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 patti...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.展开更多
Slurry-phase hydrogenation technology is the frontier topic in the efficient conversion of heavy oils into light fractions around the world.Developing highly active dispersed MoS_(2) catalysts is the major obstacle to...Slurry-phase hydrogenation technology is the frontier topic in the efficient conversion of heavy oils into light fractions around the world.Developing highly active dispersed MoS_(2) catalysts is the major obstacle to realize the industrial application of upgrading heavy oils.In this work,both top-down ball-milling method and bottom-up hydrothermal method were designed to synthesize MoS_(2) catalysts with controllable layer structures.The stacking layers and lateral sizes for micro-scaled MoS_(2) catalysts by ball-milling method can be reduced to their limits and stabilize at 6~8 layers and lateral size of ca.30 nm.The more flexible bottom-up hydrothermal method can construct MoS_(2) catalysts with much smaller lateral sizes and fewer stacking layers,especially,MoS_(2) catalyst fabricated with ammonium tetrathiomolybdate as Mo and S precursor possesses average stacking layers of 2 and lateral size of 5 ~ 10 nm.Polycyclic aromatic hydrocarbons anthracene,phenanthrene and naphthalene were used as model compounds of heavy oils to investigate the catalytic hydrogenation performance of designed MoS_(2) catalysts.The catalytic activities of MoS_(2) catalysts can be well correlated with their stacking layers and lateral size.The edges of top and bottom S-Mo-S atomic layers for MoS_(2) sheets,named rim sites,are positively correlated with the exposure of active sites for catalytic hydrogenation of PAHs.The highest catalytic activity of MoS_(2) catalyst results from its layer structures of 100% rim sites and the smallest lateral size of5 ~ 10 nm,which is beneficial to expose maximum active sites for catalytic hydrogenation reactions.This work can guide us to design the highly active hydrogenation catalysts,and promote the industrial application of upgrading heavy oils.展开更多
An efficient and environment-friendly method for simultaneous determination of 13 typical derivatives of polycyclic aromatic hydrocarbon(PAH)in petroleum-polluted soil with nitro-,oxy-and alkylfunctional group was dev...An efficient and environment-friendly method for simultaneous determination of 13 typical derivatives of polycyclic aromatic hydrocarbon(PAH)in petroleum-polluted soil with nitro-,oxy-and alkylfunctional group was developed using supercritical fluid extraction(SFE)followed by ultra-high performance supercritical fluid chromatography(UHPSFC).Parameters of UHPSFC,including type of stationary phase and mobile phase modifiers,gradient elution process,backpressure,column temperature,and the flow rate of mobile phase,were systematically optimized,achieving a fast separation within4.2 min.Limits of detection(LOD)were 0.005-0.1μg mL^(-1)or 0.1-2.0 ng g^(-1),respectively,with a good repeatability(RSD<5.0%).Before UHPSFC-PDA analysis,the PAH-derivatives in soil samples were effectively enriched in 15.0 min using SFE with an online carbon nanotubes(CNTs)collection trap.The soil samples were analyzed by the proposed method and the results were verified by GC-MS.Thus,SFE equipped with an online CNTs trap followed by UHPSFC-PDA analysis,which only consumed about2.0 mL organic solvent for a whole run,has been demonstrated to be an efficient way for screening and quantitative analysis of trace-level PAH-derivatives in soil samples.展开更多
The effect of polycyclic aromatic hydrocarbons(PAHs)on the stability of the hydrogenation catalyst for production of ultra-low sulfur diesel was studied in a pilot plant using Ni-Mo-W/γ-Al_(2)O_(3)catalyst.The mechan...The effect of polycyclic aromatic hydrocarbons(PAHs)on the stability of the hydrogenation catalyst for production of ultra-low sulfur diesel was studied in a pilot plant using Ni-Mo-W/γ-Al_(2)O_(3)catalyst.The mechanisms of catalyst deactivation were analyzed by the methods of elemental analysis,nitrogen adsorption-desorption,thermogravimetry-mass spectrometry(TG-MS)technology,X-ray photoelectron spectroscopy(XPS)and high resolution transmission electron microscopy(HRTEM).The results demonstrated that PAHs had little effect on the activity of catalyst at the beginning of operation,during which the reaction temperature was increased by only 1-4℃.However,the existence of PAHs significantly accelerated the deactivation of catalyst and weakened the stability of catalyst.This phenomenon could be explained by the reason that the catalyst deactivation is not only related to the formation of carbon deposit,but is also closely related to the loss of pore volume and the decrease of Ni-W-S phase ratio after adding PAHs.展开更多
