Ethylene(C_(2)H_(4))is a core raw material for the petrochemical industry.It is of economic and environmental significance to use C_(2)H_(6)as the fuel and proton-conducting solid oxide fuel cells(P-SOFC)as the reacto...Ethylene(C_(2)H_(4))is a core raw material for the petrochemical industry.It is of economic and environmental significance to use C_(2)H_(6)as the fuel and proton-conducting solid oxide fuel cells(P-SOFC)as the reactor to co-generate electricity and C_(2)H_(4).However,the large-sized Ni particles in the conventional Nicermet anode directly crack C_(2)H_(6);and oxide materials with a mild capability of breaking C-C bonds are generally limited to electrolyte-supported structures with high ohmic impedance.This research for the first time constructs an anode-supported cell using BZCY as the porous scaffold and impregnated double perovskite(PrBa)_(0.95)(Fe_(0.8)Ni_(0.2))_(1.8)Mo_(0.2)O_(6-δ)(PBFNM0.2)as the anode electrocatalysis.FeNi3 nanoparticles exsolve from PBFNM0.2 in H_(2) and uniformly distribute on the surface of perovskite substrate,acting as an active component for C_(2)H_(6)dehydrogenation and electrochemical performance enhancement.The cell with 30 wt%PBFNM0.2 impregnated anode showing a high power density of 508 and 386mW/cm^(2) with H_(2) and C_(2)H_(6)fuels,respectively;high C_(2)H_(6)conversion of 50.9%,C_(2)H_(4)selectivity of 92.1%,and C_(2)H_(4)yield of 46.9%are achieved at 750℃and 700mA/cm^(2),which outperforms all previously electrolyte-supported cells for co-generated electricity and ethylene.Moreover,the cell demonstrated excellent recoverability throughout three dehydrogenation-regeneration cycles.This work provides a practical way with broad application potential to create a novel anode-supported cell efficiently realizing the co-generation of electricity and C_(2)H_(4)from C_(2)H_(6).展开更多
In response to the increasing demand of ethylene,electrochemical ethane nonoxidative dehydrogenation(EENDH)to ethylene by protonic ceramic electrolysis cells(PCECs)is developed.However,existing anode materials exhibit...In response to the increasing demand of ethylene,electrochemical ethane nonoxidative dehydrogenation(EENDH)to ethylene by protonic ceramic electrolysis cells(PCECs)is developed.However,existing anode materials exhibit poor proton conductivity and limited catalytic activity.Herein,a novel Sr_(1.95)Fe_(1.4)Co_(0.1)Mo_(0.4)Zr_(0.1)O_(6-δ)(SFCMZ)anode is prepared as PCECs anode for EENDH.Zr doping increases the oxygen vacancies and enhances the proton conductivity of SFCMZ.Moreover,an alloy-oxide heterostructure(Co Fe@SFCMZ)is formed through in-situ exsolution of Co Fe alloy nanoparticles under reduction conditions,generating abundant oxygen vacancies and improving its catalytic activity.Co Fe@SFCMZ cell achieves an electrolysis current density of 0.87 A/cm^(2) at 700℃ under 1.6 V,with an ethane conversion rate of 34.22%and corresponding ethylene selectivity of 93.4%.These results demonstrate that Co Fe@SFCMZ anode exhibits excellent electrocatalytic activity,suggesting promising applications for EENDH.展开更多
Chemical-looping oxidative dehydrogenation(CL-ODH)is a process designed for the conversion of alkanes into olefins through cyclic redox reactions,eliminating the need for gaseous O_(2).In this work,we investigated the...Chemical-looping oxidative dehydrogenation(CL-ODH)is a process designed for the conversion of alkanes into olefins through cyclic redox reactions,eliminating the need for gaseous O_(2).In this work,we investigated the use of Ca_(2)MnO_(4)-layered perovskites modified with NaNO_(3) dopants,serving as redox catalysts(also known as oxygen carriers),for the CL-ODH of ethane within a temperature range of 700-780℃.Our findings revealed that the incorporation of NaNO_(3) as a modifier significantly-nhanced the selectivity for-thylene generation from Ca_(2)MnO_(4).At 750℃and a gas hourly space velocity of 1300 h^(-1),we achieved an-thane conversion up to 68.17%,accompanied by a corresponding-thylene yield of 57.39%.X-ray photoelectron spectroscopy analysis unveiled that the doping NaNO_(3) onto Ca_(2)MnO_(4) not only played a role in reducing the oxidation state of Mn ions but also increased the lattice oxygen content of the redox catalyst.Furthermore,formation of NaNO_(3) shell on the surface of Ca_(2)MnO_(4) led to a reduction in the concentration of manganese sites and modulated the oxygen-releasing behavior in a step-wise manner.This modulation contributed significantly to the enhanced selectivity for ethylene of the NaNO_(3)-doped Ca_(2)MnO_(4) catalyst.These findings provide compelling evidence for the potential of Ca_(2)MnO_(4)-layered perovskites as promising redox catalysts in the context of CL-ODH reactions.展开更多
Thermocatalytic nonoxidative ethane dehydrogenation(EDH)is a promising strategy for ethene production but suffers from intense energy consumption and poor catalyst durability;exploring technology that permits efficien...Thermocatalytic nonoxidative ethane dehydrogenation(EDH)is a promising strategy for ethene production but suffers from intense energy consumption and poor catalyst durability;exploring technology that permits efficient EDH by solar energy remains a giant challenge.Herein,we present that an oxygen vacancy(O_v)-rich LaVO_(4)(LaVO_(4)-O_v)catalyst is highly active and stable for photocatalytic EDH,through a dynamic lattice oxygen(O_(latt.))and O_(v)co-mediated mechanism.Irradiated by simulated sunlight at mild conditions,LaVO_(4)-O_(v)effectively dehydrogenates undiluted ethane to produce C_(2)H_(4)and CO with a conversion of 2.3%.By loading a small amount of Pt cocatalyst,the evolution and selectivity of C_(2)H_(4)are enhanced to 275μmol h^(-1)g^(-1)and 96.8%.Of note,LaVO_(4)-O_(v)appears nearly no carbon deposition after the reaction.The isotope tracked reactions reveal that the consumed O_(latt.)recuperates by exposing the used catalyst with O_(2),thus establishing a dynamic cycle of O_(latt.)and achieving a facile catalyst regeneration to preserve its intrinsic activity.The refreshed LaVO_(4)-O_(v)exhibits superior reusability and delivers a turnover number of about 305.The O_(v)promotes photo absorption,boosts ethane adsorption/activation,and accelerates charge separation/transfer,thus improving the photocatalytic efficiency.The possible photocatalytic EDH mechanism is proposed,considering the key intermediates predicted by density functional theory(DFT)and monitored by in-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS).展开更多
