1-hexene aromatization is a promising technology to convert excess olefin in fluid catalytic cracking(FCC)gasoline to high-value benzene(B),toluene(T),and xylene.Besides,the increasing market demand of xylene has put ...1-hexene aromatization is a promising technology to convert excess olefin in fluid catalytic cracking(FCC)gasoline to high-value benzene(B),toluene(T),and xylene.Besides,the increasing market demand of xylene has put forward higher requirements for new generation of catalyst.For increasing xylene yield in 1-hexene aromatization,the effect of mesopore structure and spatial distribution on product distribution and Zn loading was studied.Catalysts with different mesopore spatial distribution were prepared by post-treatment of parent HZSM-5 zeolite,including NaOH treatment,tetra-propylammonium hydroxide(TPAOH)treatment,and recrystallization.It was found the evenly distributed mesopore mainly prolongs the catalyst lifetime by enhancing diffusion properties but reduces the aromatics selectivity,as a result of damage of micropores close to the catalyst surface.While the selectivity of high-value xylene can be highly promoted when the mesopore is mainly distributed interior the catalyst.Besides,the state of loaded Zn was also affected by mesopores spatial distribution.On the optimized catalyst,the xylene selectivity was enhanced by 12.4%compared with conventional Zn-loaded parent HZSM-5 catalyst at conversion over 99%.It was attributed to the synergy effect of mesopores spatial distribution and optimized acid properties.This work reveals the role of mesopores in different spatial positions of 1-hexene aromatization catalysts in the reaction process and the influence on metal distribution,as well as their synergistic effect two on the improvement of xylene selectivity,which can improve our understanding of catalyst pore structure and be helpful for the rational design of high-efficient catalyst.展开更多
Two-step conversion of methanol to aromatics via light hydrocarbons can significantly improve the conversion stability compared with direct aromatization of methanol,but it remains a challenge to achieve a high p-xyle...Two-step conversion of methanol to aromatics via light hydrocarbons can significantly improve the conversion stability compared with direct aromatization of methanol,but it remains a challenge to achieve a high p-xylene(PX)selectivity.Herein,silica coating was firstly used to passivate external acid sites of ZSM-5 catalyst for the aromatization of light hydrocarbons by the chemical liquid deposition method.With the increase of SiO_(2) deposition,the density of the external acid sites of the catalyst was decreased from 0.1 to 0.03 mmol·g^(-1),which inhibited the surface secondary reactions and increased the PX/X from 34.6% to 60.0%.In view of the fact that the aromatization process in the second step was partly inhibited as methanol was consumed in advance in the upper methanol-to-light hydrocarbons catalyst layer,part of methanol was directly introduced into the lower aromatization catalyst layer to promote the alkylation process during the aromatization,which decreased the toluene selectivity from 34.5% to 14.3% but increased the xylene selectivity from 40.0%to 55.3%.It was also found that an appropriate external acid density was needed for aromatization catalyst to strengthen the alkylation process and improve the selectivity of xylene under the conditions of methanol introduction.展开更多
The ethylene aromatization is critical for the methanol to aromatics and light alkane dehydroaromatization process.The single-event microkinetic(SEMK)model combining the linear free energy theory and solid acid distri...The ethylene aromatization is critical for the methanol to aromatics and light alkane dehydroaromatization process.The single-event microkinetic(SEMK)model combining the linear free energy theory and solid acid distribution concept were established and extend for the ethylene aromatization process,which can reduce the kinetic parameters and simplify the reaction network by comparison with the SEMK model including subtype elementary steps based on the type of carbenium ions.Further introducing deactivation parametersφinto the model and applying the linear free energy model to the deactivation experimental data,the obtained deactivation parametersφindicate that the carbon deposition precursors have the greatest impact on reducing the reaction rate of single-molecular reactions and the smallest impact on the hydrogen transfer reaction.Meanwhile,according to the change of reaction enthalpy,effect of carbenium ion structure on methylation,ethylation,cyclization and endo-βscission was investigated by introducing linear free energy concept into the SEMK model.The effect of different acid strengths on elementary steps was investigated based on the acid strength distribution model,it was found that the methylation and oligomerization reactions,the ali-βscission reaction,endo-βscission reaction and the cyclization reaction were more sensitive to strong acidity sites.The physisorption and chemisorption heat are separated from the protonation heat in the linear free energy kinetic model and the acid strength distribution kinetic model,and the absolute values of the obtained physisorption and chemisorption heat increase with the carbon number of carbenium ions.Furthermore,the parameters of the acid strength distribution kinetic model were applied to propane dehydroaromatization on H-ZSM-5 and the ethane dehydroaromatization on Zn/ZSM-5 to confirm the independence of parameters in the SEMK model with the similar reaction network.展开更多
The separation of aromatics from aliphatics is essential for achieving maximum exploitation of oil resources in the petrochemical industry.In this study,a series of metal chloride-based ionic liquids were prepared and...The separation of aromatics from aliphatics is essential for achieving maximum exploitation of oil resources in the petrochemical industry.In this study,a series of metal chloride-based ionic liquids were prepared and their performances in the separation of 1,2,3,4-tetrahydronaphthalene(tetralin)/dodecane and tetralin/decalin systems were studied.Among these ionic liquids,1-ethyl-3-methylimidazolium tetrachloroferrate([EMIM][FeCl_(4)])with the highest selectivity was used as the extractant.Density functional theory calculations showed that[EMIM][FeCl_(4)]interacted more strongly with tetralin than with dodecane and decalin.Energy decomposition analysis of[EMIM][FeCl_(4)]-tetralin indicated that electrostatics and dispersion played essential roles,and induction cannot be neglected.The van der Waals forces was a main effect in[EMIM][FeCl_(4)]-tetralin by independent gradient model analysis.The tetralin distribution coefficient and selectivity were 0.8 and 110,respectively,with 10%(mol)tetralin in the initial tetralin/dodecane system,and 0.67 and 19.5,respectively,with 10%(mol)tetralin in the initial tetralin/decalin system.The selectivity increased with decreasing alkyl chain length of the extractant.The influence of the extraction temperature,extractant dosage,and initial concentrations of the system components on the separation performance were studied.Recycling experiments showed that the regenerated[EMIM][FeCl_(4)]could be used repeatedly.展开更多