An efficient analytical method combining pyrolysis and capillary GC/MS has been developed for determination and quantitation of targeted polycyclic aromatic hydrocarbons.The limit of detection ranged from 0.29 μg/g t...An efficient analytical method combining pyrolysis and capillary GC/MS has been developed for determination and quantitation of targeted polycyclic aromatic hydrocarbons.The limit of detection ranged from 0.29 μg/g to 43.46 μg/g,and repeatability values were between 0.1% and 8.2% for blank spiked samples and between 0.1 % and 9.8% for real samples of heavy oils.Through application of the proposed method in hydrotreating processes,it has been found out that heavy oils before and after the specified hydroprocessing treatment exhibited a diverse PAHs distribution which might be determined by the discrepancy in their intrinsic contents and hydrogenation reactivity.Furthermore,the hydrogenation reactivity of different polycyclic aromatic hydrocarbons was further investigated and discovered to be more interrelated to molecular structure and rings alignment or conjugation mode.展开更多
Coriander(Coriandrum sativum L.)is recognized for its antioxidant property,as a kind of natural phenolic-rich ingredient.Polycyclic aromatic hydrocarbons(PAHs)present a class of heat-driven hazards in foods,especially...Coriander(Coriandrum sativum L.)is recognized for its antioxidant property,as a kind of natural phenolic-rich ingredient.Polycyclic aromatic hydrocarbons(PAHs)present a class of heat-driven hazards in foods,especially the processed meat.In this study,the effect of coriander root and leaf extract on the formation and inhibition of PAH8 in roasted duck wings was firstly investigated.Coriander root extract(CRE)and coriander leaf extract(CLE)with five concentration groups(200,400,600,800,1000 mg/L)were prepared respectively to marinate the duck wings.CRE marinade exhibited greater inhibitory effect on PAH8 formation in roasted duck wings that ranged from 65.0%-87.4%.The electron spin resonance study indicated a significantly positive correlation between PAH8 and free radical level,suggesting the participation of radicals in PAHs formation.Also,it was speculated that the inhibitory effect on PAH8 was related to the phenolic compounds identified in coriander marinades.CRE made greater inhibitory effect on the formation of PAH8 and could be considered as a kind of natural source to mitigate PAHs in heat-processed meat products.展开更多
Low-carbon process for resource utilization of polycyclic aromatic hydrocarbons(PAHs)in zeolitecatalyzed processes,geared to carbon neutrality-a prominent trend throughout human activities,has been bottlenecked by the...Low-carbon process for resource utilization of polycyclic aromatic hydrocarbons(PAHs)in zeolitecatalyzed processes,geared to carbon neutrality-a prominent trend throughout human activities,has been bottlenecked by the lack of a complete mechanistic understanding of coking and decoking chemistry,involving the speciation and molecular evolution of PAHs,the plethora of which causes catalyst deactivation and forces regeneration,rendering significant CO_(2) emission.Herein,by exploiting the high-resolution matrix-assisted laser desorption/ionization Fourier-transform ion cyclotron resonance mass spectrometry(MALDI FT-ICR MS),we unveil the missing fingerprints of the mechanistic pathways for both formation and decomposition of cross-linked cage-passing PAHs for SAPO-34-catalyzed,industrially relevant methanol-to-olefins(MTO)as a model reaction.Notable is the molecule-resolved symmetrical signature:their speciation originates exclusively from the direct coupling of in-cage hydrocarbon pool(HCP)species,whereas water-promoted decomposition of cage-passing PAHs initiates with selective cracking of inter-cage local structures at 8-rings followed by deep aromatic steam