harmful effects of petroleum hydrocarbons and PAHs.The outcome of OME-FES revealed that the biological effect levels of the sampling sites ranged from level Ⅰ(no stress) to level Ⅲ(medium stress),which is further corroborated by the findings of nested analysis of variance(ANOVA) models.Our results suggest that the OME-FES is an effective tool for evaluating and ranking the biological effects of marine petroleum hydrocarbons and PAHs.This method may also be applied to evaluate other marine pollutants based on its framework.

Single-atom catalysts for the electrochemical reduction of carbon dioxide into hydrocarbons and oxygenates

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.

Geochemical identification of a source rock affected by migrated hydrocarbons and its geological significance:Fengcheng Formation,southern Mahu Sag,Junggar Basin,NW China

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.

Changes in the Non-targeted Metabolomic Profile of Three-year-old Toddlers with Elevated Exposure to Polycyclic Aromatic Hydrocarbons

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.

Efficient adsorption separation of methane from C_(2)-C_(3) hydrocarbons in a Co(Ⅱ)-nodes metal-organic framework

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.

Mitigation of polycyclic aromatic hydrocarbons(PAHs)in roasted beef patties by cold plasma treatment and products quality evaluation

The cold plasma(CP)technique was applied to alleviate the contamination of polycyclic aromatic hydrocarbon(PAH)in this investigation.Two different CP treatments methods were implemented in the production of beef patties,to investigate their inhibition and degradation capacity on PAHs.With 5 different cooking oils and fats addition,the inhibition mechanism of in-package cold plasma(ICP)pretreatment was explored from the aspect of raw patties fatty acids composition variation.The results of principal component analysis showed that the first two principal components accounted for more than 80%of the total variation in the original data,indicating that the content of saturated fatty acids was significantly positively correlated with the formation of PAHs.ICP pretreatment inhibited the formation of PAHs by changing the composition of fatty acids,which showed that the total amount of polyunsaturated fatty acids decreased and the total amount of monounsaturated fatty acids increased.Sensory discrimination tests demonstrated there were discernable differences between 2 CP treated samples and the controls,utilization of the ICP pretreatment in meat products processing was expected to achieve satisfying eating quality.In conclusion,CP treatment degraded PAHs through stepwise ring-opening oxidation in 2 reported pathways,the toxicity of PAHs contaminated products was alleviated after CP treatment.

Investigation of the effect of hydrocarbons and monoesters in the gelators’composition on the properties of edible oleogel

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.

Study on Adsorption Removal of Polycyclic Aromatic Hydrocarbons by Modified Mussel Shells

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.

Eco-toxicity and health risk assessment of polycyclic aromatic hydrocarbons in surface sediments of Burullus Lake in Egypt

Polycyclic aromatic hydrocarbons(PAHs)are ubiquitous environmental contaminants of growing concern due to their potential ecological and human health risks.This study presents a comprehensive assessment of PAHs contamination in the surface sediments of Burullus Lake,a vital and second largest delta lake in Egypt.The aim was to evaluate the eco-toxicity and potential health risks associated with the presence of these compounds.Surface seven sediment samples were collected from various drains in the southern part of Burullus Lake.Soxhlet extraction method was employed to extract PAHs(16PAHs)from the sediment sample.Analytically,target compounds were located using HPLC.The results showed that samples contained PAHs levels ranging from 0.038×10^(-6)to 0.459×10^(-6),which is considered heavily polluted by the European standard for PAHs pollution.Additionally,there was no apparent source of PAHs in the ElKhashah drain or the Brinbal Canal,as HPLC found none of the compounds.The most prevalent compound in sediment samples along the study area was fluoranthene.The diagnostic indices in the present study indicated that the hydrocarbons in the region originated from pyrolytic and man-made sources along the drains of Burullus Lake.The principal component analysis(PCA)and diagnostic ratios revealed that coal combustion and pyrolytic sources were responsible for the PAHs contamination in the surface sediments.The non-carcinogenic risk(HI),which is the product of the HQs for the adult and child populations,respectively,was calculated.HI values under 1,therefore,demonstrated that they had no carcinogenic effects on human health.TEQs and MEQs in the sediments of Burullus Lake do not have a cancer-causing impact on people.For the safety of nearby wildlife,aquatic life,and people,all activities that raise petroleum hydrocarbon levels in Burullus Lake must be adequately regulated and controlled.According to the ecological risk assessment,there is little chance that PAHs will be found in the sediments of Burullus Lake.This study underscores the urgent need for effective pollution control measures and regular monitoring of PAHs levels in Burullus Lake sediments to protect the aquatic ecosystem and public health.It also highlights the importance of considering eco-toxicity and human health risks in integrated risk assessments of PAHs-contaminated environments.