Rice is one of the most widely cultivated cereals in the world, and its aroma is increasingly in demand. With the advancement of research, a major rice flavor gene has been identified on rice chromosome 8. It encodes ...Rice is one of the most widely cultivated cereals in the world, and its aroma is increasingly in demand. With the advancement of research, a major rice flavor gene has been identified on rice chromosome 8. It encodes non-functional betaine aldehyde dehydrogenase leading to the accumulation of 2-acetyl-1-pyrroline which is the major olfactory compound that confers the fragrant character to rice. The aroma of rice is considered a special trait of enormous economic importance that determines the prime price in world trade. To satisfy the needs of the population and reduce rice imports into Benin, we conducted this study to identify aromatic rice accessions grown in Benin. Seventy-two rice accessions collected across Benin were PCR amplified with three SSR markers RM 7049, Aro 7, and RM 223, linked to the fgr (fragrance of rice) aroma gene. Molecular analysis revealed that 12 of the 72 accessions, namely Bagou 19, Bagou 22, Tchaka 34, Foun 15, Tchaka 41, Nana 32, Kan 61, Kung 69, Kung 67, Bagou 20, Agbab 101 and Koum 55 possess the fgr gene and can be considered as aromatic rice accessions. A sensory phenotypic test using KOH was carried out on rice accessions carrying fgr gene. Of the twelve positives, only one had the smell of aromatic rice, like the Azucena control. These results show that Benin also has aromatic rice varieties that can be sold on national and international markets.展开更多
In order to obtain liquefied products with higher yields of aromatic molecules to produce mesophase pitch,a good understanding of the relevant reaction mechanisms is required.Reactive molecular dynamics simulations we...In order to obtain liquefied products with higher yields of aromatic molecules to produce mesophase pitch,a good understanding of the relevant reaction mechanisms is required.Reactive molecular dynamics simulations were used to study the thermal reactions of pyrene,1-methylpyrene,7,8,9,10-tetrahydrobenzopyrene,and mixtures of pyrene with 1-octene,cyclohexene,or styrene.The reactant conversion rates,reaction rates,and product distributions were calculated and compared,and the mechanisms were analyzed and discussed.The results demonstrated that methyl and naphthenic structures in aromatics might improve the conversion rates of reactants in hydrogen transfer processes,but their steric hindrances prohibited the generation of high polymers.The naphthenic structures could generate more free radicals and presented a more obvious inhibition effect on the condensation of polymers compared with the methyl side chains.It was discovered that when different olefins were mixed with pyrene,1-octene primarily underwent pyrolysis reactions,whereas cyclohexene mainly underwent hydrogen transfer reactions with pyrene and styrene,mostly producing superconjugated biradicals through condensation reactions with pyrene.In the mixture systems,the olefins scattered aromatic molecules,hindering the formation of pyrene trimers and higher polymers.According to the reactive molecular dynamics simulations,styrene may enhance the yield of dimer and enable the controlled polycondensation of pyrene.展开更多
Drought poses a significant challenge,restricting the productivity of medicinal and aromatic plants.The strain induced by drought can impede vital processes like respiration and photosynthesis,affecting various aspect...Drought poses a significant challenge,restricting the productivity of medicinal and aromatic plants.The strain induced by drought can impede vital processes like respiration and photosynthesis,affecting various aspects of plants’growth and metabolism.In response to this adversity,medicinal plants employ mechanisms such as morphological and structural adjustments,modulation of drought-resistant genes,and augmented synthesis of secondary metabolites and osmotic regulatory substances to alleviate the stress.Extreme water scarcity can lead to leaf wilting and may ultimately result in plant death.The cultivation and management of medicinal plants under stress conditions often differ from those of other crops.This is because the main goal with medicinal plants is not only to increase the yield of the above-ground parts but also to enhance the production of active ingredients such as essential oils.To elucidate these mechanisms of drought resistance in medicinal and aromatic plants,the current review provides a summary of recent literature encompassing studies on the morphology,physiology,and biochemistry of medicinal and aromatic plants under drought conditions.展开更多
The separation of aromatic/aliphatic hydrocarbon mixtures is crucial in the petrochemical industry.Pervaporation is regarded as a promising approach for the separation of aromatic compounds from alkanes. Developing me...The separation of aromatic/aliphatic hydrocarbon mixtures is crucial in the petrochemical industry.Pervaporation is regarded as a promising approach for the separation of aromatic compounds from alkanes. Developing membrane materials with efficient separation performance is still the main task since the membrane should provide chemical stability, high permeation flux, and selectivity. In this study, the hyperbranched polymer(HBP) was deposited on the outer surface of a polyvinylidene fluoride(PVDF)hollow-fiber ultrafiltration membrane by a facile dip-coating method. The dip-coating rate, HBP concentration, and thermal cross-linking temperature were regulated to optimize the membrane structure.The obtained HBP/PVDF hollow-fiber-composite membrane had a good separation performance for aromatic/aliphatic hydrocarbon mixtures. For the 50%/50%(mass) toluene/n-heptane mixture, the permeation flux of optimized composite membranes could reach 1766 g·m^(-2)·h^(-1), with a separation factor of 4.1 at 60℃. Therefore, the HBP/PVDF hollow-fiber-composite membrane has great application prospects in the pervaporation separation of aromatic/aliphatic hydrocarbon mixtures.展开更多
Porous aromatic framework 1(PAF-1)is an extremely representative nanoporous organic framework owing to its high stability and exceptionally high surface area.Currently,the synthesis of PAF-1 is catalyzed by the Ni(COD...Porous aromatic framework 1(PAF-1)is an extremely representative nanoporous organic framework owing to its high stability and exceptionally high surface area.Currently,the synthesis of PAF-1 is catalyzed by the Ni(COD)2/COD/bpy system,suffering from great instability and high cost.Herein,we developed an in situ reduction of the Ni(II)catalytic system to synthesize PAF-1 in low cost and high yield.The active Ni(0)species produced from the NiCl_(2)/bpy/NaI/Mg catalyst system can effectively catalyze homocoupling of tetrakis(4-bromophenyl)methane at the room temperature to form PAF-1 with high Brunauer-Emmett-Teller(BET)-specific surface area up to 4948 m^(2) g^(−1)(Langmuir surface area,6785 m2 g−1).The possible halogen exchange and dehalogenation coupling mechanisms for this new catalytic process in PAF's synthesis are discussed in detail.The efficiency and universality of this innovative catalyst system have also been demonstrated in other PAFs'synthesis.This work provides a cheap,facile,and efficient method for scalable synthesis of PAFs and explores their application for high-pressure storage of Xe and Kr.展开更多
