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
In-situ conversion processing (ICP) of shale oil underground at the depth ranging from 300 m to 3 000 m is a physical and chemical process caused by using horizontal drilling and electric heating technology, which con...In-situ conversion processing (ICP) of shale oil underground at the depth ranging from 300 m to 3 000 m is a physical and chemical process caused by using horizontal drilling and electric heating technology, which converts heavy oil, bitumen and various organic matter into light oil and gas in a large scale, which can be called"underground refinery". ICP has several advantages as in CO2capture, recoverable resource potential and the quality of hydrocarbon output. Based on the geothermal evolution mechanism of organic materials established by Tissot et al., this study reveals that in the nonmarine organic-rich shale sequence, the amount of liquid hydrocarbon maintaining in the shale is as high as 25%in the liquid hydrocarbon window stage (R o less than 1.0%), and the unconverted organic materials (low mature-immature organic materials) in the shale interval can reach 40%to 100%. The conditions of organic-rich shale suitable for underground in-situ conversion of shale oil should be satisfied in the following aspects, TOC higher than 6%, R o ranging between 0.5%and 1%, concentrated thickness of organic-rich shale greater than 15 meters, burial depth less than 3 000 m, covering area bigger than 50 km2, good sealing condition in both up-and down-contacting sequences and water content smaller than 5%, etc. The shale oil resource in China’s onshore region is huge. It is estimated with this paper that the technical recoverable resource reaches 70-90 billion tons of oil and 60-65 trillion cubic meters of gas. The ICP of shale oil underground is believed to be a fairway to find big oil in the source kitchen in the near future. And it is also believed to be a milestone to keep China long-term stability of oil and gas sufficient supply by putting ICP of shale oil underground into real practice in the future.展开更多
New methods are presented for processing and interpretation of shallow marine differential magnetic data, including constructing maps of offshore total magnetic anomalies with an extremely high reso- lution of up to 1...New methods are presented for processing and interpretation of shallow marine differential magnetic data, including constructing maps of offshore total magnetic anomalies with an extremely high reso- lution of up to 1-2 nT, mapping weak anomalies of 5-10 nT caused by mineralization effects at the contacts of hydrocarbons with host rocks, estimating depths to upper and lower boundaries of anom- alous magnetic sources, and estimating thickness of magnetic layers and boundaries of tectonic blocks. Horizontal dimensions of tectonic blocks in the so-called ＂seismic gap＂ region in the central Kuril Arc vary from 10 to 100 km, with typical dimensions of 25-30 km. The area of the ＂seismic gap＂ is a zone of intense tectonic activity and recent volcanism. Deep sources causing magnetic anomalies in the area are similar to the ＂magnetic belt＂ near Hokkaido. In the southern and central parts of Barents Sea, tectonic blocks with widths of 30-100 kin, and upper and lower boundaries of magnetic layers ranging from depths of 10 to 5 km and 18 to 30 km are calculated. Models of the magnetic layer underlying the Mezen Basin in an inland part of the White Sea-Barents Sea paleorift indicate depths to the lower boundary of the layer of 12-30 km. Weak local magnetic anomalies of 2-5 nT in the northern and central Caspian Sea were identified using the new methods, and drilling confirms that the anomalies are related to concentrations of hydrocarbon. Two layers causing magnetic anomalies are identified in the northern Caspian Sea from magnetic anomaly spectra. The upper layer lies immediately beneath the sea bottom and the lower layer occurs at depths between 30-40 m and 150-200 m.展开更多
The RTS technology can produce ultra-low sulfur diesel at lower costs using available hydrogenation catalyst and device.However,with the increase of the mixing proportion of secondary processed diesel fuel in the feed...The RTS technology can produce ultra-low sulfur diesel at lower costs using available hydrogenation catalyst and device.However,with the increase of the mixing proportion of secondary processed diesel fuel in the feed,the content of nitrogen compounds and polycyclic aromatic hydrocarbons in the feed increased,leading to the acceleration of the deactivation rate of the primary catalyst and the shortening of the service cycle.In order to fully understand the reason of catalyst deactivation,the effect of mixing secondary processed diesel fuel oil on the operating stability of the catalyst in the first reactor was investigated in a medium-sized fixed-bed hydrogenation unit.The results showed that the nitrogen compounds mainly affected the initial activity of the catalyst,but had little effect on the stability of the catalyst.The PAHs had little effect on the initial activity of the catalyst,but could significantly accelerate the deactivation of the catalyst.Combined with the analysis of the reason of catalyst deactivation and the study of RTS technology,the direction of RTS technology process optimization was put forward,and the stability of catalyst was improved obviously after process optimization.展开更多