Light alkanes non-oxidative dehydrogenation is an attractive non-oil route for olefins production.The alkane dehydrogenation reaction is limited by thermodynamic equilibrium,and the C-H bond cleavage is commonly consi...Light alkanes non-oxidative dehydrogenation is an attractive non-oil route for olefins production.The alkane dehydrogenation reaction is limited by thermodynamic equilibrium,and the C-H bond cleavage is commonly considered as the rate-determined step.The valence state of metal sites in catalysts will influence the stabilization of the vital intermediate(i.e.,C_(x)H_(y)...M^(δ+)...H)during the C-H bond cleavage process,which in turn affects the catalytic reactivity.Herein,we explicitly investigated the effect of different valence states of framework-Fe in silicate-1 zeolite on ethane dehydrogenation reaction through the combination of experimental and theoretical study.Fe(Ⅱ)-S-1 and Fe(Ⅲ)-S-1 catalysts are successfully synthesized by ligand-assisted in situ crystallization method,In-situ C_(2)H_6-FTIR shows the higher coverage of hydrocarbon intermediates on Fe(Ⅱ)-S-1,Under the same evaluation co nditio n,Fe(Ⅱ)-S-1 exhibits a higher space time yield of ethylene.Density functional theory(DFT)results reveal that the more coordinate-unsaturated and electron-enriched Fe(Ⅱ)sites boost the first C-H bond activation by slight deformation and efficient electron donation with C_(2)H_(5)^(*)species.Remarkably,the second C-H bond cleavage on Fe(Ⅱ)-S-1 undergoes a spin-crossing process from quintet state to triplet state,which involves a two-electro n-two-orbital interaction,further promoting the formation of ethylene.Microkinetic analysis is consistent with the experimental and DFT results.This work could provide methodology for elucidating the effect of metal valence states on catalytic performance as well as offer guidance for designing more efficient Fe-zeolite catalysts.展开更多
The C–H bond activation in alkane dehydrogenation reactions is a key step in determining the reaction rate.To understand the impact of entropy,we performed ab initio static and molecular dynamics free energy simulati...The C–H bond activation in alkane dehydrogenation reactions is a key step in determining the reaction rate.To understand the impact of entropy,we performed ab initio static and molecular dynamics free energy simulations of ethane dehydrogenation over Co@BEA zeolite at different temperatures.AIMD simulations showed that a sharp decrease in free energy barrier as temperature increased.Our analysis of the temperature dependence of activation free energies uncovered an unusual entropic effect accompanying the reaction.The unique spatial structures around the Co active site at different temperatures influenced both the extent of charge transfer in the transition state and the arrangement of 3d orbital energy levels.We provided explanations consistent with the principles of thermodynamics and statistical physics.The insights gained at the atomic level have offered a fresh interpretation of the intricate long-range interplay between local chemical reactions and extensive chemical environments.展开更多
Chemical looping oxidative dehydrogenation (CL-ODH) is an economically promising method for convertingethane into higher value-added ethylene utilizing lattice oxygen in redox catalysts, also known as oxygen carriers....Chemical looping oxidative dehydrogenation (CL-ODH) is an economically promising method for convertingethane into higher value-added ethylene utilizing lattice oxygen in redox catalysts, also known as oxygen carriers. Inthis study, perovskite-type oxide SrCoO_(3-δ) and B-site Mn ion-doped oxygen carriers (SrCo_(1-x)MnxO_(3-δ), x=0.1, 0.2, 0.3)were prepared and tested for the CL-ODH of ethane. The oxygen-deficient perovskite SrCoO_(3-δ) exhibited high ethyleneselectivity of up to 96.7% due to its unique oxygen vacancies and lattice oxygen migration rates. However, its low ethyleneyield limits its application in the CL-ODH of ethane. Mn doping promoted the reducibility of SrCoO_(3-δ) oxygen carriers,thereby improving ethane conversion and ethylene yield, as demonstrated by characterization and evaluation experiments.X-ray diffraction results confirmed the doping of Mn into the lattice of SrCoO_(3-δ), while X-ray photoelectron spectroscopy(XPS) indicated an increase in lattice oxygen ratio upon incorporation of Mn into the SrCoO_(3-δ) lattice. Additionally, H2temperature-programmed reduction (H2-TPR) tests revealed more peaks at lower temperature reduction zones and a declinein peak positions at higher temperatures. Among the four tested oxygen carriers, SrCo0.8Mn0.2O_(3-δ) exhibited satisfactoryperformance with an ethylene yield of 50% at 710 °C and good stability over 20 redox cycles. The synergistic effect of Mnplays a key role in increasing ethylene yields of SrCoO_(3-δ) oxygen carriers. Accordingly, SrCo0.8Mn0.2O_(3-δ) shows promisingpotential for the efficient production of ethylene from ethane via CL-ODH.展开更多
Ethane chemical looping oxidative dehydrogenation(CL-ODH)to ethylene is a new technology for converting ethane to ethylene.In the current study MeO/LaCoO_(3)(MeO=Fe_(2)O_(3),NiO or Co_(2)O_(3))composite metal oxides w...Ethane chemical looping oxidative dehydrogenation(CL-ODH)to ethylene is a new technology for converting ethane to ethylene.In the current study MeO/LaCoO_(3)(MeO=Fe_(2)O_(3),NiO or Co_(2)O_(3))composite metal oxides were prepared via citrate gel and impregnation methods,and used as oxygen carriers for CL-ODH.X-ray diffraction results indicated that all oxygen carriers had a perovskite structure even after eight redox cycles.Under a reaction temperature of 650°C,a reaction pressure of 0.1 MPa,and a weight hourly space velocity(WHSV)of 7500 mL/(g·h),ethane conversion over Co_(2)O_(3)/LaCoO_(3) reached 100%and ethylene selectivity reached 60%,both of which were better than corresponding values attained over Fe_(2)O_(3)/LaCoO_(3) and NiO/LaCoO_(3).Ethylene selectivity remained stable for 80 cycles over Co_(2)O_(3)/LaCoO_(3),then decreased gradually after 80 cycles.X-ray photoelectron spectroscopy results and evaluation results indicated that lattice oxygen and O_(2)2-had a direct relationship with ethane conversion and ethylene selectivity.Co_(2)O_(3)/LaCoO_(3) exhibited a strong capacity to release and absorb oxygen,mainly due to interaction between Co_(2)O_(3) and LaCoO_(3).展开更多