Objective To investigate changes in the urinary metabolite profiles of children exposed to polycyclic aromatic hydrocarbons(PAHs)during critical brain development and explore their potential link with the intestinal m...Objective To investigate changes in the urinary metabolite profiles of children exposed to polycyclic aromatic hydrocarbons(PAHs)during critical brain development and explore their potential link with the intestinal microbiota.Methods Liquid chromatography-tandem mass spectrometry was used to determine ten hydroxyl metabolites of PAHs(OH-PAHs)in 36-month-old children.Subsequently,37 children were categorized into low-and high-exposure groups based on the sum of the ten OH-PAHs.Ultra-high-performance liquid chromatography coupled with quadrupole time-of-flight mass spectrometry was used to identify non-targeted metabolites in the urine samples.Furthermore,fecal flora abundance was assessed by 16S rRNA gene sequencing using Illumina MiSeq.Results The concentrations of 21 metabolites were significantly higher in the high exposure group than in the low exposure group(variable importance for projection>1,P<0.05).Most of these metabolites were positively correlated with the hydroxyl metabolites of naphthalene,fluorine,and phenanthrene(r=0.336–0.531).The identified differential metabolites primarily belonged to pathways associated with inflammation or proinflammatory states,including amino acid,lipid,and nucleotide metabolism.Additionally,these distinct metabolites were significantly associated with specific intestinal flora abundances(r=0.34–0.55),which were mainly involved in neurodevelopment.Conclusion Higher PAH exposure in young children affected metabolic homeostasis,particularly that of certain gut microbiota-derived metabolites.Further investigation is needed to explore the potential influence of PAHs on the gut microbiota and their possible association with neurodevelopmental outcomes.展开更多
Applying iodine fertilizers to cultivate iodine-rich crops for daily intake is an effective approach for iodine supplementation,especially for aromatic rice.Field experiments were conducted during the early growing se...Applying iodine fertilizers to cultivate iodine-rich crops for daily intake is an effective approach for iodine supplementation,especially for aromatic rice.Field experiments were conducted during the early growing seasons of 2021 and 2022 to evaluate the impacts of foliar application of iodine fertilizer on aromatic rice and to explore the optimal iodine fertilizer concentration.At the full heading stage,six different concentrations of sodium iodide solutions of 0%(CK),0.010%(T1),0.025%(T2),0.050%(T3),0.075%(T4),and 0.100%(T5)were applied to indica aromatic rice cultivars Meixiangzhan 2 and Xiangyaxiangzhan.The results showed that sodium iodide treatments significantly increased the iodine and sodium contents in both leaves and grains.Compared with the CK,the T1 and T2 treatments increased the 2-acetyl-1-pyrroline(2-AP)content in mature grains by 8.41%-101.66%and 13.58%-74.60%,respectively.Improvements in the contents of 1-pyrroline-5-carboxylic acid,proline,1-pyrroline,and methylglyoxal,as well as the activity of proline dehydrogenase were also detected.Additionally,sodium iodide treatments remarkably decreased the chalky grain rate,chalkiness area,and chalkiness degree of aromatic rice,with the T2 treatment exhibiting a 17.79%-47.42%decrease in chalkiness degree compared with the CK.Meanwhile,T1 and T2 treatments showed beneficial impacts on chlorophyll content,photosynthetic characteristics,and yield components,while T3,T4,and T5 treatments exhibited adverse effects on leaf and grain yields.The linear discriminant analysis revealed significant differences between treatments.The correlation analysis and piecewise structural equation modeling showed that the iodine and sodium influenced the photosynthetic characteristics and chlorophyll content of the leaves,thereby regulating the 2-AP biosynthesis and yield components,ultimately affecting the 2-AP content and yield.Overall,this study suggests that foliar application of 0.025%sodium iodide is an effective method to enrich the iodine content in rice grains,improve the grain aroma and appearance quality of aromatic rice,without detrimental effects on grain yield.展开更多
In this paper, the preparation technique of lavender essential oil microcapsules and the construction method of aromatic textiles were expounded, and the research status of bed curtains and lavender microcapsules at h...In this paper, the preparation technique of lavender essential oil microcapsules and the construction method of aromatic textiles were expounded, and the research status of bed curtains and lavender microcapsules at home and abroad was analyzed and studied from the perspective of application in textiles. The application of lavender essential oil to bed curtains through the microcapsule technique was put forward to allow lavender essential oil to play its role of helping sleep in bed curtains. This paper expounded the material selection and preparation technique of lavender microcapsule agents, and put forward the preparation method of microcapsules with mixed solutions of pure Chinese medicine extracts and natural essences as core material and high-viscosity epoxy resin as wall materials. The post-processing techniques and the spray ironing method for clothing were studied and developed, and these techniques and methods were applied to bed curtains, and good results were obtained.展开更多
The aromatic compounds,including o-xylene,m-xylene,p-xylene,and ethylbenzene,primarily originate from the catalytic reforming of crude oil,and have a wide variety of applications.However,because of similar physical an...The aromatic compounds,including o-xylene,m-xylene,p-xylene,and ethylbenzene,primarily originate from the catalytic reforming of crude oil,and have a wide variety of applications.However,because of similar physical and chemical properties,these compounds are difficult to be identified by gas chromatography(GC)without standard samples.With the development of modern nuclear magnetic resonance(NMR)techniques,NMR has emerged as a powerful and efficient tool for the rapid analysis of complex and crude mixtures without purification.In this study,the parameters of one-dimensional(1D)total correlation spectroscopy(TOCSY)NMR techniques,including 1D selective gradient TOCSY and 1D chemicalshift-selective filtration(CSSF)with TOCSY,were optimized to obtain comprehensive molecular structure information.The results indicate that the overlapped signals in NMR spectra of nonpolar aromatic compounds(including o-xylene,m-xylene,p-xylene and ethylbenzene),polar aromatic compounds(benzyl alcohol,benzaldehyde,benzoic acid),and aromatic compounds with additional conjugated bonds(styrene)can be resolved in 1D TOCSY.More importantly,full molecular structures can be clearly distinguished by setting appropriate mixing time in 1D TOCSY.This approach simplifies the NMR spectra,provides structural information of entire molecules,and can be applied for the analysis of other structural isomers.展开更多
Petroleum hydrocarbon pollution is a global concern,particularly in coastal environments.Polycyclic aromatic hydrocarbons(PAHs) are regarded as the most toxic components of petroleum hydrocarbons.In this study,the bio...Petroleum hydrocarbon pollution is a global concern,particularly in coastal environments.Polycyclic aromatic hydrocarbons(PAHs) are regarded as the most toxic components of petroleum hydrocarbons.In this study,the biomonitoring and ranking effects of petroleum hydrocarbons and PAHs on the marine fish model Oryzias melastigma embryos were determined in the Jiulong River Estuary(JRE) and its adjacent waters in China.The results showed that the levels of petroleum hydrocarbons from almost all sites met the primary standard for marine seawater quality,and the concentrations of the 16 priority PAHs in the surface seawater were lower compared with those in other coastal areas worldwide.A new fish expert system based on the embryotoxicity of O.melastigma(OME-FES) was developed and applied in the field to evaluate the biological effects of petroleum hydrocarbons and PAHs.The selected physiological index and molecular indicators in OME-FES were appropriate biomarkers for indicating the harmful effects of petroleum hydrocarbons and PAHs.The outcome of OME-FES revealed that the biological effect levels of the sampling sites ranged from level Ⅰ(no stress) to level Ⅲ(medium stress),which is further corroborated by the findings of nested analysis of variance(ANOVA) models.Our results suggest that the OME-FES is an effective tool for evaluating and ranking the biological effects of marine petroleum hydrocarbons and PAHs.This method may also be applied to evaluate other marine pollutants based on its framework.展开更多