Recently, as a direct consequence of the dwindling world oil reserves and the growing awareness of the environmental problems associated with the use of coal as energy source, there is growing interest in cheaper, abu...Recently, as a direct consequence of the dwindling world oil reserves and the growing awareness of the environmental problems associated with the use of coal as energy source, there is growing interest in cheaper, abundant and cleaner burning methane. The Gas-to-Liquid technology offers perhaps the most attractive routes for the exploitation of the world huge and growing natural gas resources. Using this process the erstwhile stranded gas is converted to premium grade liquid fuels and chemicals that are easily transported. However, a widespread application of the GTL process is being hampered by economical and technical challenges. The high cost of synthesis gas, for instance, weighs heavily on the economics and competitiveness of the process limiting its wider application. This work presented a modified Gas-to-Liquid process that eliminates the costly synthesis gas production step. The proposed process utilized an alternative pathway for methane activation via the production of chloromethane derivatives which are then converted to hydrocarbons. It established that hydrocarbons mainly olefins can be economically produced from di- and tri-chloro- methanes over a typical iron-based Fischer Tropsch catalysts in a moving bed reactor at industrially relevant conditions. Some of the attractions of the proposed process include a) the elimination of the costly air separation plant requirement b) high process selectivity and c) significant reduction of carbon dioxide emissions thereby saving on feedstock loss and the costly CO2 removal and isolation processes.展开更多
This paper makes a study of some technical and engineering aspects by using C2+ hydrocarbon separation facility at Guangdong Dapeng liquefied natural gas (GDLNG) terminal. In the C2+ hydrocarbon extraction process,the...This paper makes a study of some technical and engineering aspects by using C2+ hydrocarbon separation facility at Guangdong Dapeng liquefied natural gas (GDLNG) terminal. In the C2+ hydrocarbon extraction process,the cold energy contained in LNG will be utilized. In order to ensure the optimum operating conditions of the terminal and C2+ hydrocarbon extraction facility by optimizing the current operating processes of the terminal,the C2+ hydrocarbon extraction facility construction plan is proposed. We conducted numerous calculations and simulations using such specific analysis software as PRO II<version 7.0>. Additionally available flow data are used to verify the cyclic send-out rates from the terminal,thus establishing the current and future projected load factors. This study is intended to make sure that GDLNG can continue to supply gas via the pipeline system safely without interruptions and most significantly solves the effects of flow fluctuations at the terminal gasification send-out facility on the hydrocarbons extraction,ensuring optimum pipeline operations and ensuring safe and effective means for such C2+ hydrocarbons extraction process as well. At the same time,the terminal is also in the optimum operation condition. This is very significant to the terminal safety operation and the energy conservation and emission reduction.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.
基金Supported by the International Cooperation Project of China National Petroleum Corporation(2015D-4810-02)China National Science and Technology Major Project(2016ZX05046)
文摘In-situ conversion processing (ICP) of shale oil underground at the depth ranging from 300 m to 3 000 m is a physical and chemical process caused by using horizontal drilling and electric heating technology, which converts heavy oil, bitumen and various organic matter into light oil and gas in a large scale, which can be called"underground refinery". ICP has several advantages as in CO2capture, recoverable resource potential and the quality of hydrocarbon output. Based on the geothermal evolution mechanism of organic materials established by Tissot et al., this study reveals that in the nonmarine organic-rich shale sequence, the amount of liquid hydrocarbon maintaining in the shale is as high as 25%in the liquid hydrocarbon window stage (R o less than 1.0%), and the unconverted organic materials (low mature-immature organic materials) in the shale interval can reach 40%to 100%. The conditions of organic-rich shale suitable for underground in-situ conversion of shale oil should be satisfied in the following aspects, TOC higher than 6%, R o ranging between 0.5%and 1%, concentrated thickness of organic-rich shale greater than 15 meters, burial depth less than 3 000 m, covering area bigger than 50 km2, good sealing condition in both up-and down-contacting sequences and water content smaller than 5%, etc. The shale oil resource in China’s onshore region is huge. It is estimated with this paper that the technical recoverable resource reaches 70-90 billion tons of oil and 60-65 trillion cubic meters of gas. The ICP of shale oil underground is believed to be a fairway to find big oil in the source kitchen in the near future. And it is also believed to be a milestone to keep China long-term stability of oil and gas sufficient supply by putting ICP of shale oil underground into real practice in the future.