reforming.Molecular deciphering the reversibly dynamic evolution trajectory(fate)of full-spectrum aromatic hydrocarbons and fulfilling the real-time quantitative carbon resource footprints advance the fundamental knowledge of deactivation and regeneration phenomena(decay and recovery motifs of autocatalysis)and disclose the underlying mechanisms of especially the chemistry of coking and decoking in zeolite catalysis.The positive yet divergent roles of water in these two processes are disentangled.These unprecedented insights ultimately lead us to a steam regeneration strategy with valuable CO and H_(2) as main products,negligible CO_(2) emission in steam reforming and full catalyst activity recovery,which further proves feasible in other important chemical processes,promising to be a sustainable and potent approach that contributes to carbon-neutral chemical industry.展开更多
To obtain high yields of monocyclic aromatic hydrocarbons with methyl side chains,such as toluene and xylene,methane(CH_(4))can be introduced into the hydrocracking of polycyclic aromatic hydrocarbons.CH_(4)can partic...To obtain high yields of monocyclic aromatic hydrocarbons with methyl side chains,such as toluene and xylene,methane(CH_(4))can be introduced into the hydrocracking of polycyclic aromatic hydrocarbons.CH_(4)can participate in the reaction,supply methyl side chains to the product,and improve product distribution.In this study,the hydrogenation reaction of polycyclic aromatic hydrocarbons over a carbonized NiMo/Hβcatalyst in a CH_(4)and hydrogen(H_(2))environment was investigated to study the promotional effect of CH_(4)on the hydrocracking of polycyclic aromatics.Under conditions of 3.5 MPa,380℃,volume air velocity of 4 h^(-1),gas-oil volume ratio of 800,and H_(2):CH_(4)molar ratio of 1:1,the conversion rate of naphthalene was 99.97%,the liquid phase yield was 93.62%,and the selectivity of BTX were 17.76%,25.17%,and 20.47%,respectively.In comparison to the use of a H_(2)atmosphere,the selectivity of benzene was significantly decreased,whereas the selectivity of toluene and xylene were increased.It was shown that CH_(4)can participate in the hydrocracking of naphthalene and improve the selectivity of toluene and xylene in the liquid product.The carbonized NiMo/Hβcatalyst was characterized by a range of analytical methods(such as X-ray diffraction(XRD),ammonia-temperature-programmed desorption(NH3-TPD),hydrogen-temperature-programmed reduction(H_(2)-TPR),and X-ray photoelectron spectroscopy(XPS)).The results indicated that Ni and Mo carbides were the major species in the carbonized NiMo/Hβcatalyst and were considered to be active sites for the activation of CH_(4)and H_(2).After loading the metal components,the catalyst displayed prominent weak acidic sites,which may be suitable locations for cracking,alkylation,and other related reactions.Therefore,the carbonized NiMo/Hβcatalyst displayed multiple functions during the hydrocracking of polycyclic aromatic hydrocarbons in a CH_(4)and H_(2)environment.These results could be used to develop a new way to efficiently utilize polycyclic aromatic hydrocarbons and natural gas resources.展开更多
Along with the rapid development of oil industries internationally,petroleum prospecting and exploitation activities are growing intensively.Especially in China,with the fastest economic growth in the world and shorta...Along with the rapid development of oil industries internationally,petroleum prospecting and exploitation activities are growing intensively.Especially in China,with the fastest economic growth in the world and shortage of petroleum resources,we are leading the practices of petroleum deep exploitation.Obviously,the risk of damage to the natural environment from these activities is high.Oil contamination in soils and groundwater is becoming a big issue along with pesticide pollution,which makes organic pollution prevention and control （OPPC） much more complex.In this paper,based on recent research on oil-contaminated soil at home and abroad,we make comments on the remediation technologies for polluted soil,emphasizing bioremediation techniques and degradation mechanisms in order to push forward research into bound organic pollution prevention and control （OPPC）,especially in China.展开更多