BACKGROUND The lack of specific predictors for type-2 diabetes mellitus(T2DM)severely impacts early intervention/prevention efforts.Elevated branched-chain amino acids(BCAAs:Isoleucine,leucine,valine)and aromatic amin...BACKGROUND The lack of specific predictors for type-2 diabetes mellitus(T2DM)severely impacts early intervention/prevention efforts.Elevated branched-chain amino acids(BCAAs:Isoleucine,leucine,valine)and aromatic amino acids(AAAs:Tyrosine,tryptophan,phenylalanine)show high sensitivity and specificity in predicting diabetes in animals and predict T2DM 10-19 years before T2DM onset in clinical studies.However,improvement is needed to support its clinical utility.AIM To evaluate the effects of body mass index(BMI)and sex on BCAAs/AAAs in new-onset T2DM individuals with varying body weight.METHODS Ninety-seven new-onset T2DM patients(<12 mo)differing in BMI[normal weight(NW),n=33,BMI=22.23±1.60;overweight,n=42,BMI=25.9±1.07;obesity(OB),n=22,BMI=31.23±2.31]from the First People’s Hospital of Yunnan Province,Kunming,China,were studied.One-way and 2-way ANOVAs were conducted to determine the effects of BMI and sex on BCAAs/AAAs.RESULTS Fasting serum AAAs,BCAAs,glutamate,and alanine were greater and high-density lipoprotein(HDL)was lower(P<0.05,each)in OB-T2DM patients than in NW-T2DM patients,especially in male OB-T2DM patients.Arginine,histidine,leucine,methionine,and lysine were greater in male patients than in female patients.Moreover,histidine,alanine,glutamate,lysine,valine,methionine,leucine,isoleucine,tyrosine,phenylalanine,and tryptophan were significantly correlated with abdominal adiposity,body weight and BMI,whereas isoleucine,leucine and phenylalanine were negatively correlated with HDL.CONCLUSION Heterogeneously elevated amino acids,especially BCAAs/AAAs,across new-onset T2DM patients in differing BMI categories revealed a potentially skewed prediction of T2DM development.The higher BCAA/AAA levels in obese T2DM patients would support T2DM prediction in obese individuals,whereas the lower levels of BCAAs/AAAs in NW-T2DM individuals may underestimate T2DM risk in NW individuals.This potentially skewed T2DM prediction should be considered when BCAAs/AAAs are to be used as the T2DM predictor.展开更多
Polycyclic aromatic hydrocarbons(PAHs)are typical persistent organic pollutants(POPs)that are commonly found in the environment.They are carcinogenic,teratogenic,mutagenic and biodegradable obviously.In this paper,the...Polycyclic aromatic hydrocarbons(PAHs)are typical persistent organic pollutants(POPs)that are commonly found in the environment.They are carcinogenic,teratogenic,mutagenic and biodegradable obviously.In this paper,the modified mussel shells were used to adsorb and remove anthracene.The results show that the adsorption removal rate of the mussel shells was higher after calcination at 600℃.5%H_(3)PO_(4) solution was more suitable for shell treatment than 3 mol/L ZnCl_(2) solution.As the dosage of the modified shells was 0.5 g/L,the adsorption reached a stable state,and the removal rate of PAHs was about 69.44%;the adsorption efficiency rose with the increase of time.It can be seen that as a new and cheap biological adsorbent,the modified shells can be used to remove PAHs from wastewater.展开更多
The coking kinetics and reaction-regeneration on Zn/HZSM-5 (Zn/HZ) catalyst in the conversion of methanol to aromatics were investigated. The highest initial benzene, toluene and xylene (BTX) yield of ca. 67.7% wa...The coking kinetics and reaction-regeneration on Zn/HZSM-5 (Zn/HZ) catalyst in the conversion of methanol to aromatics were investigated. The highest initial benzene, toluene and xylene (BTX) yield of ca. 67.7% was obtained on fresh Zn/HZ catalyst, which showed the worst catalytic stability. The cycle of reaction-regeneration significantly modified the texture and acidity of Zn/HZ catalyst, which in turn affected its catalytic performance and coking behavior in methanol conversion to BTX. The residual carbon located on the surface of Zn/HZ catalyst led to the decrease of acid sites and the change on the acid sites distribution, which played an important roles on its activity and deactivation. It was found that the high B/L ratio and the low total acid sites concentration of the Zn/HZ catalyst favored to the high BTX yield and good catalytic stability in methanol conversion.展开更多
Nanosized Ga-containing ZSM-5 zeolites were prepared via isomorphous substitution and impregnation followed by characterized using various techniques. The catalytic performance of the zeolites for the aromatization of...Nanosized Ga-containing ZSM-5 zeolites were prepared via isomorphous substitution and impregnation followed by characterized using various techniques. The catalytic performance of the zeolites for the aromatization of 1-hexene was investigated. The results indicate that isomorphous substitution promotes the incorporation of Ga heteroatoms into the framework along with the formation of extra-framework GaO;species([GaO;]a) that have stronger interactions with the negative potential of the framework. In addition, based on the Py-IR results and catalytic performance, the [GaO;]aspecies with stronger Lewis acid sites produced a better synergism with moderate Br?nsted acid sites and thus improved the selectivity to aromatic compounds. However, the impregnation results in the formation of Ga;O;phase and small amounts of GaO;species that are mainly located on the external surface([GaO;];), which contribute to weaker Lewis acid sites due to weaker interactions with the zeolite framework. During 1-hexene aromatization, the nanosized Ga isomorphously substituted ZSM-5 zeolite samples(Gax-NZ5) exhibited better catalytic performance compared to the impregnated samples, and the highest aromatic yield(i.e.,65.4 wt%) was achieved over the Ga4.2-NZ5 sample, which contained with the highest Ga content.展开更多
Zn/ZSM-5(NZ2) and Zn/Ni/ZSM-5(NZ3) as the catalysts for methanol to aromatics(MTA) were synthesized by a simple ultrasonic impregnation. The textural and acid properties of all catalysts were characterized using...Zn/ZSM-5(NZ2) and Zn/Ni/ZSM-5(NZ3) as the catalysts for methanol to aromatics(MTA) were synthesized by a simple ultrasonic impregnation. The textural and acid properties of all catalysts were characterized using XRD, HRTEM, NH;-TPD, Py-IR, XPS, XRF and TG techniques. The XRD and HRTEM results showed that the basic zeolite structures were not affected much with the incorporation of Zn and Ni species. However, great changes have taken place in acid properties. The Py-IR and XPS results indicated that the Zn-Lewis acid sites(ZnOH;species), which have stronger interaction with the zeolite framework compared with ZnO species, were generated at the expense of B acid sites with the incorporation of zinc species. Moreover, the product analysis results showed that the incorporation of zinc species promoted the primary aromatization by enhancing the dehydroaromatization and suppressing the cracking and subsequent H-transfer reaction. Furthermore, the addition of Ni species well inhibited the loss of zinc species by converting partial ZnO species to ZnOH;species, and thus improved the aromatization activity and catalyst stability. The catalytic performance results showed that the NZ3 possess higher conversion of methanol in a longer time and lower average rate of coke formation compared with NZ2. In addition,the NZ3 also exhibited the highest yield of BTX as the reaction proceeds.展开更多
基金supported by National Natural Science Foundation of China(22021004).