Fe-Al catalysts with hollow nano-spherical structures were synthesized following the hard template method using self-made carbon spheres as templates.The catalytic performance of these catalysts in the production of c...Fe-Al catalysts with hollow nano-spherical structures were synthesized following the hard template method using self-made carbon spheres as templates.The catalytic performance of these catalysts in the production of carbon nanotubes(CNTs)was evaluated through ethane catalytic cracking on a fixed bed reactor.Furthermore,the influence of these hollow nanospheres on the yield and quality of CNTs was investigated.The results showed that compared to the irregular-shaped catalyst synthesized by coprecipitation and the catalyst with micro-spherical structures prepared by the impregnation method,the Fe-Al hollow nano-spherical catalysts exhibited significantly enhanced specific surface area and pore volume,reaching 236 m^(2)/g and 0.77 cm^(3)/g,respectively.At a reaction temperature of 700℃ and an ethane feed rate of 90 mL/min,the CNTs yield of Fe-Al hollow nano-spherical catalyst reached as high as 48.6 gCNT/gcat,which was 1.8 and 4.6 times higher than the yield of irregular-shaped(27.7 gCNT/gcat)and micro-spherical(10.5 gCNT/gcat)catalysts,respectively.This was mainly attributed to the hollow cavity structure of Fe-Al catalyst providing sufficient space for the CNTs growth.As a result,the blockage of catalyst internal pores was prevented by the formed CNTs,which isolated ethane molecules from the active sites and lead to catalyst deactivation.Furthermore,the CNTs synthesized by Fe-Al hollow nano-spherical catalyst exhibited a uniform diameter distribution and a higher degree of graphitization.展开更多
The development of notions about the mechanism of the oxidative coupling of methane （OCM） over oxide catalysts and corresponding progress in its kinetic description are reviewed and discussed. The latter becomes ess...The development of notions about the mechanism of the oxidative coupling of methane （OCM） over oxide catalysts and corresponding progress in its kinetic description are reviewed and discussed. The latter becomes essential at the stage of scaling up and optimization of the process in pilot and industrial reactors. It is demonstrated that the main achievements in the development of kinetic models can be reached by combining the approaches conventionally used in homogeneous gas-phase kinetics and in heterogeneous catalysis. In particular, some important features of the OCM process can be described if several elementary reactions of free radical species （formation and transformation） with surface active sites are included into the detailed scheme of methane oxidation in gas. However, some important features, such as a non-additive character of the reciprocal influence of methane and ethane in the case of their simultaneous presence in the reaction mixture, cannot yet be described and comprehended in the framework of schemes developed so far. Possible ways towards an advanced kinetic model, accounting the main principles of catalyst functioning （redox nature of active sites） and pathways of product formation （via free radicals） are traced.展开更多
Boron nitride containing hydroxyl groups efficiently catalysed oxidative dehydrogenation of ethane to ethylene,offering rather high selectivity（95%） but only small amount of CO2 formation（0.4%） at a given ethane c...Boron nitride containing hydroxyl groups efficiently catalysed oxidative dehydrogenation of ethane to ethylene,offering rather high selectivity（95%） but only small amount of CO2 formation（0.4%） at a given ethane conversion of 11%.Even at high conversion level of 63%,the selectivity of ethylene retained at 80%,which is competitive with the energy-demanding industrialized steam cracking route.A long-term test for 200 h resulted in stable conversion and product selectivity,showing the excellent catalytic stability.Both experimental and computational studies have identified that the hydrogen abstraction of B-OH groups by molecular oxygen dynamically generated the active sites and triggered ethane dehydrogenation.展开更多
Gold(Au)as co-catalyst is remarkable for activating methane(CH4),especially atomically dispersed Au with maximized exposing active sites and specific electronic structure.Furthermore,singlet oxygen(^(1)O_(2))typically...Gold(Au)as co-catalyst is remarkable for activating methane(CH4),especially atomically dispersed Au with maximized exposing active sites and specific electronic structure.Furthermore,singlet oxygen(^(1)O_(2))typically manifests a mild redox capacity with a high selectivity to attack organic substrates.Peroxomonosulfate(PMS)favors to produce oxidative species 102 during the photocatalytic reactions.Thus,combining atomic Au as co-catalyst and ^(1)O_(2) as oxidant is an effective strategy to selectively convert CH4.Herein,we synthesized atomically dispersed Au on WO_(3)(Au/WO_(3)),where Au was in the forms of single atoms and clusters.At room temperature,such Au/WO_(3) exhibited enhanced photocata lytic conversion of CH4 to CH3 CH3 with a selectivity,up to 94%,under visible light.The radicals-pathway mechanism of CH4 coupling has also been investigated through detection and trapping experiment of active species.Theoretical calculations further interpret the electronic structure of Au/WO_(3) and tip-enhanced local electric field at the Au sites for promoting CH4 conversion.展开更多
A Ni-La/SiO2 catalyst was prepared through the incipient wetness impregnation method and tested in the oxidative dehydrogenation of ethane （ODHE） with CO2. The fresh and used catalysts were characterized by XRD and ...A Ni-La/SiO2 catalyst was prepared through the incipient wetness impregnation method and tested in the oxidative dehydrogenation of ethane （ODHE） with CO2. The fresh and used catalysts were characterized by XRD and SEM techniques. The Ni-La/SiO2 catalyst exhibited catalytic activity for the oxidative dehydrogenation of ethane, but with low ethylene selectivity in the absence of methane. The selectivity to ethylene increased with increasing molar ratio of methane in the feed. The carbon deposited on the catalyst surface in the sole ODHE with CO2 was mainly inert carbon, while much more filamentous carbon was formed in the presence of methane. The filamentous carbon was easy to be removed by CO2, which might play a role in improving the conversion of ethane to ethylene. The introduction of methane might affect the equilibrium of the CO2 reforming of ethane and the ODHE with CO2. As a consequence, the synthesis gas produced from CO2 reforming of methane partly inhibited the reaction of ethane and promoted the ODHE with CO2, thus increasing the selectivity of ethylene.展开更多
In this study a mathematical model of a small scale single pellet for the oxidative coupling of methane（OCM）over titanite pervoskite is developed.The method is based on a computational fluid dynamics（CFD）code whic...In this study a mathematical model of a small scale single pellet for the oxidative coupling of methane（OCM）over titanite pervoskite is developed.The method is based on a computational fluid dynamics（CFD）code which known as Fluent may be adopted to model the reactions that take place inside the porous catalyst pellet.The steady state single pellet model is coupled with a kinetic model and the intra-pellet concentration profiles of species are provided.Subsequent to achieving this goal,a nonlinear reaction network consisting of nine catalytic reactions and one gas phase reaction as an external program is successfully implemented to CFD-code as a reaction term in solving the equations.This study is based on the experimental design which is conducted in a differential reactor with a Sn/BaTiO3 catalyst（7-8 mesh） at atmospheric pressure,GHSV of 12000 h-1,ratio of methane to oxygen of 2,and three different temperatures of 1023,1048 and 1073 K.The modeling results such as selectivity and conversion at the pellet exit are in good agreement with the experimental data.Therefore,it is suggested that to achieve high yield in OCM process the modeling of the single pellet should be considered as the heart of catalytic fixed bed reactor.展开更多
