This study investigated environmental distribution and human exposure of polycyclic aromatic hydrocarbons(PAHs)and their derivatives in one Chinese petroleum refinery facility.It was found that,following with high con...This study investigated environmental distribution and human exposure of polycyclic aromatic hydrocarbons(PAHs)and their derivatives in one Chinese petroleum refinery facility.It was found that,following with high concentrations of 16 EPA PAHs(∑Parent-PAHs)in smelting subarea of studied petroleum refinery facility,total derivatives of PAHs[named as XPAHs,including nitro PAHs(NPAHs),chlorinated PAHs(Cl-PAHs),and brominated PAHs(Br-PAHs)]in gas(mean=1.57×10^(4)ng/m^(3)),total suspended particulate(TSP)(mean=4.33×10^(3) ng/m^(3))and soil(mean=4.37×10^(3) ng/g)in this subarea had 1.76-6.19 times higher levels than those from other subareas of this facility,surrounding residential areas and reference areas,indicating that petroleum refining processes would lead apparent derivation of PAHs.Especially,compared with those in residential and reference areas,gas samples in the petrochemical areas had higher∑NPAH/∑PAHs(mean=2.18),but lower∑Cl-PAH/∑PAHs(mean=1.43×10^(-1))and∑Br-PAH/∑PAHs ratios(mean=7.49×10^(-2)),indicating the richer nitrification of PAHs than chlorination during petrochemical process.The occupational exposure to PAHs and XPAHs in this petroleum refinery facility were 24-343 times higher than non-occupational exposure,and the ILCR(1.04×10^(-4))for petrochemical workers was considered to be potential high risk.Furthermore,one expanded high-resolution screening through GC Orbitrap/MS was performed for soils from petrochemical area,and another 35 PAHs were found,including alkyl-PAHs,phenyl-PAHs and other species,indicat-ing that profiles and risks of PAHs analogs in petrochemical areas deserve further expanded investigation.展开更多
An electrocoagulation treatment process was developed for treatment and upgrade of petroleum refinery effluent （wastewater）, instead of the conventional methods, which can consume higher amounts of chemicals and pro...An electrocoagulation treatment process was developed for treatment and upgrade of petroleum refinery effluent （wastewater）, instead of the conventional methods, which can consume higher amounts of chemicals and produce larger amounts of sludge. The effect of the operation parameters, such as current density, initial pH, anode material, anode dissolution, energy consumption and electrolysis time, on treatment efficiency was investigated. The experimental results showed that the effluent can be effectively treated under optimal conditions. Fourier transform infrared （FTIR） analysis of the effluent, and scanning electron microscopy （SEM） coupled with energy dispersive analysis of X-rays （EDAX） of the sludge produced, revealed that the unwanted pollutants can be eliminated. The electrocoagulation treatment process was assessed by using the removal efficiency of chemical oxygen demand （COD）, total suspended solids （TSS）, and the general physicochemical characteristics of wastewater, and the results showed that the electrocoagulation is an efficient process for recycling of petroleum wastewater; it is faster and provides better quality of treated water than the conventional methods.展开更多
A field measurement campaign for ozone and ozone precursors （VOCs and NOx） was conducted in summer 2011 around a petroleum refinery in the Beijing rural region. Three observation sites were arranged, one at southwes...A field measurement campaign for ozone and ozone precursors （VOCs and NOx） was conducted in summer 2011 around a petroleum refinery in the Beijing rural region. Three observation sites were arranged, one at southwest of the refinery as the background, and two at northeast of the refinery as the downwind receptors. Monitoring data revealed the presence of serious surface 03 pollution with the characteristics of high average daily mean and maximum concentrations （64.0 and 145.4 ppbV in no-rain days, respectively） and multi-peak diurnal variation. For NOx, the average hourly concentrations of NO2 and NO were in the range of 20.546.1 and 1.8-6.4 ppbV, respectively. For VOC measurement, a total of 51 compounds were detected. Normally, TVOCs at the background site was only dozens of ppbC, while TVOCs at the downwind sites reached several hundreds of ppbC. By subtracting the VOC concentrations at background, chemical profiles of VOC emission from the refinery were obtained, mainly including alkanes （60.0% ± 4.3%）, alkenes （21.1% ± 5.5%） and aromatics （18.9% ±3.9%）. Moreover, some differences in chemical profiles for the same measurement hours were observed between the downwind sites; the volume ratios of alkanes with low reactivity and those of alkenes with high reactivity respectively showed an increasing trend and a decreasing trend. Finally, based on temporal and spatial variations of VOC mixing ratios, their photochemical degradations and dispersion degradations were estimated to be 0.15-0.27 and 0.42-0.62, respectively, by the photochemical age calculation method, indicating stronger photochemical reactions around the refinery.展开更多