文摘1-hexene aromatization is a promising technology to convert excess olefin in fluid catalytic cracking(FCC)gasoline to high-value benzene(B),toluene(T),and xylene.Besides,the increasing market demand of xylene has put forward higher requirements for new generation of catalyst.For increasing xylene yield in 1-hexene aromatization,the effect of mesopore structure and spatial distribution on product distribution and Zn loading was studied.Catalysts with different mesopore spatial distribution were prepared by post-treatment of parent HZSM-5 zeolite,including NaOH treatment,tetra-propylammonium hydroxide(TPAOH)treatment,and recrystallization.It was found the evenly distributed mesopore mainly prolongs the catalyst lifetime by enhancing diffusion properties but reduces the aromatics selectivity,as a result of damage of micropores close to the catalyst surface.While the selectivity of high-value xylene can be highly promoted when the mesopore is mainly distributed interior the catalyst.Besides,the state of loaded Zn was also affected by mesopores spatial distribution.On the optimized catalyst,the xylene selectivity was enhanced by 12.4%compared with conventional Zn-loaded parent HZSM-5 catalyst at conversion over 99%.It was attributed to the synergy effect of mesopores spatial distribution and optimized acid properties.This work reveals the role of mesopores in different spatial positions of 1-hexene aromatization catalysts in the reaction process and the influence on metal distribution,as well as their synergistic effect two on the improvement of xylene selectivity,which can improve our understanding of catalyst pore structure and be helpful for the rational design of high-efficient catalyst.
基金financial support from the National Natural Science Foundation of China(21978191 and 22278292)Key Research and Development Project of Shanxi Province(International Science and Technology Cooperation Program)(201803D421011)。
文摘Two-step conversion of methanol to aromatics via light hydrocarbons can significantly improve the conversion stability compared with direct aromatization of methanol,but it remains a challenge to achieve a high p-xylene(PX)selectivity.Herein,silica coating was firstly used to passivate external acid sites of ZSM-5 catalyst for the aromatization of light hydrocarbons by the chemical liquid deposition method.With the increase of SiO_(2) deposition,the density of the external acid sites of the catalyst was decreased from 0.1 to 0.03 mmol·g^(-1),which inhibited the surface secondary reactions and increased the PX/X from 34.6% to 60.0%.In view of the fact that the aromatization process in the second step was partly inhibited as methanol was consumed in advance in the upper methanol-to-light hydrocarbons catalyst layer,part of methanol was directly introduced into the lower aromatization catalyst layer to promote the alkylation process during the aromatization,which decreased the toluene selectivity from 34.5% to 14.3% but increased the xylene selectivity from 40.0%to 55.3%.It was also found that an appropriate external acid density was needed for aromatization catalyst to strengthen the alkylation process and improve the selectivity of xylene under the conditions of methanol introduction.
基金supported by the Open Project of Key Laboratory of Green Chemical Engineering Process of Ministry of Education[grant number GCP20190204]Hubei Key Laboratory of Novel Reactor and Green Chemistry Technology(Wuhan Institute of Technology)[grant number 40201005]+1 种基金Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education[grant number LKF201908]Graduate Innovative Fund of Wuhan Institute of Technology[grant number CX2021028].
文摘The ethylene aromatization is critical for the methanol to aromatics and light alkane dehydroaromatization process.The single-event microkinetic(SEMK)model combining the linear free energy theory and solid acid distribution concept were established and extend for the ethylene aromatization process,which can reduce the kinetic parameters and simplify the reaction network by comparison with the SEMK model including subtype elementary steps based on the type of carbenium ions.Further introducing deactivation parametersφinto the model and applying the linear free energy model to the deactivation experimental data,the obtained deactivation parametersφindicate that the carbon deposition precursors have the greatest impact on reducing the reaction rate of single-molecular reactions and the smallest impact on the hydrogen transfer reaction.Meanwhile,according to the change of reaction enthalpy,effect of carbenium ion structure on methylation,ethylation,cyclization and endo-βscission was investigated by introducing linear free energy concept into the SEMK model.The effect of different acid strengths on elementary steps was investigated based on the acid strength distribution model,it was found that the methylation and oligomerization reactions,the ali-βscission reaction,endo-βscission reaction and the cyclization reaction were more sensitive to strong acidity sites.The physisorption and chemisorption heat are separated from the protonation heat in the linear free energy kinetic model and the acid strength distribution kinetic model,and the absolute values of the obtained physisorption and chemisorption heat increase with the carbon number of carbenium ions.Furthermore,the parameters of the acid strength distribution kinetic model were applied to propane dehydroaromatization on H-ZSM-5 and the ethane dehydroaromatization on Zn/ZSM-5 to confirm the independence of parameters in the SEMK model with the similar reaction network.
基金supported by the National Natural Science Foundation of China(22125802,22078010).
文摘The separation of aromatics from aliphatics is essential for achieving maximum exploitation of oil resources in the petrochemical industry.In this study,a series of metal chloride-based ionic liquids were prepared and their performances in the separation of 1,2,3,4-tetrahydronaphthalene(tetralin)/dodecane and tetralin/decalin systems were studied.Among these ionic liquids,1-ethyl-3-methylimidazolium tetrachloroferrate([EMIM][FeCl_(4)])with the highest selectivity was used as the extractant.Density functional theory calculations showed that[EMIM][FeCl_(4)]interacted more strongly with tetralin than with dodecane and decalin.Energy decomposition analysis of[EMIM][FeCl_(4)]-tetralin indicated that electrostatics and dispersion played essential roles,and induction cannot be neglected.The van der Waals forces was a main effect in[EMIM][FeCl_(4)]-tetralin by independent gradient model analysis.The tetralin distribution coefficient and selectivity were 0.8 and 110,respectively,with 10%(mol)tetralin in the initial tetralin/dodecane system,and 0.67 and 19.5,respectively,with 10%(mol)tetralin in the initial tetralin/decalin system.The selectivity increased with decreasing alkyl chain length of the extractant.The influence of the extraction temperature,extractant dosage,and initial concentrations of the system components on the separation performance were studied.Recycling experiments showed that the regenerated[EMIM][FeCl_(4)]could be used repeatedly.