This manuscript is reviewing the presence of substances of safety concern that may be generated in different types of meat products.Such substances include N-nitrosamines that can be generated under certain conditions...This manuscript is reviewing the presence of substances of safety concern that may be generated in different types of meat products.Such substances include N-nitrosamines that can be generated under certain conditions when using nitrite as preservative,the polycyclic aromatic hydrocarbons generated as a consequence of particular smoking processes,heterocyclic aromatic amines generated under particular cooking conditions,compounds released from the oxidation of lipids and proteins,Maillard reaction products like acrylamide and carboxymethyl lysine,and amines that can be generated and accumulated in fermented meats.These hazardous compounds,their mechanisms of generation,risks for health and ways of preventing its presence in meat products are briefly described in this review.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
The individual particles collected from a power station were analyzed by time of flight secondary ion mass spectrometry (TOF SIMS). The result indicates the presence of the polycyclic aromatic hydrocarbon (PAHs) as we...The individual particles collected from a power station were analyzed by time of flight secondary ion mass spectrometry (TOF SIMS). The result indicates the presence of the polycyclic aromatic hydrocarbon (PAHs) as well as the oxygenated one. They might be derived from the incomplete combustion of coals. SIMS has proved to be a rapid method for the qualitative analysis of PAHs and OPAHs absorbed on the aerosol particles. New perspectives for better understanding the SIMS spectra obtained from complex mixture such as environmental samples have been opened.展开更多
基金supported by the Key Scientific and Technological Research Projects of Xinjiang Production and Construction Corps (2022AB001)the Henan Key Laboratory of Cold Chain Food Quality and Safety Control (CCFQ2022)+2 种基金the National Key R&D Program of China (2019YFC1606200),funded by Ministry of Science and Technology of the People’s Republic of Chinathe China Agriculture Research System (CARS-41), which was funded by the Chinese Ministry of Agriculturethe Priority Academic Program Development of Jiangsu Higher Education Institution (PAPD)
文摘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.
基金financially supported by the Autonomous Region Key R&D Program of Xin Jiang (2017B02007-1, 2017B02007-2)the High Level Talent Innovation and Entrepreneurship Project of Dalian (2019CT04)。
文摘Slurry-phase hydrogenation technology is the frontier topic in the efficient conversion of heavy oils into light fractions around the world.Developing highly active dispersed MoS_(2) catalysts is the major obstacle to realize the industrial application of upgrading heavy oils.In this work,both top-down ball-milling method and bottom-up hydrothermal method were designed to synthesize MoS_(2) catalysts with controllable layer structures.The stacking layers and lateral sizes for micro-scaled MoS_(2) catalysts by ball-milling method can be reduced to their limits and stabilize at 6~8 layers and lateral size of ca.30 nm.The more flexible bottom-up hydrothermal method can construct MoS_(2) catalysts with much smaller lateral sizes and fewer stacking layers,especially,MoS_(2) catalyst fabricated with ammonium tetrathiomolybdate as Mo and S precursor possesses average stacking layers of 2 and lateral size of 5 ~ 10 nm.Polycyclic aromatic hydrocarbons anthracene,phenanthrene and naphthalene were used as model compounds of heavy oils to investigate the catalytic hydrogenation performance of designed MoS_(2) catalysts.The catalytic activities of MoS_(2) catalysts can be well correlated with their stacking layers and lateral size.The edges of top and bottom S-Mo-S atomic layers for MoS_(2) sheets,named rim sites,are positively correlated with the exposure of active sites for catalytic hydrogenation of PAHs.The highest catalytic activity of MoS_(2) catalyst results from its layer structures of 100% rim sites and the smallest lateral size of5 ~ 10 nm,which is beneficial to expose maximum active sites for catalytic hydrogenation reactions.This work can guide us to design the highly active hydrogenation catalysts,and promote the industrial application of upgrading heavy oils.