Because of the ever-increasing consumption of crude oil, the role played bythe natural gas as a raw material has become more and more important in chemical industry and thepotential of methane used as a source for the...Because of the ever-increasing consumption of crude oil, the role played bythe natural gas as a raw material has become more and more important in chemical industry and thepotential of methane used as a source for the production of ethylene has attracted much attention.In this paper, the LiCl-B_2O_3/MnO_2 and Li_2SO_4-Mn_xO_y/TiO_2 catalysts for Oxidative Coupling ofMethane (OCM) have been studied, and the results show that the catalysts exhibit high activity andselectivity. Furthermore, The influence of the components in the catalyst and the reactionconditions on OCM performance has been studied and a possible active new component, cubicLi_4B_7O_(12)Cl, has been found.展开更多
Two new zinc（Ⅱ） compounds with dibenzoylmethane and N-donor ancillary ligands,[Zn（μ-pyz）（dbm）_2]_n（1） and [Zn（dbm）_2（μ-bpe）Zn（dbm）_2]（2）（Hdbm = dibenzoylmethane,pyz = pyrazine and bpe = 1,2-bis（4-...Two new zinc（Ⅱ） compounds with dibenzoylmethane and N-donor ancillary ligands,[Zn（μ-pyz）（dbm）_2]_n（1） and [Zn（dbm）_2（μ-bpe）Zn（dbm）_2]（2）（Hdbm = dibenzoylmethane,pyz = pyrazine and bpe = 1,2-bis（4-pyridyl）ethane）,have been prepared and characterized using elemental analysis,IR,~1H NMR and 13 C NMR spectroscopy,and studied by thermal gravimetric analysis as well as single-crystal X-ray diffraction. The crystal and molecular structures of 1 and 2 have been solved by X-ray diffraction and they turned out to be a one-dimensional coordination polymer with linear dispositions of metal atoms and binuclear compound,respectively. These one-dimensional polymers are further connected to form a 3D supramolecular network by C–H···O（only in 2） and π-π interactions.展开更多
Aim： To quantitatively study the histological changes of the testis and epididymis as a result of a drastic reduction of testosterone secretion. Methods： Fourteen adult Sprague-Dawley rats were injected intraperiton...Aim： To quantitatively study the histological changes of the testis and epididymis as a result of a drastic reduction of testosterone secretion. Methods： Fourteen adult Sprague-Dawley rats were injected intraperitoneally with ethane dimethane sulfonate （EDS, 75 mg/kg） and the same number of animals were injected with normal saline as a control. At days 7 and 12 （after treatment）, respectively, half of the animals from each group were killed. The testes and epididymides were removed and tissue blocks embedded in methacrylate resin. The cell number per testis was estimated using the stereological optical disector and some other parameters were obtained using other morphometric methods. Results： The EDS treatment resulted in an almost complete elimination of Leydig cells but had no effect on the numbers of Sertoli cells per testis. At day 7 after EDS treatment, many elongated spermatids were retained in the seminiferous epithelium and many round spermatids could be seen in the epididymal ducts. At day 12, a looser arrangement of spermatids and spermatocytes became evident, with apparent narrow empty spaces being formed between germ cells in an approximately radial direction towards the tubule lumen; the numbers （per testis） of non-type B spermatogonia and spermatocytes were similar to controls, whereas that of type B spermatogonia increased by 59%, and that of early round, elongating and late elongated spermatids decreased by 37%, 72% and 52%, respectively. Conclusion： The primary spermatogenic lesions following EDS administration were （i） spermiation failure and （ii） detachment of spermatids and spermatocytes associated with impairment in spermiogenesis and meiosis.展开更多
Objective This study aimed to evaluate the hepatotoxicity, metabolic disturbance activity and endocrine disrupting activity of mice treated by Decabromodiphenyl ethane （DBDPE）. Methods In this study, Balb/C mice wer...Objective This study aimed to evaluate the hepatotoxicity, metabolic disturbance activity and endocrine disrupting activity of mice treated by Decabromodiphenyl ethane （DBDPE）. Methods In this study, Balb/C mice were treated orally by gavage with various doses of DBDPE. After 30 days of treatment, mice were sacrificed; blood, livers and thyroid glands were obtained, and hepatic microsomes were isolated. Biochemical parameters including 8 clinical chemistry parameters, blood glucose and hormone levels including insulin and thyroid hormone were assayed. The effects of DBDPE on hepatic cytochrome P450 （CYP） levels and activities and uridinediphosphate-glucuronosyltransferase （UDPGT） activities were investigated. Liver and thyroid glands were observed. Results There were no obvious signs of toxicity and no significant treatment effect on body weight, or liver-to-body weight ratios between treatment groups. The levels of ALT and AST of higher dose treatment groups were markedly increased. Blood glucose levels of treatment groups were higher than those of control group. There was also an induction in TSH, T3, and f T3. UDPGT, PROD, and EROD activities were found to have been increased significantly in the high dose group. Histopathologic liver changes were characterized by hepatocyte hypertrophy and cytoplasmic vacuolization. Our findings suggest that DBDPE can cause a certain degree of mouse liver damage and insufficiency. Conclusion DBDPE has the activity of endocrine disruptors in Bal/C mice, which may induce drug-metabolizing enzymes including CYPs and UDPGT, and interfere with thyroid hormone levels mediated by Ah R and CAR signaling pathways. Endocrine disrupting activity of DBDPE could also affect the glucose metabolism homeostasis.展开更多