Novel Mn–Fe–Mg-and Mn–Fe–Ce-loaded alumina（Mn–Fe–Mg/Al2O3 and Mn–Fe–Ce/Al2O3） were developed to catalytically ozonate reverse osmosis concentrates generated from petroleum refinery wastewaters（PRW-ROC）. Hi...Novel Mn–Fe–Mg-and Mn–Fe–Ce-loaded alumina（Mn–Fe–Mg/Al2O3 and Mn–Fe–Ce/Al2O3） were developed to catalytically ozonate reverse osmosis concentrates generated from petroleum refinery wastewaters（PRW-ROC）. Highly dispersed 100–300-nm deposits of composite multivalent metal oxides of Mn（Mn^2＋）, Mn^3＋,and Mn^4＋, Fe（Fe^2＋）and Fe^3＋ and Mg（Mg^2＋）, or Ce（Ce^4＋） were achieved on Al2O3 supports. The developed Mn–Fe–Mg/Al2O3 and Mn–Fe–Ce/Al2O3 exhibited higher catalytic activity during the ozonation of PRW-ROC than Mn–Fe/Al2O3, Mn/Al2O-3, Fe/Al2O3, and Al2O3. Chemical oxygen demand removal by Mn–Fe–Mg/Al2O3-or Mn–Fe–Ce/Al2O3-catalyzed ozonation increased by 23.9% and23.2%, respectively, in comparison with single ozonation.Mn–Fe–Mg/Al2O3 and Mn–Fe–Ce/Al2O3 notably promoted áOH generation and áOH-mediated oxidation. This study demonstrated the potential use of composite metal oxide-loaded Al2O3 in advanced treatment of bio-recalcitrant wastewaters.展开更多
Aerobic granular sludge technology has great potential for the treatment of petroleum refinery wastewater.However,strategies to shorten the granulation time and improvement the stability still need to be developed.In ...Aerobic granular sludge technology has great potential for the treatment of petroleum refinery wastewater.However,strategies to shorten the granulation time and improvement the stability still need to be developed.In this work,biochar was prepared from waste petroleum activated sludge(biochar-WPS) and used in a sequencing batch reactor for the treatment of petroleum refinery wastewater.Biochar-WPS presented the surface area of 229.77 m2/g,pore volume of 0.28 cm3/g,H/C and O/C atomic ratios of 0.42 and 0.21,respectively.The porous structure and a high degree of hydrophilicity were found to facilitate microbial colonization and adhesion as well as particle aggregation.Application of biochar-WPS resulted in the formation of more substantial and stable aerobic granules(~66% of granules> 0.46 mm diameter) 15 days earlier compared with the control.The addition of biochar-WPS enhanced the average removal efficiency of chemical organic demand(~3%),oil(~4%)and total nitrogen(~10%) over the control.Increased microbial richness and diversity were observed within the formed granules and had an increased(~4%) proportion of denitrifying bacteria.These results indicate that an aerobic granulation mechanism using biochar-WPS is a feasible option for the treatment of petroleum refinery wastewater.展开更多
Conventional biological treatment process is not very efficient for the treatment of petroleum refinery wastewater （PRW） that contains high-concentration of organic contaminants. Prior to biological treatment, an ad...Conventional biological treatment process is not very efficient for the treatment of petroleum refinery wastewater （PRW） that contains high-concentration of organic contaminants. Prior to biological treatment, an additional pretreatment process for PRW is required for the effluent to meet the discharge standards. While re-circulated bio-filter （RBF） has been applied as a pretreatment process in several PRW treatment plants, its effects have not been comprehen- sively evaluated. In this study, the parameters of operation, the changes in pollution indexes and contaminant composition in an engineered RBF have been investigated. We found that mainly highly active de-carbonization bacteria were present in the RBF, while no nitrification bacteria were found in the RBF. This indicated the absence of nitrification in this process. The biodegradable organic contaminants were susceptible to degradation by RBF, which decreased the Biological Oxygen Demand （BODs） by 83.64% and the Chemical Oxygen Demand （CODcr） by 54.63%. Consequently, the alkalinity and pH value of RBF effluent significantly increased, which was unfavorable for the control of operating parameters in subsequent biological treatment. Along with the decrease of CODcr, the RBF effluent exhibited a reduction in biodegradability. 834 kinds of recalcitrant polar organic contaminants remained in the effluent; most of the contaminant molecules having complex structures of aromatic, polycyclic and heterocyclic rings. The results of this study showed that RBF could efficiently treat PRW for biodegradable organic contaminants removal; however, it is difficult to treat bio-refractory organic contaminants, which was unfavorable for the subsequent biological treatment process operation. An improved process might provide overall guarantees for the PRW treatment.展开更多