文摘Rice is one of the most widely cultivated cereals in the world, and its aroma is increasingly in demand. With the advancement of research, a major rice flavor gene has been identified on rice chromosome 8. It encodes non-functional betaine aldehyde dehydrogenase leading to the accumulation of 2-acetyl-1-pyrroline which is the major olfactory compound that confers the fragrant character to rice. The aroma of rice is considered a special trait of enormous economic importance that determines the prime price in world trade. To satisfy the needs of the population and reduce rice imports into Benin, we conducted this study to identify aromatic rice accessions grown in Benin. Seventy-two rice accessions collected across Benin were PCR amplified with three SSR markers RM 7049, Aro 7, and RM 223, linked to the fgr (fragrance of rice) aroma gene. Molecular analysis revealed that 12 of the 72 accessions, namely Bagou 19, Bagou 22, Tchaka 34, Foun 15, Tchaka 41, Nana 32, Kan 61, Kung 69, Kung 67, Bagou 20, Agbab 101 and Koum 55 possess the fgr gene and can be considered as aromatic rice accessions. A sensory phenotypic test using KOH was carried out on rice accessions carrying fgr gene. Of the twelve positives, only one had the smell of aromatic rice, like the Azucena control. These results show that Benin also has aromatic rice varieties that can be sold on national and international markets.
基金financially supported by the National Natural Science Foundation of China(Approval No.42172168).
文摘In order to obtain liquefied products with higher yields of aromatic molecules to produce mesophase pitch,a good understanding of the relevant reaction mechanisms is required.Reactive molecular dynamics simulations were used to study the thermal reactions of pyrene,1-methylpyrene,7,8,9,10-tetrahydrobenzopyrene,and mixtures of pyrene with 1-octene,cyclohexene,or styrene.The reactant conversion rates,reaction rates,and product distributions were calculated and compared,and the mechanisms were analyzed and discussed.The results demonstrated that methyl and naphthenic structures in aromatics might improve the conversion rates of reactants in hydrogen transfer processes,but their steric hindrances prohibited the generation of high polymers.The naphthenic structures could generate more free radicals and presented a more obvious inhibition effect on the condensation of polymers compared with the methyl side chains.It was discovered that when different olefins were mixed with pyrene,1-octene primarily underwent pyrolysis reactions,whereas cyclohexene mainly underwent hydrogen transfer reactions with pyrene and styrene,mostly producing superconjugated biradicals through condensation reactions with pyrene.In the mixture systems,the olefins scattered aromatic molecules,hindering the formation of pyrene trimers and higher polymers.According to the reactive molecular dynamics simulations,styrene may enhance the yield of dimer and enable the controlled polycondensation of pyrene.
文摘Drought poses a significant challenge,restricting the productivity of medicinal and aromatic plants.The strain induced by drought can impede vital processes like respiration and photosynthesis,affecting various aspects of plants’growth and metabolism.In response to this adversity,medicinal plants employ mechanisms such as morphological and structural adjustments,modulation of drought-resistant genes,and augmented synthesis of secondary metabolites and osmotic regulatory substances to alleviate the stress.Extreme water scarcity can lead to leaf wilting and may ultimately result in plant death.The cultivation and management of medicinal plants under stress conditions often differ from those of other crops.This is because the main goal with medicinal plants is not only to increase the yield of the above-ground parts but also to enhance the production of active ingredients such as essential oils.To elucidate these mechanisms of drought resistance in medicinal and aromatic plants,the current review provides a summary of recent literature encompassing studies on the morphology,physiology,and biochemistry of medicinal and aromatic plants under drought conditions.
基金financially supported by the National Natural Science Foundation of China (22178008, 22125801)Petrochina (2022DJ6004)。
文摘The separation of aromatic/aliphatic hydrocarbon mixtures is crucial in the petrochemical industry.Pervaporation is regarded as a promising approach for the separation of aromatic compounds from alkanes. Developing membrane materials with efficient separation performance is still the main task since the membrane should provide chemical stability, high permeation flux, and selectivity. In this study, the hyperbranched polymer(HBP) was deposited on the outer surface of a polyvinylidene fluoride(PVDF)hollow-fiber ultrafiltration membrane by a facile dip-coating method. The dip-coating rate, HBP concentration, and thermal cross-linking temperature were regulated to optimize the membrane structure.The obtained HBP/PVDF hollow-fiber-composite membrane had a good separation performance for aromatic/aliphatic hydrocarbon mixtures. For the 50%/50%(mass) toluene/n-heptane mixture, the permeation flux of optimized composite membranes could reach 1766 g·m^(-2)·h^(-1), with a separation factor of 4.1 at 60℃. Therefore, the HBP/PVDF hollow-fiber-composite membrane has great application prospects in the pervaporation separation of aromatic/aliphatic hydrocarbon mixtures.
基金National Natural Science Foundation of China,Grant/Award Numbers:21975096,22178280Key Laboratory of Nuclear Data Foundation,Grant/Award Number:JCKY2021201C151Young Talent Support Plan,Grant/Award Number:HG6J001。
文摘Porous aromatic framework 1(PAF-1)is an extremely representative nanoporous organic framework owing to its high stability and exceptionally high surface area.Currently,the synthesis of PAF-1 is catalyzed by the Ni(COD)2/COD/bpy system,suffering from great instability and high cost.Herein,we developed an in situ reduction of the Ni(II)catalytic system to synthesize PAF-1 in low cost and high yield.The active Ni(0)species produced from the NiCl_(2)/bpy/NaI/Mg catalyst system can effectively catalyze homocoupling of tetrakis(4-bromophenyl)methane at the room temperature to form PAF-1 with high Brunauer-Emmett-Teller(BET)-specific surface area up to 4948 m^(2) g^(−1)(Langmuir surface area,6785 m2 g−1).The possible halogen exchange and dehalogenation coupling mechanisms for this new catalytic process in PAF's synthesis are discussed in detail.The efficiency and universality of this innovative catalyst system have also been demonstrated in other PAFs'synthesis.This work provides a cheap,facile,and efficient method for scalable synthesis of PAFs and explores their application for high-pressure storage of Xe and Kr.
基金partly supported by grants from the National Natural Science Foundation of China(No:81372955)BiosTime Maternal and Infant Nutrition and Health Research Fund(2017FYH008)+1 种基金the Projects of Medical and Health Technology Development Program in Shandong Province(No:2016WS0309)Qingdao Outstanding Health Professional Development Fund(2020-2022,2022-2024)。
文摘Objective To investigate changes in the urinary metabolite profiles of children exposed to polycyclic aromatic hydrocarbons(PAHs)during critical brain development and explore their potential link with the intestinal microbiota.Methods Liquid chromatography-tandem mass spectrometry was used to determine ten hydroxyl metabolites of PAHs(OH-PAHs)in 36-month-old children.Subsequently,37 children were categorized into low-and high-exposure groups based on the sum of the ten OH-PAHs.Ultra-high-performance liquid chromatography coupled with quadrupole time-of-flight mass spectrometry was used to identify non-targeted metabolites in the urine samples.Furthermore,fecal flora abundance was assessed by 16S rRNA gene sequencing using Illumina MiSeq.Results The concentrations of 21 metabolites were significantly higher in the high exposure group than in the low exposure group(variable importance for projection>1,P<0.05).Most of these metabolites were positively correlated with the hydroxyl metabolites of naphthalene,fluorine,and phenanthrene(r=0.336–0.531).The identified differential metabolites primarily belonged to pathways associated with inflammation or proinflammatory states,including amino acid,lipid,and nucleotide metabolism.Additionally,these distinct metabolites were significantly associated with specific intestinal flora abundances(r=0.34–0.55),which were mainly involved in neurodevelopment.Conclusion Higher PAH exposure in young children affected metabolic homeostasis,particularly that of certain gut microbiota-derived metabolites.Further investigation is needed to explore the potential influence of PAHs on the gut microbiota and their possible association with neurodevelopmental outcomes.