基金financially supported by the National Natural Science Foundation of China(No.21874153)Science Foundation of China University of Petroleum,Beijing(No.2462017BJB09)PetroChina Innovation Foundation(No.2016D-5007-0402)。
文摘An efficient and environment-friendly method for simultaneous determination of 13 typical derivatives of polycyclic aromatic hydrocarbon(PAH)in petroleum-polluted soil with nitro-,oxy-and alkylfunctional group was developed using supercritical fluid extraction(SFE)followed by ultra-high performance supercritical fluid chromatography(UHPSFC).Parameters of UHPSFC,including type of stationary phase and mobile phase modifiers,gradient elution process,backpressure,column temperature,and the flow rate of mobile phase,were systematically optimized,achieving a fast separation within4.2 min.Limits of detection(LOD)were 0.005-0.1μg mL^(-1)or 0.1-2.0 ng g^(-1),respectively,with a good repeatability(RSD<5.0%).Before UHPSFC-PDA analysis,the PAH-derivatives in soil samples were effectively enriched in 15.0 min using SFE with an online carbon nanotubes(CNTs)collection trap.The soil samples were analyzed by the proposed method and the results were verified by GC-MS.Thus,SFE equipped with an online CNTs trap followed by UHPSFC-PDA analysis,which only consumed about2.0 mL organic solvent for a whole run,has been demonstrated to be an efficient way for screening and quantitative analysis of trace-level PAH-derivatives in soil samples.
基金financially supported by the Hydrogenation Process and Hydrogenation Catalyst Laboratory (RIPP,SINOPEC)
文摘The effect of polycyclic aromatic hydrocarbons(PAHs)on the stability of the hydrogenation catalyst for production of ultra-low sulfur diesel was studied in a pilot plant using Ni-Mo-W/γ-Al_(2)O_(3)catalyst.The mechanisms of catalyst deactivation were analyzed by the methods of elemental analysis,nitrogen adsorption-desorption,thermogravimetry-mass spectrometry(TG-MS)technology,X-ray photoelectron spectroscopy(XPS)and high resolution transmission electron microscopy(HRTEM).The results demonstrated that PAHs had little effect on the activity of catalyst at the beginning of operation,during which the reaction temperature was increased by only 1-4℃.However,the existence of PAHs significantly accelerated the deactivation of catalyst and weakened the stability of catalyst.This phenomenon could be explained by the reason that the catalyst deactivation is not only related to the formation of carbon deposit,but is also closely related to the loss of pore volume and the decrease of Ni-W-S phase ratio after adding PAHs.
基金support from the National Key Basic Research Science Foundation (Grant No. 2006CB202500. 4-1)
文摘An efficient analytical method combining pyrolysis and capillary GC/MS has been developed for determination and quantitation of targeted polycyclic aromatic hydrocarbons.The limit of detection ranged from 0.29 μg/g to 43.46 μg/g,and repeatability values were between 0.1% and 8.2% for blank spiked samples and between 0.1 % and 9.8% for real samples of heavy oils.Through application of the proposed method in hydrotreating processes,it has been found out that heavy oils before and after the specified hydroprocessing treatment exhibited a diverse PAHs distribution which might be determined by the discrepancy in their intrinsic contents and hydrogenation reactivity.Furthermore,the hydrogenation reactivity of different polycyclic aromatic hydrocarbons was further investigated and discovered to be more interrelated to molecular structure and rings alignment or conjugation mode.
基金funded by the National Key R&D Program of China(2016YFD040040303).
