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
The hydrocarbon accumulation coefficient is a key parameter in resources evaluation by genetic techniques. Methods of obtaining its value scientifically have always been an important factor influencing evaluation cred...The hydrocarbon accumulation coefficient is a key parameter in resources evaluation by genetic techniques. Methods of obtaining its value scientifically have always been an important factor influencing evaluation credibility. In this paper, the hydrocarbon accumulation system is evaluated quantitatively by establishing a hierarchy structure model based on an analytical hierarchy process. The hydrocarbon accumulation system of a higher exploration degree is selected as a calibration area and its hydrocarbon accumulation coefficient can be calculated using methods of hydrocarbon generation potential and reservoir-scale sequence. The hydrocarbon accumulation coefficient of a petroleum accumulation system can be gained by analogy of reservoir forming comprehensive evaluation results with the calibration area. The hydrocarbon accumulation coefficient of each petroleum accumulation system in the upper reservoir-forming combination of the Liaohe Western Sag can be obtained with this method. Practice shows that using the analytical hierarchy process to quantitatively evaluate the hydrocarbon accumulation system and then quantitatively predict the hydrocarbon accumulation coefficient decreases the influence of human factors in resources evaluation, and makes the resources assessment more objective and closer to the actual geological condition.展开更多
The formation mechanisms and processes of geochemical anomalies used as proxies in surface geochemistry exploration （SGE） have not been well understood. Previous studies cannot realize 3D measurement of microseeping...The formation mechanisms and processes of geochemical anomalies used as proxies in surface geochemistry exploration （SGE） have not been well understood. Previous studies cannot realize 3D measurement of microseeping hydrocarbons from reservoirs to the surface, which made it difficult to understand the features and pathways of deep hydrocarbon microseepages. Understanding the processes of hydrocarbon microseepages will contribute to the acceptance and effectiveness of surface geochemistry. Based on a simplified geological model of hydrocarbon microseepages, including hydrocarbon reservoir, direct caprock, overlying strata and Quaternary sediments, this work established a 3D experimental system to simulate the mechanisms and processes of deep hydrocarbon microseepes extending to the surface. The dispersive halos of microseeping hydrocarbons in the subsurface were adequately described by using this 3D experimental system. Results indicate that different migration patterns of hydrocarbons above the point gas source within the simulated caprock and overlying strata can be reflected by the ratio of i-butane to n-butane （i-C4/n-C4）, which follow diffusion and infiltration （buoyancy） mechanisms. This is not the case for vertical measurement lines far from the point gas source. A vertical gas flow in the form of a plume was found during hydrocarbon microseepage. For sampling methods, the high-density grid sampling is favorable for delineating prospecting targets. Hydrocarbon infiltration or buoyancy flow occurs in the zones of infiltration clusters, coupling with a diffusion mechanism at the top of the water table and forming surface geochemical anomalies. These results are significant in understanding hydrocarbon microseepage and interpreting SGE data.展开更多
A series of bifunctional catalysts composed of a component for higher alcohol synthesis （Cu-CoMn oxides, CCM） and an acidic zeolite （SAPO-34, ZSM-5, Y, MCM-41） were prepared for production of liquid hydrocarbon di...A series of bifunctional catalysts composed of a component for higher alcohol synthesis （Cu-CoMn oxides, CCM） and an acidic zeolite （SAPO-34, ZSM-5, Y, MCM-41） were prepared for production of liquid hydrocarbon directly from a bio-syngas through a one-stage pro-cess. The effects of zeolite type, zeolite content, Si/Al ratio and preparation method on catalyst texture and its reaction performance were investigated. Higher selectivities and yields of liquid