Separation of ethane from ethylene is a very important but challenging process in the petrochemical industry.Finding an alternative method would reduce the energy needed to make 170 million tons of ethylene manufactur...Separation of ethane from ethylene is a very important but challenging process in the petrochemical industry.Finding an alternative method would reduce the energy needed to make 170 million tons of ethylene manufactured worldwide each year.Adsorptive separation using C2H6-selective porous materials to directly produce high-purity C2H4 is more energy-efficient.We herein report the"reversed C2H6/C2H4 adsorption"in a metal–organic framework Cr-BTC via the introduction of oxygen on its open metal sites.The oxidized Cr-BTC(O2)can bind C2H6 over C2H4 through the active Cr-superoxo sites,which was elucidated by the gas sorption isotherms and density functional theory calculations.This material thus exhibits a good performance for the separation of 50/50 C2H6/C2H4 mixtures to produce 99.99%pure C2H4 in a single separation operation.展开更多
Abstract Objective To investigate the toxic effects of decabromodiphenyl ethane （DBDPE）, used as an alternative to decabromodiphenyl ether in vitro. Methods HepG2 cells were cultured in the presence of DBDPE at vari...Abstract Objective To investigate the toxic effects of decabromodiphenyl ethane （DBDPE）, used as an alternative to decabromodiphenyl ether in vitro. Methods HepG2 cells were cultured in the presence of DBDPE at various concentrations （3.125-100.0 mg/L） for 24, 48, and 72 h respectively and the toxic effect of DBDPE was studied. Results As evaluated by the 3-（4,5-dimethylthiazol-2-yl）-2,5-diphenyl tetrazolium bromide and lactate dehydrogenase assays and nuclear morphological changes, DBDPE inhibited HepG2 viability in a time- and dose-dependent manner within a range of 12.5 mg/L to 100 mg/L and for 48 h and 72 h. Induction of apoptosis was detected at 12.5-100 mg/L at 48 h and 72 h by propidium iodide staining, accompanied with overproduction of reactive oxygen species （ROS）. Furthermore, N-acetyI-L-cysteine, a widely used ROS scavenger, significantly reduced DBDPE-induced ROS levels and increased HepG2 cells viability. Conclusion DBDPE has cytotoxic and anti-proliferation effect and can induce apoptosis in which ROS plays an important role展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.52072134,52272205)Hubei Province(Nos.2021BCA149,2021CFA072,2022BAA087)the special fund for Science and Technology Innovation Teams of Shanxi Province(No.202304051001007)。
文摘Ethylene(C_(2)H_(4))is a core raw material for the petrochemical industry.It is of economic and environmental significance to use C_(2)H_(6)as the fuel and proton-conducting solid oxide fuel cells(P-SOFC)as the reactor to co-generate electricity and C_(2)H_(4).However,the large-sized Ni particles in the conventional Nicermet anode directly crack C_(2)H_(6);and oxide materials with a mild capability of breaking C-C bonds are generally limited to electrolyte-supported structures with high ohmic impedance.This research for the first time constructs an anode-supported cell using BZCY as the porous scaffold and impregnated double perovskite(PrBa)_(0.95)(Fe_(0.8)Ni_(0.2))_(1.8)Mo_(0.2)O_(6-δ)(PBFNM0.2)as the anode electrocatalysis.FeNi3 nanoparticles exsolve from PBFNM0.2 in H_(2) and uniformly distribute on the surface of perovskite substrate,acting as an active component for C_(2)H_(6)dehydrogenation and electrochemical performance enhancement.The cell with 30 wt%PBFNM0.2 impregnated anode showing a high power density of 508 and 386mW/cm^(2) with H_(2) and C_(2)H_(6)fuels,respectively;high C_(2)H_(6)conversion of 50.9%,C_(2)H_(4)selectivity of 92.1%,and C_(2)H_(4)yield of 46.9%are achieved at 750℃and 700mA/cm^(2),which outperforms all previously electrolyte-supported cells for co-generated electricity and ethylene.Moreover,the cell demonstrated excellent recoverability throughout three dehydrogenation-regeneration cycles.This work provides a practical way with broad application potential to create a novel anode-supported cell efficiently realizing the co-generation of electricity and C_(2)H_(4)from C_(2)H_(6).
基金financially supported by the National Natural Science Foundation of China(Nos.52272190 and 22178023)the National Key R&D Program of China(No.2021YFB4001401)。
文摘In response to the increasing demand of ethylene,electrochemical ethane nonoxidative dehydrogenation(EENDH)to ethylene by protonic ceramic electrolysis cells(PCECs)is developed.However,existing anode materials exhibit poor proton conductivity and limited catalytic activity.Herein,a novel Sr_(1.95)Fe_(1.4)Co_(0.1)Mo_(0.4)Zr_(0.1)O_(6-δ)(SFCMZ)anode is prepared as PCECs anode for EENDH.Zr doping increases the oxygen vacancies and enhances the proton conductivity of SFCMZ.Moreover,an alloy-oxide heterostructure(Co Fe@SFCMZ)is formed through in-situ exsolution of Co Fe alloy nanoparticles under reduction conditions,generating abundant oxygen vacancies and improving its catalytic activity.Co Fe@SFCMZ cell achieves an electrolysis current density of 0.87 A/cm^(2) at 700℃ under 1.6 V,with an ethane conversion rate of 34.22%and corresponding ethylene selectivity of 93.4%.These results demonstrate that Co Fe@SFCMZ anode exhibits excellent electrocatalytic activity,suggesting promising applications for EENDH.
基金support of National Natural Science Foundation of China(22179027)gratefully acknowledged.This work was also supported by the Natural Science Foundation of Guangxi Province(2021GXNSFAA075063,2018GXNSFDA281005)+1 种基金the National Key Research and Development Program of China(2017YFE0105500)Science&Technology Research Project of Guangdong Province(2017A020216009).
文摘Chemical-looping oxidative dehydrogenation(CL-ODH)is a process designed for the conversion of alkanes into olefins through cyclic redox reactions,eliminating the need for gaseous O_(2).In this work,we investigated the use of Ca_(2)MnO_(4)-layered perovskites modified with NaNO_(3) dopants,serving as redox catalysts(also known as oxygen carriers),for the CL-ODH of ethane within a temperature range of 700-780℃.Our findings revealed that the incorporation of NaNO_(3) as a modifier significantly-nhanced the selectivity for-thylene generation from Ca_(2)MnO_(4).At 750℃and a gas hourly space velocity of 1300 h^(-1),we achieved an-thane conversion up to 68.17%,accompanied by a corresponding-thylene yield of 57.39%.X-ray photoelectron spectroscopy analysis unveiled that the doping NaNO_(3) onto Ca_(2)MnO_(4) not only played a role in reducing the oxidation state of Mn ions but also increased the lattice oxygen content of the redox catalyst.Furthermore,formation of NaNO_(3) shell on the surface of Ca_(2)MnO_(4) led to a reduction in the concentration of manganese sites and modulated the oxygen-releasing behavior in a step-wise manner.This modulation contributed significantly to the enhanced selectivity for ethylene of the NaNO_(3)-doped Ca_(2)MnO_(4) catalyst.These findings provide compelling evidence for the potential of Ca_(2)MnO_(4)-layered perovskites as promising redox catalysts in the context of CL-ODH reactions.