基金supported by the Russian Fund of Fundamental Research(Grant No.11-05-00280)
文摘New methods are presented for processing and interpretation of shallow marine differential magnetic data, including constructing maps of offshore total magnetic anomalies with an extremely high reso- lution of up to 1-2 nT, mapping weak anomalies of 5-10 nT caused by mineralization effects at the contacts of hydrocarbons with host rocks, estimating depths to upper and lower boundaries of anom- alous magnetic sources, and estimating thickness of magnetic layers and boundaries of tectonic blocks. Horizontal dimensions of tectonic blocks in the so-called ＂seismic gap＂ region in the central Kuril Arc vary from 10 to 100 km, with typical dimensions of 25-30 km. The area of the ＂seismic gap＂ is a zone of intense tectonic activity and recent volcanism. Deep sources causing magnetic anomalies in the area are similar to the ＂magnetic belt＂ near Hokkaido. In the southern and central parts of Barents Sea, tectonic blocks with widths of 30-100 kin, and upper and lower boundaries of magnetic layers ranging from depths of 10 to 5 km and 18 to 30 km are calculated. Models of the magnetic layer underlying the Mezen Basin in an inland part of the White Sea-Barents Sea paleorift indicate depths to the lower boundary of the layer of 12-30 km. Weak local magnetic anomalies of 2-5 nT in the northern and central Caspian Sea were identified using the new methods, and drilling confirms that the anomalies are related to concentrations of hydrocarbon. Two layers causing magnetic anomalies are identified in the northern Caspian Sea from magnetic anomaly spectra. The upper layer lies immediately beneath the sea bottom and the lower layer occurs at depths between 30-40 m and 150-200 m.
基金This work was financially supported by the Technology Development Project of SINOPEC(121025)All of the staff in our laboratory had provided a lot of support in the analysis of oil samples and catalyst characterization.
文摘The RTS technology can produce ultra-low sulfur diesel at lower costs using available hydrogenation catalyst and device.However,with the increase of the mixing proportion of secondary processed diesel fuel in the feed,the content of nitrogen compounds and polycyclic aromatic hydrocarbons in the feed increased,leading to the acceleration of the deactivation rate of the primary catalyst and the shortening of the service cycle.In order to fully understand the reason of catalyst deactivation,the effect of mixing secondary processed diesel fuel oil on the operating stability of the catalyst in the first reactor was investigated in a medium-sized fixed-bed hydrogenation unit.The results showed that the nitrogen compounds mainly affected the initial activity of the catalyst,but had little effect on the stability of the catalyst.The PAHs had little effect on the initial activity of the catalyst,but could significantly accelerate the deactivation of the catalyst.Combined with the analysis of the reason of catalyst deactivation and the study of RTS technology,the direction of RTS technology process optimization was put forward,and the stability of catalyst was improved obviously after process optimization.
文摘Recently, as a direct consequence of the dwindling world oil reserves and the growing awareness of the environmental problems associated with the use of coal as energy source, there is growing interest in cheaper, abundant and cleaner burning methane. The Gas-to-Liquid technology offers perhaps the most attractive routes for the exploitation of the world huge and growing natural gas resources. Using this process the erstwhile stranded gas is converted to premium grade liquid fuels and chemicals that are easily transported. However, a widespread application of the GTL process is being hampered by economical and technical challenges. The high cost of synthesis gas, for instance, weighs heavily on the economics and competitiveness of the process limiting its wider application. This work presented a modified Gas-to-Liquid process that eliminates the costly synthesis gas production step. The proposed process utilized an alternative pathway for methane activation via the production of chloromethane derivatives which are then converted to hydrocarbons. It established that hydrocarbons mainly olefins can be economically produced from di- and tri-chloro- methanes over a typical iron-based Fischer Tropsch catalysts in a moving bed reactor at industrially relevant conditions. Some of the attractions of the proposed process include a) the elimination of the costly air separation plant requirement b) high process selectivity and c) significant reduction of carbon dioxide emissions thereby saving on feedstock loss and the costly CO2 removal and isolation processes.
文摘This paper makes a study of some technical and engineering aspects by using C2+ hydrocarbon separation facility at Guangdong Dapeng liquefied natural gas (GDLNG) terminal. In the C2+ hydrocarbon extraction process,the cold energy contained in LNG will be utilized. In order to ensure the optimum operating conditions of the terminal and C2+ hydrocarbon extraction facility by optimizing the current operating processes of the terminal,the C2+ hydrocarbon extraction facility construction plan is proposed. We conducted numerous calculations and simulations using such specific analysis software as PRO II<version 7.0>. Additionally available flow data are used to verify the cyclic send-out rates from the terminal,thus establishing the current and future projected load factors. This study is intended to make sure that GDLNG can continue to supply gas via the pipeline system safely without interruptions and most significantly solves the effects of flow fluctuations at the terminal gasification send-out facility on the hydrocarbons extraction,ensuring optimum pipeline operations and ensuring safe and effective means for such C2+ hydrocarbons extraction process as well. At the same time,the terminal is also in the optimum operation condition. This is very significant to the terminal safety operation and the energy conservation and emission reduction.