A novel data-driven, soft sensor based on support vector regression （SVR） integrated with a data compression technique was developed to predict the product quality for the hydrodesulfurization （HDS） process. A wid...A novel data-driven, soft sensor based on support vector regression （SVR） integrated with a data compression technique was developed to predict the product quality for the hydrodesulfurization （HDS） process. A wide range of experimental data was taken from a HDS setup to train and test the SVR model. Hyper-parameter tuning is one of the main challenges to improve predictive accuracy of the SVR model. Therefore, a hybrid approach using a combination of genetic algorithm （GA） and sequential quadratic programming （SQP） methods （GA-SQP） was developed. Performance of different optimization algorithms including GA-SQP, GA, pattern search （PS）, and grid search （GS） indicated that the best average absolute relative error （AARE）, squared correlation coefficient （R2）, and computation time （CT） （AARE = 0.0745, R2 = 0.997 and CT = 56 s） was accomplished by the hybrid algorithm. Moreover, to reduce the CT and improve the accuracy of the SVR model, the vector quantization （VQ） technique was used. The results also showed that the VQ technique can decrease the training time and improve prediction performance of the SVR model. The proposed method can provide a robust, soft sensor in a wide range of sulfur contents with good accuracy.展开更多
Currently ＂The Crude Formulation Technique＂ developed by the SINOPEC Research Institute of Petroleum Processing（RIPP） has passed the technical review sponsored by the Sinopec Corp.This technique by means of adopti...Currently ＂The Crude Formulation Technique＂ developed by the SINOPEC Research Institute of Petroleum Processing（RIPP） has passed the technical review sponsored by the Sinopec Corp.This technique by means of adopting the advanced algorithm on the basis of the crude assay data bank and the large crude spectroscopic database can intelligently blend together different kinds of crude oils to obtain multiple crude formulations, the quality of which is quite close to the target crude in a bid to provide technical support to the refining enterprises in the area of crude procurement and sustained property stabilization of crude oils pro-cessed thereby.展开更多
基金supported by the National Key Research and Development Program of China(No.2019YFC1804501)the National Natural Science Foundation of China(Nos.22036007 and 22122611)+1 种基金the Natural Science Foundation of Shandong Province(No.ZR2020ME228)the Introduction and Cultivation Plan for Young Innovative Talents of Colleges and Universities.
文摘This study investigated environmental distribution and human exposure of polycyclic aromatic hydrocarbons(PAHs)and their derivatives in one Chinese petroleum refinery facility.It was found that,following with high concentrations of 16 EPA PAHs(∑Parent-PAHs)in smelting subarea of studied petroleum refinery facility,total derivatives of PAHs[named as XPAHs,including nitro PAHs(NPAHs),chlorinated PAHs(Cl-PAHs),and brominated PAHs(Br-PAHs)]in gas(mean=1.57×10^(4)ng/m^(3)),total suspended particulate(TSP)(mean=4.33×10^(3) ng/m^(3))and soil(mean=4.37×10^(3) ng/g)in this subarea had 1.76-6.19 times higher levels than those from other subareas of this facility,surrounding residential areas and reference areas,indicating that petroleum refining processes would lead apparent derivation of PAHs.Especially,compared with those in residential and reference areas,gas samples in the petrochemical areas had higher∑NPAH/∑PAHs(mean=2.18),but lower∑Cl-PAH/∑PAHs(mean=1.43×10^(-1))and∑Br-PAH/∑PAHs ratios(mean=7.49×10^(-2)),indicating the richer nitrification of PAHs than chlorination during petrochemical process.The occupational exposure to PAHs and XPAHs in this petroleum refinery facility were 24-343 times higher than non-occupational exposure,and the ILCR(1.04×10^(-4))for petrochemical workers was considered to be potential high risk.Furthermore,one expanded high-resolution screening through GC Orbitrap/MS was performed for soils from petrochemical area,and another 35 PAHs were found,including alkyl-PAHs,phenyl-PAHs and other species,indicat-ing that profiles and risks of PAHs analogs in petrochemical areas deserve further expanded investigation.