基金financially supported by the National Key R&D Program of China(Nos.2021YFA1502100 and 2022YFE0114800)the National Natural Science Foundation of China(No.21973014)。
文摘Thermocatalytic nonoxidative ethane dehydrogenation(EDH)is a promising strategy for ethene production but suffers from intense energy consumption and poor catalyst durability;exploring technology that permits efficient EDH by solar energy remains a giant challenge.Herein,we present that an oxygen vacancy(O_v)-rich LaVO_(4)(LaVO_(4)-O_v)catalyst is highly active and stable for photocatalytic EDH,through a dynamic lattice oxygen(O_(latt.))and O_(v)co-mediated mechanism.Irradiated by simulated sunlight at mild conditions,LaVO_(4)-O_(v)effectively dehydrogenates undiluted ethane to produce C_(2)H_(4)and CO with a conversion of 2.3%.By loading a small amount of Pt cocatalyst,the evolution and selectivity of C_(2)H_(4)are enhanced to 275μmol h^(-1)g^(-1)and 96.8%.Of note,LaVO_(4)-O_(v)appears nearly no carbon deposition after the reaction.The isotope tracked reactions reveal that the consumed O_(latt.)recuperates by exposing the used catalyst with O_(2),thus establishing a dynamic cycle of O_(latt.)and achieving a facile catalyst regeneration to preserve its intrinsic activity.The refreshed LaVO_(4)-O_(v)exhibits superior reusability and delivers a turnover number of about 305.The O_(v)promotes photo absorption,boosts ethane adsorption/activation,and accelerates charge separation/transfer,thus improving the photocatalytic efficiency.The possible photocatalytic EDH mechanism is proposed,considering the key intermediates predicted by density functional theory(DFT)and monitored by in-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS).
基金the financial support from the National Natural Science Foundation of China (22035009,22178381)the National Key R&D Program of China (2021YFA1501301,2021YFC2901100)。
文摘Light alkanes non-oxidative dehydrogenation is an attractive non-oil route for olefins production.The alkane dehydrogenation reaction is limited by thermodynamic equilibrium,and the C-H bond cleavage is commonly considered as the rate-determined step.The valence state of metal sites in catalysts will influence the stabilization of the vital intermediate(i.e.,C_(x)H_(y)...M^(δ+)...H)during the C-H bond cleavage process,which in turn affects the catalytic reactivity.Herein,we explicitly investigated the effect of different valence states of framework-Fe in silicate-1 zeolite on ethane dehydrogenation reaction through the combination of experimental and theoretical study.Fe(Ⅱ)-S-1 and Fe(Ⅲ)-S-1 catalysts are successfully synthesized by ligand-assisted in situ crystallization method,In-situ C_(2)H_6-FTIR shows the higher coverage of hydrocarbon intermediates on Fe(Ⅱ)-S-1,Under the same evaluation co nditio n,Fe(Ⅱ)-S-1 exhibits a higher space time yield of ethylene.Density functional theory(DFT)results reveal that the more coordinate-unsaturated and electron-enriched Fe(Ⅱ)sites boost the first C-H bond activation by slight deformation and efficient electron donation with C_(2)H_(5)^(*)species.Remarkably,the second C-H bond cleavage on Fe(Ⅱ)-S-1 undergoes a spin-crossing process from quintet state to triplet state,which involves a two-electro n-two-orbital interaction,further promoting the formation of ethylene.Microkinetic analysis is consistent with the experimental and DFT results.This work could provide methodology for elucidating the effect of metal valence states on catalytic performance as well as offer guidance for designing more efficient Fe-zeolite catalysts.
文摘The C–H bond activation in alkane dehydrogenation reactions is a key step in determining the reaction rate.To understand the impact of entropy,we performed ab initio static and molecular dynamics free energy simulations of ethane dehydrogenation over Co@BEA zeolite at different temperatures.AIMD simulations showed that a sharp decrease in free energy barrier as temperature increased.Our analysis of the temperature dependence of activation free energies uncovered an unusual entropic effect accompanying the reaction.The unique spatial structures around the Co active site at different temperatures influenced both the extent of charge transfer in the transition state and the arrangement of 3d orbital energy levels.We provided explanations consistent with the principles of thermodynamics and statistical physics.The insights gained at the atomic level have offered a fresh interpretation of the intricate long-range interplay between local chemical reactions and extensive chemical environments.
基金the SINOPEC Research and Development Project(No.JR22094).
文摘Chemical looping oxidative dehydrogenation (CL-ODH) is an economically promising method for convertingethane into higher value-added ethylene utilizing lattice oxygen in redox catalysts, also known as oxygen carriers. Inthis study, perovskite-type oxide SrCoO_(3-δ) and B-site Mn ion-doped oxygen carriers (SrCo_(1-x)MnxO_(3-δ), x=0.1, 0.2, 0.3)were prepared and tested for the CL-ODH of ethane. The oxygen-deficient perovskite SrCoO_(3-δ) exhibited high ethyleneselectivity of up to 96.7% due to its unique oxygen vacancies and lattice oxygen migration rates. However, its low ethyleneyield limits its application in the CL-ODH of ethane. Mn doping promoted the reducibility of SrCoO_(3-δ) oxygen carriers,thereby improving ethane conversion and ethylene yield, as demonstrated by characterization and evaluation experiments.X-ray diffraction results confirmed the doping of Mn into the lattice of SrCoO_(3-δ), while X-ray photoelectron spectroscopy(XPS) indicated an increase in lattice oxygen ratio upon incorporation of Mn into the SrCoO_(3-δ) lattice. Additionally, H2temperature-programmed reduction (H2-TPR) tests revealed more peaks at lower temperature reduction zones and a declinein peak positions at higher temperatures. Among the four tested oxygen carriers, SrCo0.8Mn0.2O_(3-δ) exhibited satisfactoryperformance with an ethylene yield of 50% at 710 °C and good stability over 20 redox cycles. The synergistic effect of Mnplays a key role in increasing ethylene yields of SrCoO_(3-δ) oxygen carriers. Accordingly, SrCo0.8Mn0.2O_(3-δ) shows promisingpotential for the efficient production of ethylene from ethane via CL-ODH.
文摘Ethane chemical looping oxidative dehydrogenation(CL-ODH)to ethylene is a new technology for converting ethane to ethylene.In the current study MeO/LaCoO_(3)(MeO=Fe_(2)O_(3),NiO or Co_(2)O_(3))composite metal oxides were prepared via citrate gel and impregnation methods,and used as oxygen carriers for CL-ODH.X-ray diffraction results indicated that all oxygen carriers had a perovskite structure even after eight redox cycles.Under a reaction temperature of 650°C,a reaction pressure of 0.1 MPa,and a weight hourly space velocity(WHSV)of 7500 mL/(g·h),ethane conversion over Co_(2)O_(3)/LaCoO_(3) reached 100%and ethylene selectivity reached 60%,both of which were better than corresponding values attained over Fe_(2)O_(3)/LaCoO_(3) and NiO/LaCoO_(3).Ethylene selectivity remained stable for 80 cycles over Co_(2)O_(3)/LaCoO_(3),then decreased gradually after 80 cycles.X-ray photoelectron spectroscopy results and evaluation results indicated that lattice oxygen and O_(2)2-had a direct relationship with ethane conversion and ethylene selectivity.Co_(2)O_(3)/LaCoO_(3) exhibited a strong capacity to release and absorb oxygen,mainly due to interaction between Co_(2)O_(3) and LaCoO_(3).