Gas source of the Middle Jurassic Shaximiao Formation in the Zhongjiang large gas field of Western Sichuan Depression:Constraints from geochemical characteristics of light hydrocarbons

The Zhongjiang gas field is a typical large gas field in terrigenous strata of the Western Sichuan Depression.It remains debatable which member of the Upper Triassic Xujiahe Formation served as the source rocks and how significant the member contributed to the gas accumulations in the Zhongjiang gas field.In this study,we analyzed the essential characteristics of the Lower Jurassic source rocks and the geochemical features of light hydrocarbons in natural gas from the 2nd(T_(3)χ^(2))and 4th members(T_(3)χ^(4))of the Upper Triassic Xujiahe Formation(T_(3)χ),as well as the Middle Jurassic Shaximiao(J_(2)s)and Qianfoya(J_(2)q)formations.Based on this,we explored the sources of the natural gas in the Zhongjiang gas field and determined the natural gas migration patterns and their effects on the properties of light hydrocarbons in the natural gas.The results indicate that the Lower Jurassic lacustrine source rocks of the Zhongjiang gas field contain humic organic matter,with vitrinite reflectance(R_(0))values ranging from 0.86%to 0.98%.Samples meeting the criterion for effective source rocks[total organic carbon(TOC)content≥0.75%]exhibited an average TOC content of merely 1.02%,suggesting significantly lower hydrocarbon generation potential than source rocks in the underlying T3x,which show higher thermal maturity and TOC contents.For natural gas samples from T_(3)χ^(2),T_(3)χ^(4),J_(2)s,and J_(2)q reservoirs,their C_(5-7)iso-alkane content was significantly higher than their n-alkane content,and their methylcyclohexane(MCH)index ranged from 59.0%to 77.3%,indicating the predominance of methylcyclohexane in C_(7)light hydrocarbons.As indicated by the origin identification and gas-source correlation based on the geochemical features of light hydrocarbons,the natural gas in the Zhongjiang gas field is typical coal-derived gas.The gas from the primary pay zone of the Shaximiao Formation,with significantly high K_(1),(P_(2)+N_(2))/C_(7),and P_(3)/C_(7)values,predominantly originated from the 5th member of the T3x and migrated in the free phase,with a small amount possibly sourced from the Lower Jurassic source rocks.The dissolution and adsorption during gas migration led to a decrease in the aromatic content in C_(6-7)light hydrocarbons and an increase in the isoheptane values.Therefore,their effects must be considered when determining the gas origin and thermal maturity based on the aromatic content in C_(6-7) light hydrocarbons and iso-heptane values.

Tracing of natural gas migration by light hydrocarbons:A case study of the Dongsheng gas field in the Ordos Basin,NW China

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.

Preparation of aromatic hydrocarbons from catalytic pyrolysis of digestate

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.

Inhibitory effect of coriander(Coriandrum sativum L.)extract marinades on the formation of polycyclic aromatic hydrocarbons in roasted duck wings

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.

Transport and behavior of marine oil spill containing polycyclic aromatic hydrocarbons in mesocosm experiments

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.

Abundance and Source Identification of Polycyclic Aromatic Hydrocarbons in Sediments of the Ivory Coastal Zone (Toukouzou Hozalem-Assinie)

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.

Fate of Parent and Substituted Polycyclic Aromatic Hydrocarbons in SBR/MBBR Treatment Process:Experimental Value Against Model Prediction

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.

Coking and decoking chemistry for resource utilization of polycyclic aromatic hydrocarbons(PAHs)and low-carbon process

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.

Enrichment factors of movable hydrocarbons in lacustrine shale oil and exploration potential of shale oil in Gulong Sag,Songliao Basin,NE China

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.

Reactive ball-milling synthesis of Co-Fe bimetallic catalyst for efficient hydrogenation of carbon dioxide to value-added hydrocarbons

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.

Source rock geochemistry of central and northwestern Niger Delta: Inference from aromatic hydrocarbons content

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.