文摘Coriander(Coriandrum sativum L.)is recognized for its antioxidant property,as a kind of natural phenolic-rich ingredient.Polycyclic aromatic hydrocarbons(PAHs)present a class of heat-driven hazards in foods,especially the processed meat.In this study,the effect of coriander root and leaf extract on the formation and inhibition of PAH8 in roasted duck wings was firstly investigated.Coriander root extract(CRE)and coriander leaf extract(CLE)with five concentration groups(200,400,600,800,1000 mg/L)were prepared respectively to marinate the duck wings.CRE marinade exhibited greater inhibitory effect on PAH8 formation in roasted duck wings that ranged from 65.0%-87.4%.The electron spin resonance study indicated a significantly positive correlation between PAH8 and free radical level,suggesting the participation of radicals in PAHs formation.Also,it was speculated that the inhibitory effect on PAH8 was related to the phenolic compounds identified in coriander marinades.CRE made greater inhibitory effect on the formation of PAH8 and could be considered as a kind of natural source to mitigate PAHs in heat-processed meat products.
基金financial support from the National Natural Science Foundation of China(21991092,21991090,22022202,21972142,21902153,21974138)the Chinese Academy of Sciences(QYZDY-SSW-SC024)the Dalian Institute of Chemical Physics(DICP I201926,DICP I201947)。
文摘Low-carbon process for resource utilization of polycyclic aromatic hydrocarbons(PAHs)in zeolitecatalyzed processes,geared to carbon neutrality-a prominent trend throughout human activities,has been bottlenecked by the lack of a complete mechanistic understanding of coking and decoking chemistry,involving the speciation and molecular evolution of PAHs,the plethora of which causes catalyst deactivation and forces regeneration,rendering significant CO_(2) emission.Herein,by exploiting the high-resolution matrix-assisted laser desorption/ionization Fourier-transform ion cyclotron resonance mass spectrometry(MALDI FT-ICR MS),we unveil the missing fingerprints of the mechanistic pathways for both formation and decomposition of cross-linked cage-passing PAHs for SAPO-34-catalyzed,industrially relevant methanol-to-olefins(MTO)as a model reaction.Notable is the molecule-resolved symmetrical signature:their speciation originates exclusively from the direct coupling of in-cage hydrocarbon pool(HCP)species,whereas water-promoted decomposition of cage-passing PAHs initiates with selective cracking of inter-cage local structures at 8-rings followed by deep aromatic steam reforming.Molecular deciphering the reversibly dynamic evolution trajectory(fate)of full-spectrum aromatic hydrocarbons and fulfilling the real-time quantitative carbon resource footprints advance the fundamental knowledge of deactivation and regeneration phenomena(decay and recovery motifs of autocatalysis)and disclose the underlying mechanisms of especially the chemistry of coking and decoking in zeolite catalysis.The positive yet divergent roles of water in these two processes are disentangled.These unprecedented insights ultimately lead us to a steam regeneration strategy with valuable CO and H_(2) as main products,negligible CO_(2) emission in steam reforming and full catalyst activity recovery,which further proves feasible in other important chemical processes,promising to be a sustainable and potent approach that contributes to carbon-neutral chemical industry.