基金supported by the National Natural Science Foundation of China(Grant No.31971843)the Technology System of Modern Agricultural Industry in Guangdong Province,China(Grant No.2020KJ105)+1 种基金the Guangzhou Science and Technology Project,Guangdong Province,China(Grant No.202103000075)the Special Rural Revitalization Funds of Guangdong Province,China(Grant No.2021KJ382)。
文摘Applying iodine fertilizers to cultivate iodine-rich crops for daily intake is an effective approach for iodine supplementation,especially for aromatic rice.Field experiments were conducted during the early growing seasons of 2021 and 2022 to evaluate the impacts of foliar application of iodine fertilizer on aromatic rice and to explore the optimal iodine fertilizer concentration.At the full heading stage,six different concentrations of sodium iodide solutions of 0%(CK),0.010%(T1),0.025%(T2),0.050%(T3),0.075%(T4),and 0.100%(T5)were applied to indica aromatic rice cultivars Meixiangzhan 2 and Xiangyaxiangzhan.The results showed that sodium iodide treatments significantly increased the iodine and sodium contents in both leaves and grains.Compared with the CK,the T1 and T2 treatments increased the 2-acetyl-1-pyrroline(2-AP)content in mature grains by 8.41%-101.66%and 13.58%-74.60%,respectively.Improvements in the contents of 1-pyrroline-5-carboxylic acid,proline,1-pyrroline,and methylglyoxal,as well as the activity of proline dehydrogenase were also detected.Additionally,sodium iodide treatments remarkably decreased the chalky grain rate,chalkiness area,and chalkiness degree of aromatic rice,with the T2 treatment exhibiting a 17.79%-47.42%decrease in chalkiness degree compared with the CK.Meanwhile,T1 and T2 treatments showed beneficial impacts on chlorophyll content,photosynthetic characteristics,and yield components,while T3,T4,and T5 treatments exhibited adverse effects on leaf and grain yields.The linear discriminant analysis revealed significant differences between treatments.The correlation analysis and piecewise structural equation modeling showed that the iodine and sodium influenced the photosynthetic characteristics and chlorophyll content of the leaves,thereby regulating the 2-AP biosynthesis and yield components,ultimately affecting the 2-AP content and yield.Overall,this study suggests that foliar application of 0.025%sodium iodide is an effective method to enrich the iodine content in rice grains,improve the grain aroma and appearance quality of aromatic rice,without detrimental effects on grain yield.
基金Supported by Undergraduate Training Program for Innovation and Entrepreneurship of Guangxi University of Chinese Medicine in 2023(S202310600084)。
文摘In this paper, the preparation technique of lavender essential oil microcapsules and the construction method of aromatic textiles were expounded, and the research status of bed curtains and lavender microcapsules at home and abroad was analyzed and studied from the perspective of application in textiles. The application of lavender essential oil to bed curtains through the microcapsule technique was put forward to allow lavender essential oil to play its role of helping sleep in bed curtains. This paper expounded the material selection and preparation technique of lavender microcapsule agents, and put forward the preparation method of microcapsules with mixed solutions of pure Chinese medicine extracts and natural essences as core material and high-viscosity epoxy resin as wall materials. The post-processing techniques and the spray ironing method for clothing were studied and developed, and these techniques and methods were applied to bed curtains, and good results were obtained.
基金We thank the Natural Science Foundation of Shanxi Province(202103021224439)National Natural Science Foundation of China(22075308)for financial support.
文摘The aromatic compounds,including o-xylene,m-xylene,p-xylene,and ethylbenzene,primarily originate from the catalytic reforming of crude oil,and have a wide variety of applications.However,because of similar physical and chemical properties,these compounds are difficult to be identified by gas chromatography(GC)without standard samples.With the development of modern nuclear magnetic resonance(NMR)techniques,NMR has emerged as a powerful and efficient tool for the rapid analysis of complex and crude mixtures without purification.In this study,the parameters of one-dimensional(1D)total correlation spectroscopy(TOCSY)NMR techniques,including 1D selective gradient TOCSY and 1D chemicalshift-selective filtration(CSSF)with TOCSY,were optimized to obtain comprehensive molecular structure information.The results indicate that the overlapped signals in NMR spectra of nonpolar aromatic compounds(including o-xylene,m-xylene,p-xylene and ethylbenzene),polar aromatic compounds(benzyl alcohol,benzaldehyde,benzoic acid),and aromatic compounds with additional conjugated bonds(styrene)can be resolved in 1D TOCSY.More importantly,full molecular structures can be clearly distinguished by setting appropriate mixing time in 1D TOCSY.This approach simplifies the NMR spectra,provides structural information of entire molecules,and can be applied for the analysis of other structural isomers.
基金The Scientific Research Foundation of the Third Institute of Oceanography,Ministry of Natural Resources under contract Nos 2020014 and 2020017the National Natural Science Foundation of China under contract No. 41977211the National Program on Global Change and Air-Sea Interaction under contract No. GASI-02-SCS-YDsum。
文摘Petroleum hydrocarbon pollution is a global concern,particularly in coastal environments.Polycyclic aromatic hydrocarbons(PAHs) are regarded as the most toxic components of petroleum hydrocarbons.In this study,the biomonitoring and ranking effects of petroleum hydrocarbons and PAHs on the marine fish model Oryzias melastigma embryos were determined in the Jiulong River Estuary(JRE) and its adjacent waters in China.The results showed that the levels of petroleum hydrocarbons from almost all sites met the primary standard for marine seawater quality,and the concentrations of the 16 priority PAHs in the surface seawater were lower compared with those in other coastal areas worldwide.A new fish expert system based on the embryotoxicity of O.melastigma(OME-FES) was developed and applied in the field to evaluate the biological effects of petroleum hydrocarbons and PAHs.The selected physiological index and molecular indicators in OME-FES were appropriate biomarkers for indicating the harmful effects of petroleum hydrocarbons and PAHs.The outcome of OME-FES revealed that the biological effect levels of the sampling sites ranged from level Ⅰ(no stress) to level Ⅲ(medium stress),which is further corroborated by the findings of nested analysis of variance(ANOVA) models.Our results suggest that the OME-FES is an effective tool for evaluating and ranking the biological effects of marine petroleum hydrocarbons and PAHs.This method may also be applied to evaluate other marine pollutants based on its framework.
基金Supported by the Open Project Grant for Clinical Medical Center of Yunnan Province,No.2019LCZXKF-NM03Medical Leader Training Grant,No.L-201624and Yunnan Province Ten Thousand Talents:“Medical Expert”grant,No.YNWR-MY-2019-020.