基金the financial support from the Ministry of Higher Education and Scientific Research-Iraq
文摘An electrocoagulation treatment process was developed for treatment and upgrade of petroleum refinery effluent （wastewater）, instead of the conventional methods, which can consume higher amounts of chemicals and produce larger amounts of sludge. The effect of the operation parameters, such as current density, initial pH, anode material, anode dissolution, energy consumption and electrolysis time, on treatment efficiency was investigated. The experimental results showed that the effluent can be effectively treated under optimal conditions. Fourier transform infrared （FTIR） analysis of the effluent, and scanning electron microscopy （SEM） coupled with energy dispersive analysis of X-rays （EDAX） of the sludge produced, revealed that the unwanted pollutants can be eliminated. The electrocoagulation treatment process was assessed by using the removal efficiency of chemical oxygen demand （COD）, total suspended solids （TSS）, and the general physicochemical characteristics of wastewater, and the results showed that the electrocoagulation is an efficient process for recycling of petroleum wastewater; it is faster and provides better quality of treated water than the conventional methods.
基金supported by the National Natural Science Foundation of China (No. 51108006)Ph.D. Programs Foundation of the Ministry of Education of China (No. 20111103120008)the State Environmental Protection Key Laboratory of Sources and Control of Air Pollution Complex
文摘A field measurement campaign for ozone and ozone precursors （VOCs and NOx） was conducted in summer 2011 around a petroleum refinery in the Beijing rural region. Three observation sites were arranged, one at southwest of the refinery as the background, and two at northeast of the refinery as the downwind receptors. Monitoring data revealed the presence of serious surface 03 pollution with the characteristics of high average daily mean and maximum concentrations （64.0 and 145.4 ppbV in no-rain days, respectively） and multi-peak diurnal variation. For NOx, the average hourly concentrations of NO2 and NO were in the range of 20.546.1 and 1.8-6.4 ppbV, respectively. For VOC measurement, a total of 51 compounds were detected. Normally, TVOCs at the background site was only dozens of ppbC, while TVOCs at the downwind sites reached several hundreds of ppbC. By subtracting the VOC concentrations at background, chemical profiles of VOC emission from the refinery were obtained, mainly including alkanes （60.0% ± 4.3%）, alkenes （21.1% ± 5.5%） and aromatics （18.9% ±3.9%）. Moreover, some differences in chemical profiles for the same measurement hours were observed between the downwind sites; the volume ratios of alkanes with low reactivity and those of alkenes with high reactivity respectively showed an increasing trend and a decreasing trend. Finally, based on temporal and spatial variations of VOC mixing ratios, their photochemical degradations and dispersion degradations were estimated to be 0.15-0.27 and 0.42-0.62, respectively, by the photochemical age calculation method, indicating stronger photochemical reactions around the refinery.
基金supported in part by the National Science and Technology Major Project of China (No. 2016ZX05040-003)
文摘Novel Mn–Fe–Mg-and Mn–Fe–Ce-loaded alumina（Mn–Fe–Mg/Al2O3 and Mn–Fe–Ce/Al2O3） were developed to catalytically ozonate reverse osmosis concentrates generated from petroleum refinery wastewaters（PRW-ROC）. Highly dispersed 100–300-nm deposits of composite multivalent metal oxides of Mn（Mn^2＋）, Mn^3＋,and Mn^4＋, Fe（Fe^2＋）and Fe^3＋ and Mg（Mg^2＋）, or Ce（Ce^4＋） were achieved on Al2O3 supports. The developed Mn–Fe–Mg/Al2O3 and Mn–Fe–Ce/Al2O3 exhibited higher catalytic activity during the ozonation of PRW-ROC than Mn–Fe/Al2O3, Mn/Al2O-3, Fe/Al2O3, and Al2O3. Chemical oxygen demand removal by Mn–Fe–Mg/Al2O3-or Mn–Fe–Ce/Al2O3-catalyzed ozonation increased by 23.9% and23.2%, respectively, in comparison with single ozonation.Mn–Fe–Mg/Al2O3 and Mn–Fe–Ce/Al2O3 notably promoted áOH generation and áOH-mediated oxidation. This study demonstrated the potential use of composite metal oxide-loaded Al2O3 in advanced treatment of bio-recalcitrant wastewaters.