文摘Fe-Al catalysts with hollow nano-spherical structures were synthesized following the hard template method using self-made carbon spheres as templates.The catalytic performance of these catalysts in the production of carbon nanotubes(CNTs)was evaluated through ethane catalytic cracking on a fixed bed reactor.Furthermore,the influence of these hollow nanospheres on the yield and quality of CNTs was investigated.The results showed that compared to the irregular-shaped catalyst synthesized by coprecipitation and the catalyst with micro-spherical structures prepared by the impregnation method,the Fe-Al hollow nano-spherical catalysts exhibited significantly enhanced specific surface area and pore volume,reaching 236 m^(2)/g and 0.77 cm^(3)/g,respectively.At a reaction temperature of 700℃ and an ethane feed rate of 90 mL/min,the CNTs yield of Fe-Al hollow nano-spherical catalyst reached as high as 48.6 gCNT/gcat,which was 1.8 and 4.6 times higher than the yield of irregular-shaped(27.7 gCNT/gcat)and micro-spherical(10.5 gCNT/gcat)catalysts,respectively.This was mainly attributed to the hollow cavity structure of Fe-Al catalyst providing sufficient space for the CNTs growth.As a result,the blockage of catalyst internal pores was prevented by the formed CNTs,which isolated ethane molecules from the active sites and lead to catalyst deactivation.Furthermore,the CNTs synthesized by Fe-Al hollow nano-spherical catalyst exhibited a uniform diameter distribution and a higher degree of graphitization.
文摘The development of notions about the mechanism of the oxidative coupling of methane （OCM） over oxide catalysts and corresponding progress in its kinetic description are reviewed and discussed. The latter becomes essential at the stage of scaling up and optimization of the process in pilot and industrial reactors. It is demonstrated that the main achievements in the development of kinetic models can be reached by combining the approaches conventionally used in homogeneous gas-phase kinetics and in heterogeneous catalysis. In particular, some important features of the OCM process can be described if several elementary reactions of free radical species （formation and transformation） with surface active sites are included into the detailed scheme of methane oxidation in gas. However, some important features, such as a non-additive character of the reciprocal influence of methane and ethane in the case of their simultaneous presence in the reaction mixture, cannot yet be described and comprehended in the framework of schemes developed so far. Possible ways towards an advanced kinetic model, accounting the main principles of catalyst functioning （redox nature of active sites） and pathways of product formation （via free radicals） are traced.
基金supported by the National Natural Science Foundation of China (21225312, U1462120, 21473206)Cheung Kong Scholars Programme of China (T2015036)~~
文摘Boron nitride containing hydroxyl groups efficiently catalysed oxidative dehydrogenation of ethane to ethylene,offering rather high selectivity（95%） but only small amount of CO2 formation（0.4%） at a given ethane conversion of 11%.Even at high conversion level of 63%,the selectivity of ethylene retained at 80%,which is competitive with the energy-demanding industrialized steam cracking route.A long-term test for 200 h resulted in stable conversion and product selectivity,showing the excellent catalytic stability.Both experimental and computational studies have identified that the hydrogen abstraction of B-OH groups by molecular oxygen dynamically generated the active sites and triggered ethane dehydrogenation.
基金sponsored by Shanghai Pujiang Program(No.19PJ1405200)the Startup Fund for Youngman Research at SJTU(SFYR at SJTU,No.WF220516003)。
文摘Gold(Au)as co-catalyst is remarkable for activating methane(CH4),especially atomically dispersed Au with maximized exposing active sites and specific electronic structure.Furthermore,singlet oxygen(^(1)O_(2))typically manifests a mild redox capacity with a high selectivity to attack organic substrates.Peroxomonosulfate(PMS)favors to produce oxidative species 102 during the photocatalytic reactions.Thus,combining atomic Au as co-catalyst and ^(1)O_(2) as oxidant is an effective strategy to selectively convert CH4.Herein,we synthesized atomically dispersed Au on WO_(3)(Au/WO_(3)),where Au was in the forms of single atoms and clusters.At room temperature,such Au/WO_(3) exhibited enhanced photocata lytic conversion of CH4 to CH3 CH3 with a selectivity,up to 94%,under visible light.The radicals-pathway mechanism of CH4 coupling has also been investigated through detection and trapping experiment of active species.Theoretical calculations further interpret the electronic structure of Au/WO_(3) and tip-enhanced local electric field at the Au sites for promoting CH4 conversion.
基金supported by the NNSFC (Nos. 20976109, 21021001)the Special Research Foundation of Doctoral Education of China (No.20090181110046)
文摘A Ni-La/SiO2 catalyst was prepared through the incipient wetness impregnation method and tested in the oxidative dehydrogenation of ethane （ODHE） with CO2. The fresh and used catalysts were characterized by XRD and SEM techniques. The Ni-La/SiO2 catalyst exhibited catalytic activity for the oxidative dehydrogenation of ethane, but with low ethylene selectivity in the absence of methane. The selectivity to ethylene increased with increasing molar ratio of methane in the feed. The carbon deposited on the catalyst surface in the sole ODHE with CO2 was mainly inert carbon, while much more filamentous carbon was formed in the presence of methane. The filamentous carbon was easy to be removed by CO2, which might play a role in improving the conversion of ethane to ethylene. The introduction of methane might affect the equilibrium of the CO2 reforming of ethane and the ODHE with CO2. As a consequence, the synthesis gas produced from CO2 reforming of methane partly inhibited the reaction of ethane and promoted the ODHE with CO2, thus increasing the selectivity of ethylene.
文摘In this study a mathematical model of a small scale single pellet for the oxidative coupling of methane（OCM）over titanite pervoskite is developed.The method is based on a computational fluid dynamics（CFD）code which known as Fluent may be adopted to model the reactions that take place inside the porous catalyst pellet.The steady state single pellet model is coupled with a kinetic model and the intra-pellet concentration profiles of species are provided.Subsequent to achieving this goal,a nonlinear reaction network consisting of nine catalytic reactions and one gas phase reaction as an external program is successfully implemented to CFD-code as a reaction term in solving the equations.This study is based on the experimental design which is conducted in a differential reactor with a Sn/BaTiO3 catalyst（7-8 mesh） at atmospheric pressure,GHSV of 12000 h-1,ratio of methane to oxygen of 2,and three different temperatures of 1023,1048 and 1073 K.The modeling results such as selectivity and conversion at the pellet exit are in good agreement with the experimental data.Therefore,it is suggested that to achieve high yield in OCM process the modeling of the single pellet should be considered as the heart of catalytic fixed bed reactor.