文摘BACKGROUND The lack of specific predictors for type-2 diabetes mellitus(T2DM)severely impacts early intervention/prevention efforts.Elevated branched-chain amino acids(BCAAs:Isoleucine,leucine,valine)and aromatic amino acids(AAAs:Tyrosine,tryptophan,phenylalanine)show high sensitivity and specificity in predicting diabetes in animals and predict T2DM 10-19 years before T2DM onset in clinical studies.However,improvement is needed to support its clinical utility.AIM To evaluate the effects of body mass index(BMI)and sex on BCAAs/AAAs in new-onset T2DM individuals with varying body weight.METHODS Ninety-seven new-onset T2DM patients(<12 mo)differing in BMI[normal weight(NW),n=33,BMI=22.23±1.60;overweight,n=42,BMI=25.9±1.07;obesity(OB),n=22,BMI=31.23±2.31]from the First People’s Hospital of Yunnan Province,Kunming,China,were studied.One-way and 2-way ANOVAs were conducted to determine the effects of BMI and sex on BCAAs/AAAs.RESULTS Fasting serum AAAs,BCAAs,glutamate,and alanine were greater and high-density lipoprotein(HDL)was lower(P<0.05,each)in OB-T2DM patients than in NW-T2DM patients,especially in male OB-T2DM patients.Arginine,histidine,leucine,methionine,and lysine were greater in male patients than in female patients.Moreover,histidine,alanine,glutamate,lysine,valine,methionine,leucine,isoleucine,tyrosine,phenylalanine,and tryptophan were significantly correlated with abdominal adiposity,body weight and BMI,whereas isoleucine,leucine and phenylalanine were negatively correlated with HDL.CONCLUSION Heterogeneously elevated amino acids,especially BCAAs/AAAs,across new-onset T2DM patients in differing BMI categories revealed a potentially skewed prediction of T2DM development.The higher BCAA/AAA levels in obese T2DM patients would support T2DM prediction in obese individuals,whereas the lower levels of BCAAs/AAAs in NW-T2DM individuals may underestimate T2DM risk in NW individuals.This potentially skewed T2DM prediction should be considered when BCAAs/AAAs are to be used as the T2DM predictor.
基金the Technology Research Project(LGF22D060003)Zhoushan Municipal Science and Technology Cooperation(Active Design)Project(2023C13015).
文摘Polycyclic aromatic hydrocarbons(PAHs)are typical persistent organic pollutants(POPs)that are commonly found in the environment.They are carcinogenic,teratogenic,mutagenic and biodegradable obviously.In this paper,the modified mussel shells were used to adsorb and remove anthracene.The results show that the adsorption removal rate of the mussel shells was higher after calcination at 600℃.5%H_(3)PO_(4) solution was more suitable for shell treatment than 3 mol/L ZnCl_(2) solution.As the dosage of the modified shells was 0.5 g/L,the adsorption reached a stable state,and the removal rate of PAHs was about 69.44%;the adsorption efficiency rose with the increase of time.It can be seen that as a new and cheap biological adsorbent,the modified shells can be used to remove PAHs from wastewater.
基金supported by the National Ministry of Education(NCET-10-878)Shaanxi"13115"Innovation Project(2009ZDKJ-70)Shaanxi Key Innovation Project(2011ZKC4-08)
文摘The coking kinetics and reaction-regeneration on Zn/HZSM-5 (Zn/HZ) catalyst in the conversion of methanol to aromatics were investigated. The highest initial benzene, toluene and xylene (BTX) yield of ca. 67.7% was obtained on fresh Zn/HZ catalyst, which showed the worst catalytic stability. The cycle of reaction-regeneration significantly modified the texture and acidity of Zn/HZ catalyst, which in turn affected its catalytic performance and coking behavior in methanol conversion to BTX. The residual carbon located on the surface of Zn/HZ catalyst led to the decrease of acid sites and the change on the acid sites distribution, which played an important roles on its activity and deactivation. It was found that the high B/L ratio and the low total acid sites concentration of the Zn/HZ catalyst favored to the high BTX yield and good catalytic stability in methanol conversion.
基金supported by the National Natural Science Foundation of China(Nos.21276067 and 21676074)Programs of International S&T cooperation(No.2014DFR41110)
文摘Nanosized Ga-containing ZSM-5 zeolites were prepared via isomorphous substitution and impregnation followed by characterized using various techniques. The catalytic performance of the zeolites for the aromatization of 1-hexene was investigated. The results indicate that isomorphous substitution promotes the incorporation of Ga heteroatoms into the framework along with the formation of extra-framework GaO;species([GaO;]a) that have stronger interactions with the negative potential of the framework. In addition, based on the Py-IR results and catalytic performance, the [GaO;]aspecies with stronger Lewis acid sites produced a better synergism with moderate Br?nsted acid sites and thus improved the selectivity to aromatic compounds. However, the impregnation results in the formation of Ga;O;phase and small amounts of GaO;species that are mainly located on the external surface([GaO;];), which contribute to weaker Lewis acid sites due to weaker interactions with the zeolite framework. During 1-hexene aromatization, the nanosized Ga isomorphously substituted ZSM-5 zeolite samples(Gax-NZ5) exhibited better catalytic performance compared to the impregnated samples, and the highest aromatic yield(i.e.,65.4 wt%) was achieved over the Ga4.2-NZ5 sample, which contained with the highest Ga content.
基金entrusted by the Project of "utilization of low rank coal" strategic leading special fundstrategic leading special fund of CAS (XDA-07070800 and XDA-07070400)the Opening Foundation of State Key Laboratory of Coal Conversion (J16-17-602)
文摘Zn/ZSM-5(NZ2) and Zn/Ni/ZSM-5(NZ3) as the catalysts for methanol to aromatics(MTA) were synthesized by a simple ultrasonic impregnation. The textural and acid properties of all catalysts were characterized using XRD, HRTEM, NH;-TPD, Py-IR, XPS, XRF and TG techniques. The XRD and HRTEM results showed that the basic zeolite structures were not affected much with the incorporation of Zn and Ni species. However, great changes have taken place in acid properties. The Py-IR and XPS results indicated that the Zn-Lewis acid sites(ZnOH;species), which have stronger interaction with the zeolite framework compared with ZnO species, were generated at the expense of B acid sites with the incorporation of zinc species. Moreover, the product analysis results showed that the incorporation of zinc species promoted the primary aromatization by enhancing the dehydroaromatization and suppressing the cracking and subsequent H-transfer reaction. Furthermore, the addition of Ni species well inhibited the loss of zinc species by converting partial ZnO species to ZnOH;species, and thus improved the aromatization activity and catalyst stability. The catalytic performance results showed that the NZ3 possess higher conversion of methanol in a longer time and lower average rate of coke formation compared with NZ2. In addition,the NZ3 also exhibited the highest yield of BTX as the reaction proceeds.