基金supported in part by the Science Foundation of China University of Petroleum-Beijing,China(No.2462018BJB001 and 2462020XKJS04)the National Natural Science Foundation of China,China(No.21776307)the Independent Project Program of State Key Laboratory of Petroleum Pollution Control,China(Grant No.PPCIP2017004)。
文摘Aerobic granular sludge technology has great potential for the treatment of petroleum refinery wastewater.However,strategies to shorten the granulation time and improvement the stability still need to be developed.In this work,biochar was prepared from waste petroleum activated sludge(biochar-WPS) and used in a sequencing batch reactor for the treatment of petroleum refinery wastewater.Biochar-WPS presented the surface area of 229.77 m2/g,pore volume of 0.28 cm3/g,H/C and O/C atomic ratios of 0.42 and 0.21,respectively.The porous structure and a high degree of hydrophilicity were found to facilitate microbial colonization and adhesion as well as particle aggregation.Application of biochar-WPS resulted in the formation of more substantial and stable aerobic granules(~66% of granules> 0.46 mm diameter) 15 days earlier compared with the control.The addition of biochar-WPS enhanced the average removal efficiency of chemical organic demand(~3%),oil(~4%)and total nitrogen(~10%) over the control.Increased microbial richness and diversity were observed within the formed granules and had an increased(~4%) proportion of denitrifying bacteria.These results indicate that an aerobic granulation mechanism using biochar-WPS is a feasible option for the treatment of petroleum refinery wastewater.
基金supported by the National Natural Science Foundation of China (No. U1462201)China National Offshore Oil Corporation (CNOOC-KJ125 ZDXM 15 LH007 LH12) project
文摘Conventional biological treatment process is not very efficient for the treatment of petroleum refinery wastewater （PRW） that contains high-concentration of organic contaminants. Prior to biological treatment, an additional pretreatment process for PRW is required for the effluent to meet the discharge standards. While re-circulated bio-filter （RBF） has been applied as a pretreatment process in several PRW treatment plants, its effects have not been comprehen- sively evaluated. In this study, the parameters of operation, the changes in pollution indexes and contaminant composition in an engineered RBF have been investigated. We found that mainly highly active de-carbonization bacteria were present in the RBF, while no nitrification bacteria were found in the RBF. This indicated the absence of nitrification in this process. The biodegradable organic contaminants were susceptible to degradation by RBF, which decreased the Biological Oxygen Demand （BODs） by 83.64% and the Chemical Oxygen Demand （CODcr） by 54.63%. Consequently, the alkalinity and pH value of RBF effluent significantly increased, which was unfavorable for the control of operating parameters in subsequent biological treatment. Along with the decrease of CODcr, the RBF effluent exhibited a reduction in biodegradability. 834 kinds of recalcitrant polar organic contaminants remained in the effluent; most of the contaminant molecules having complex structures of aromatic, polycyclic and heterocyclic rings. The results of this study showed that RBF could efficiently treat PRW for biodegradable organic contaminants removal; however, it is difficult to treat bio-refractory organic contaminants, which was unfavorable for the subsequent biological treatment process operation. An improved process might provide overall guarantees for the PRW treatment.
文摘A novel data-driven, soft sensor based on support vector regression （SVR） integrated with a data compression technique was developed to predict the product quality for the hydrodesulfurization （HDS） process. A wide range of experimental data was taken from a HDS setup to train and test the SVR model. Hyper-parameter tuning is one of the main challenges to improve predictive accuracy of the SVR model. Therefore, a hybrid approach using a combination of genetic algorithm （GA） and sequential quadratic programming （SQP） methods （GA-SQP） was developed. Performance of different optimization algorithms including GA-SQP, GA, pattern search （PS）, and grid search （GS） indicated that the best average absolute relative error （AARE）, squared correlation coefficient （R2）, and computation time （CT） （AARE = 0.0745, R2 = 0.997 and CT = 56 s） was accomplished by the hybrid algorithm. Moreover, to reduce the CT and improve the accuracy of the SVR model, the vector quantization （VQ） technique was used. The results also showed that the VQ technique can decrease the training time and improve prediction performance of the SVR model. The proposed method can provide a robust, soft sensor in a wide range of sulfur contents with good accuracy.
文摘Currently ＂The Crude Formulation Technique＂ developed by the SINOPEC Research Institute of Petroleum Processing（RIPP） has passed the technical review sponsored by the Sinopec Corp.This technique by means of adopting the advanced algorithm on the basis of the crude assay data bank and the large crude spectroscopic database can intelligently blend together different kinds of crude oils to obtain multiple crude formulations, the quality of which is quite close to the target crude in a bid to provide technical support to the refining enterprises in the area of crude procurement and sustained property stabilization of crude oils pro-cessed thereby.