products were obtained by using bifunctional catalysts. The yields of liquid hydrocarbons decreased in the order CCM-ZSM-5〉CCM-SAPO-34〉CCM-Y〉CCM-MCM-41. CCM-ZSM-5 （20wt%, Si/Al=100） prepared by coprecipitation method displayed the optimal catalytic performance with the highest CO conversion （76%） and yield of liquid products （30%）. The catalysts were characterized by N2 adsorption/desorption, NH3-TPD, XRD, and H2-TPR analysis. The results showed that higher speci c surface areas and pore volumes of bifunctional catalysts were achieved by adding zeolites into CuCoMn precursors. Medium pore dimension and moderate acidity in CCM-ZSM-5 were observed, which proba-bly resulted in its excellent reaction performance. Additionally, a higher number of weaker acid sites （weak and/or medium acid sites） were formed by increasing ZSM-5 content in CCM-ZSM-5 or decreasing Si/Al ratio in ZSM-5. It was also seen that metal dispersion was higher and reducibility of metal ions was easier on the CCM-ZSM-5 catalyst prepared by coprecipitation. The higher alcohols-to-hydrocarbon process provides a promising route to hydrocarbon fuels via higher alcohols from syngas or biobased feedstocks.展开更多
Novel coal gangue-based persulfate catalyst(CG-FeCl_(2))was successfully synthesized by the means of calcinating under nitrogen atmosphere with the addition of ferrous chloride tetrahydrate(FeCl_(2)·_(4)H_(2)O).T...Novel coal gangue-based persulfate catalyst(CG-FeCl_(2))was successfully synthesized by the means of calcinating under nitrogen atmosphere with the addition of ferrous chloride tetrahydrate(FeCl_(2)·_(4)H_(2)O).The phase transformation of the prepared materials and gas products during the heating process are thoroughly investigated.It is suggested that ferrous chloride participated in the phase transformation and formed Si-O-Fe bonds.And the main gaseous products are H_(2)O,H_(2),and HCl during the heating process.Besides,the ability of CG-FeCl_(2) to activate peroxymonosulfate(PMS)for catalytic degradation of polycyclic aromatic hydrocarbons(PAHs)and phenol was deeply studied.More than 95%of naphthyl,phenanthrene and phenol were removed under optimizied conditions.In addition,1O_(2),·OH,and SO_(4)·−were involved in the CG-FeCl_(2)/PMS system from the free radical scavenging experiment,where 1O_(2) played a major role during the oxidation process.Furthermore,CG-FeCl_(2)/PMS system exhibited superior stability in a relatively wide pH range and the presence of common anion from related degradation experiments.Overall,the novel CG-FeCl_(2) is an efficient and environmentally friendly catalyst,displaying potential application prospect in the field of PAHs and phenol-contaminated wastewater treatment.展开更多
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supported by the Foundation Projectof State Key Laboratory of Petroleum Resources and Prospecting (PRPDX2008-05)the "973" National Key Basic Research Program (2006CB202308)
文摘The hydrocarbon accumulation coefficient is a key parameter in resources evaluation by genetic techniques. Methods of obtaining its value scientifically have always been an important factor influencing evaluation credibility. In this paper, the hydrocarbon accumulation system is evaluated quantitatively by establishing a hierarchy structure model based on an analytical hierarchy process. The hydrocarbon accumulation system of a higher exploration degree is selected as a calibration area and its hydrocarbon accumulation coefficient can be calculated using methods of hydrocarbon generation potential and reservoir-scale sequence. The hydrocarbon accumulation coefficient of a petroleum accumulation system can be gained by analogy of reservoir forming comprehensive evaluation results with the calibration area. The hydrocarbon accumulation coefficient of each petroleum accumulation system in the upper reservoir-forming combination of the Liaohe Western Sag can be obtained with this method. Practice shows that using the analytical hierarchy process to quantitatively evaluate the hydrocarbon accumulation system and then quantitatively predict the hydrocarbon accumulation coefficient decreases the influence of human factors in resources evaluation, and makes the resources assessment more objective and closer to the actual geological condition.