基金Project supported by the Foundation of Shanghai Science and Technology Development(No.023012007)
文摘Because of the ever-increasing consumption of crude oil, the role played bythe natural gas as a raw material has become more and more important in chemical industry and thepotential of methane used as a source for the production of ethylene has attracted much attention.In this paper, the LiCl-B_2O_3/MnO_2 and Li_2SO_4-Mn_xO_y/TiO_2 catalysts for Oxidative Coupling ofMethane (OCM) have been studied, and the results show that the catalysts exhibit high activity andselectivity. Furthermore, The influence of the components in the catalyst and the reactionconditions on OCM performance has been studied and a possible active new component, cubicLi_4B_7O_(12)Cl, has been found.
文摘Two new zinc（Ⅱ） compounds with dibenzoylmethane and N-donor ancillary ligands,[Zn（μ-pyz）（dbm）_2]_n（1） and [Zn（dbm）_2（μ-bpe）Zn（dbm）_2]（2）（Hdbm = dibenzoylmethane,pyz = pyrazine and bpe = 1,2-bis（4-pyridyl）ethane）,have been prepared and characterized using elemental analysis,IR,~1H NMR and 13 C NMR spectroscopy,and studied by thermal gravimetric analysis as well as single-crystal X-ray diffraction. The crystal and molecular structures of 1 and 2 have been solved by X-ray diffraction and they turned out to be a one-dimensional coordination polymer with linear dispositions of metal atoms and binuclear compound,respectively. These one-dimensional polymers are further connected to form a 3D supramolecular network by C–H···O（only in 2） and π-π interactions.
文摘Aim： To quantitatively study the histological changes of the testis and epididymis as a result of a drastic reduction of testosterone secretion. Methods： Fourteen adult Sprague-Dawley rats were injected intraperitoneally with ethane dimethane sulfonate （EDS, 75 mg/kg） and the same number of animals were injected with normal saline as a control. At days 7 and 12 （after treatment）, respectively, half of the animals from each group were killed. The testes and epididymides were removed and tissue blocks embedded in methacrylate resin. The cell number per testis was estimated using the stereological optical disector and some other parameters were obtained using other morphometric methods. Results： The EDS treatment resulted in an almost complete elimination of Leydig cells but had no effect on the numbers of Sertoli cells per testis. At day 7 after EDS treatment, many elongated spermatids were retained in the seminiferous epithelium and many round spermatids could be seen in the epididymal ducts. At day 12, a looser arrangement of spermatids and spermatocytes became evident, with apparent narrow empty spaces being formed between germ cells in an approximately radial direction towards the tubule lumen; the numbers （per testis） of non-type B spermatogonia and spermatocytes were similar to controls, whereas that of type B spermatogonia increased by 59%, and that of early round, elongating and late elongated spermatids decreased by 37%, 72% and 52%, respectively. Conclusion： The primary spermatogenic lesions following EDS administration were （i） spermiation failure and （ii） detachment of spermatids and spermatocytes associated with impairment in spermiogenesis and meiosis.
基金supported by the National Natural Science Foundation[No.21407179]
文摘Objective This study aimed to evaluate the hepatotoxicity, metabolic disturbance activity and endocrine disrupting activity of mice treated by Decabromodiphenyl ethane （DBDPE）. Methods In this study, Balb/C mice were treated orally by gavage with various doses of DBDPE. After 30 days of treatment, mice were sacrificed; blood, livers and thyroid glands were obtained, and hepatic microsomes were isolated. Biochemical parameters including 8 clinical chemistry parameters, blood glucose and hormone levels including insulin and thyroid hormone were assayed. The effects of DBDPE on hepatic cytochrome P450 （CYP） levels and activities and uridinediphosphate-glucuronosyltransferase （UDPGT） activities were investigated. Liver and thyroid glands were observed. Results There were no obvious signs of toxicity and no significant treatment effect on body weight, or liver-to-body weight ratios between treatment groups. The levels of ALT and AST of higher dose treatment groups were markedly increased. Blood glucose levels of treatment groups were higher than those of control group. There was also an induction in TSH, T3, and f T3. UDPGT, PROD, and EROD activities were found to have been increased significantly in the high dose group. Histopathologic liver changes were characterized by hepatocyte hypertrophy and cytoplasmic vacuolization. Our findings suggest that DBDPE can cause a certain degree of mouse liver damage and insufficiency. Conclusion DBDPE has the activity of endocrine disruptors in Bal/C mice, which may induce drug-metabolizing enzymes including CYPs and UDPGT, and interfere with thyroid hormone levels mediated by Ah R and CAR signaling pathways. Endocrine disrupting activity of DBDPE could also affect the glucose metabolism homeostasis.
基金the financial support from the National Natural Science Foundation of China(Nos.21606163 and 21878205)Coal Bed Methane Joint Foundation of Shanxi(2016012006)+2 种基金Foundation of State Key Laboratory of Coal Conversion(J18-19-610)Welch Foundation(grant AX-1730)the Distinguished Scientist Fellowship Program(DSFP)at KSU.
文摘Separation of ethane from ethylene is a very important but challenging process in the petrochemical industry.Finding an alternative method would reduce the energy needed to make 170 million tons of ethylene manufactured worldwide each year.Adsorptive separation using C2H6-selective porous materials to directly produce high-purity C2H4 is more energy-efficient.We herein report the"reversed C2H6/C2H4 adsorption"in a metal–organic framework Cr-BTC via the introduction of oxygen on its open metal sites.The oxidized Cr-BTC(O2)can bind C2H6 over C2H4 through the active Cr-superoxo sites,which was elucidated by the gas sorption isotherms and density functional theory calculations.This material thus exhibits a good performance for the separation of 50/50 C2H6/C2H4 mixtures to produce 99.99%pure C2H4 in a single separation operation.
基金supported by the NSFC(No.20877102)"973"project(No.2010CB933904)
文摘Abstract Objective To investigate the toxic effects of decabromodiphenyl ethane （DBDPE）, used as an alternative to decabromodiphenyl ether in vitro. Methods HepG2 cells were cultured in the presence of DBDPE at various concentrations （3.125-100.0 mg/L） for 24, 48, and 72 h respectively and the toxic effect of DBDPE was studied. Results As evaluated by the 3-（4,5-dimethylthiazol-2-yl）-2,5-diphenyl tetrazolium bromide and lactate dehydrogenase assays and nuclear morphological changes, DBDPE inhibited HepG2 viability in a time- and dose-dependent manner within a range of 12.5 mg/L to 100 mg/L and for 48 h and 72 h. Induction of apoptosis was detected at 12.5-100 mg/L at 48 h and 72 h by propidium iodide staining, accompanied with overproduction of reactive oxygen species （ROS）. Furthermore, N-acetyI-L-cysteine, a widely used ROS scavenger, significantly reduced DBDPE-induced ROS levels and increased HepG2 cells viability. Conclusion DBDPE has cytotoxic and anti-proliferation effect and can induce apoptosis in which ROS plays an important role