基金the financial support from the Graduate Student Innovation and Practical Ability Training Program of Xi’an Shiyou University (No. YCS21212111)Open Fund Project of the State Key Laboratory of Heavy Oil, China (SKLHOP201703)+3 种基金National Natural Science Foundation of China (No. 52274039)Natural Science Foundation of Shaanxi Provincial Department of Education (Grant 2023-JC-YB-414)Natural Science Foundation of Shaanxi Province in China (No. 2022JZ-28)the Open Fund Project of the National Oil Shale Exploitation Research and Development Center, China (No. 33550022-ZC0613-0255)
文摘To obtain high yields of monocyclic aromatic hydrocarbons with methyl side chains,such as toluene and xylene,methane(CH_(4))can be introduced into the hydrocracking of polycyclic aromatic hydrocarbons.CH_(4)can participate in the reaction,supply methyl side chains to the product,and improve product distribution.In this study,the hydrogenation reaction of polycyclic aromatic hydrocarbons over a carbonized NiMo/Hβcatalyst in a CH_(4)and hydrogen(H_(2))environment was investigated to study the promotional effect of CH_(4)on the hydrocracking of polycyclic aromatics.Under conditions of 3.5 MPa,380℃,volume air velocity of 4 h^(-1),gas-oil volume ratio of 800,and H_(2):CH_(4)molar ratio of 1:1,the conversion rate of naphthalene was 99.97%,the liquid phase yield was 93.62%,and the selectivity of BTX were 17.76%,25.17%,and 20.47%,respectively.In comparison to the use of a H_(2)atmosphere,the selectivity of benzene was significantly decreased,whereas the selectivity of toluene and xylene were increased.It was shown that CH_(4)can participate in the hydrocracking of naphthalene and improve the selectivity of toluene and xylene in the liquid product.The carbonized NiMo/Hβcatalyst was characterized by a range of analytical methods(such as X-ray diffraction(XRD),ammonia-temperature-programmed desorption(NH3-TPD),hydrogen-temperature-programmed reduction(H_(2)-TPR),and X-ray photoelectron spectroscopy(XPS)).The results indicated that Ni and Mo carbides were the major species in the carbonized NiMo/Hβcatalyst and were considered to be active sites for the activation of CH_(4)and H_(2).After loading the metal components,the catalyst displayed prominent weak acidic sites,which may be suitable locations for cracking,alkylation,and other related reactions.Therefore,the carbonized NiMo/Hβcatalyst displayed multiple functions during the hydrocracking of polycyclic aromatic hydrocarbons in a CH_(4)and H_(2)environment.These results could be used to develop a new way to efficiently utilize polycyclic aromatic hydrocarbons and natural gas resources.
基金supports from the New Century Excellent Talents in University of Ministry of Education (NCET-09-0765)the China Scholarship of Council (2009644509)the Natural Scientific Funds of China (40973064)
文摘Along with the rapid development of oil industries internationally,petroleum prospecting and exploitation activities are growing intensively.Especially in China,with the fastest economic growth in the world and shortage of petroleum resources,we are leading the practices of petroleum deep exploitation.Obviously,the risk of damage to the natural environment from these activities is high.Oil contamination in soils and groundwater is becoming a big issue along with pesticide pollution,which makes organic pollution prevention and control （OPPC） much more complex.In this paper,based on recent research on oil-contaminated soil at home and abroad,we make comments on the remediation technologies for polluted soil,emphasizing bioremediation techniques and degradation mechanisms in order to push forward research into bound organic pollution prevention and control （OPPC）,especially in China.
基金Grants AGL2017-89831-R,AGL2015-64673-R and FEDER funds from the Spanish Ministry of Economy,Industry and Competitiveness are acknowledged.Ramon y Cajal postdoctoral contract to LM is also acknowledged。
文摘This manuscript is reviewing the presence of substances of safety concern that may be generated in different types of meat products.Such substances include N-nitrosamines that can be generated under certain conditions when using nitrite as preservative,the polycyclic aromatic hydrocarbons generated as a consequence of particular smoking processes,heterocyclic aromatic amines generated under particular cooking conditions,compounds released from the oxidation of lipids and proteins,Maillard reaction products like acrylamide and carboxymethyl lysine,and amines that can be generated and accumulated in fermented meats.These hazardous compounds,their mechanisms of generation,risks for health and ways of preventing its presence in meat products are briefly described in this review.
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The individual particles collected from a power station were analyzed by time of flight secondary ion mass spectrometry (TOF SIMS). The result indicates the presence of the polycyclic aromatic hydrocarbon (PAHs) as well as the oxygenated one. They might be derived from the incomplete combustion of coals. SIMS has proved to be a rapid method for the qualitative analysis of PAHs and OPAHs absorbed on the aerosol particles. New perspectives for better understanding the SIMS spectra obtained from complex mixture such as environmental samples have been opened.