基金supported by the National Natural Science Foundation of China(grants No.41373121 and 41072099)the scientific and technological project of SINOPEC under Contract No.P05069Support by SINOPEC Key Laboratory of Petroleum Accumulation Mechanisms,China
文摘The formation mechanisms and processes of geochemical anomalies used as proxies in surface geochemistry exploration （SGE） have not been well understood. Previous studies cannot realize 3D measurement of microseeping hydrocarbons from reservoirs to the surface, which made it difficult to understand the features and pathways of deep hydrocarbon microseepages. Understanding the processes of hydrocarbon microseepages will contribute to the acceptance and effectiveness of surface geochemistry. Based on a simplified geological model of hydrocarbon microseepages, including hydrocarbon reservoir, direct caprock, overlying strata and Quaternary sediments, this work established a 3D experimental system to simulate the mechanisms and processes of deep hydrocarbon microseepes extending to the surface. The dispersive halos of microseeping hydrocarbons in the subsurface were adequately described by using this 3D experimental system. Results indicate that different migration patterns of hydrocarbons above the point gas source within the simulated caprock and overlying strata can be reflected by the ratio of i-butane to n-butane （i-C4/n-C4）, which follow diffusion and infiltration （buoyancy） mechanisms. This is not the case for vertical measurement lines far from the point gas source. A vertical gas flow in the form of a plume was found during hydrocarbon microseepage. For sampling methods, the high-density grid sampling is favorable for delineating prospecting targets. Hydrocarbon infiltration or buoyancy flow occurs in the zones of infiltration clusters, coupling with a diffusion mechanism at the top of the water table and forming surface geochemical anomalies. These results are significant in understanding hydrocarbon microseepage and interpreting SGE data.
文摘A series of bifunctional catalysts composed of a component for higher alcohol synthesis （Cu-CoMn oxides, CCM） and an acidic zeolite （SAPO-34, ZSM-5, Y, MCM-41） were prepared for production of liquid hydrocarbon directly from a bio-syngas through a one-stage pro-cess. The effects of zeolite type, zeolite content, Si/Al ratio and preparation method on catalyst texture and its reaction performance were investigated. Higher selectivities and yields of liquid products were obtained by using bifunctional catalysts. The yields of liquid hydrocarbons decreased in the order CCM-ZSM-5〉CCM-SAPO-34〉CCM-Y〉CCM-MCM-41. CCM-ZSM-5 （20wt%, Si/Al=100） prepared by coprecipitation method displayed the optimal catalytic performance with the highest CO conversion （76%） and yield of liquid products （30%）. The catalysts were characterized by N2 adsorption/desorption, NH3-TPD, XRD, and H2-TPR analysis. The results showed that higher speci c surface areas and pore volumes of bifunctional catalysts were achieved by adding zeolites into CuCoMn precursors. Medium pore dimension and moderate acidity in CCM-ZSM-5 were observed, which proba-bly resulted in its excellent reaction performance. Additionally, a higher number of weaker acid sites （weak and/or medium acid sites） were formed by increasing ZSM-5 content in CCM-ZSM-5 or decreasing Si/Al ratio in ZSM-5. It was also seen that metal dispersion was higher and reducibility of metal ions was easier on the CCM-ZSM-5 catalyst prepared by coprecipitation. The higher alcohols-to-hydrocarbon process provides a promising route to hydrocarbon fuels via higher alcohols from syngas or biobased feedstocks.
基金National Key R&D Program of China(2019YFC1904903 and 2020YFC1806504)China Postdoctoral Science Foundation(2020M680757)Fundamental Research Funds for the Central Universities(2022XJHH08).
文摘Novel coal gangue-based persulfate catalyst(CG-FeCl_(2))was successfully synthesized by the means of calcinating under nitrogen atmosphere with the addition of ferrous chloride tetrahydrate(FeCl_(2)·_(4)H_(2)O).The phase transformation of the prepared materials and gas products during the heating process are thoroughly investigated.It is suggested that ferrous chloride participated in the phase transformation and formed Si-O-Fe bonds.And the main gaseous products are H_(2)O,H_(2),and HCl during the heating process.Besides,the ability of CG-FeCl_(2) to activate peroxymonosulfate(PMS)for catalytic degradation of polycyclic aromatic hydrocarbons(PAHs)and phenol was deeply studied.More than 95%of naphthyl,phenanthrene and phenol were removed under optimizied conditions.In addition,1O_(2),·OH,and SO_(4)·−were involved in the CG-FeCl_(2)/PMS system from the free radical scavenging experiment,where 1O_(2) played a major role during the oxidation process.Furthermore,CG-FeCl_(2)/PMS system exhibited superior stability in a relatively wide pH range and the presence of common anion from related degradation experiments.Overall,the novel CG-FeCl_(2) is an efficient and environmentally friendly catalyst,displaying potential application prospect in the field of PAHs and phenol-contaminated wastewater treatment.
