The low temperature coal tar(CT)is taken as the raw material,and the extraction and column chromatography are used for detailed and accurate characterization in this paper.The n-heptane soluble fraction(CT-HS)and inso...The low temperature coal tar(CT)is taken as the raw material,and the extraction and column chromatography are used for detailed and accurate characterization in this paper.The n-heptane soluble fraction(CT-HS)and insoluble fraction(CT-HI)were obtained by n-heptane Soxhlet extraction.The extraction rate of CT-HS reached 92.79%(mass),which indicated that there are few heavy compounds in it.Further,different solvents(methylbenzene,benzene,ethyl acetate,methylbenzene-ethanol)were used to elute CT-HS by chromatographic column to obtain five fractions(saturates,aromatics,heteroatoms,phenolics and resins,named CT-SA,CT-AR,CT-HE,CT-PH,CT-RE,respectively).The yields of CTSA,CT-AR,CT-HE,CT-PH,CT-RE are 42.12%,10.43%,2.19%,9.50%and 6.63%(mass),respectively.Gas chromatography-mass spectrometry analysis of eluting components show that alkanes are the main components in CT,followed by polycyclic aromatics,and the corresponding fractions are CT-SA and CT-AR,respectively.The relative content of aliphatics in CT-SA is 76.93%,and the relative content of aromatics in CT-AR is 75.05%.This separation technology effectively separates and enriches different components in CT,and the activation energy required for the pyrolysis process of a single eluting fraction is lower than that of CT,which is expected to provide an important reference for the separation,analysis and conversion of complex oil products such as coal-oil co-processing products,coal tar and other complex heavy carbon oil products.展开更多
An experimental study on co-pyrolysis of bituminous coal and biomass was performed in a pressured fluidized bed reactor.The blend ratio of biomass in the mixture was varied between 0 and 100 wt%,and the temperature wa...An experimental study on co-pyrolysis of bituminous coal and biomass was performed in a pressured fluidized bed reactor.The blend ratio of biomass in the mixture was varied between 0 and 100 wt%,and the temperature was over a range of 550–650℃ under 1.0 MPa pressure with different atmospheres.On the basis of the individual pyrolysis behavior of bituminous coal and biomass,the influences of the biomass blending ratio,temperature,pressure and atmosphere on the product distribution were investigated.The results indicated that there existed a synergetic effect in the co-pyrolysis of bituminous coal and biomass in this pressured fluidized bed reactor,especially when the condition of bituminous coal and biomass blend ratio of 70:30(w/w),600℃,and 0.3 MPa was applied.The addition of biomass influenced the tar and char yields and gas and tar composition during co-pyrolysis.The tar yields were higher than the calculated values from individual pyrolysis of each fuel,and consequently the char yields were lower.The experimental results showed that the composition of the gaseous products was not in accordance with those of their individual fuel.The improvement of composition in tar also indicated synergistic effect in the co-pyrolysis.展开更多
A pilot-scale methane dehydroaromatization–H_2regeneration fluidized bed system(MDARS)was developed.In the MDARS,the catalyst circulation between a fluidized bed reactor and a fluidized bed regenerator with the help ...A pilot-scale methane dehydroaromatization–H_2regeneration fluidized bed system(MDARS)was developed.In the MDARS,the catalyst circulation between a fluidized bed reactor and a fluidized bed regenerator with the help of a catalyst feeder allowed methane dehydroaromatization(MDA)and H_2regeneration to be carried out simultaneously,which is good for maintaining a stable MDA catalytic activity.A fixed bed reactor(FB)and a single fluidized bed reactor(SFB)were also used for a comparative study.The experimental results showed that the catalytic activity in the MDARS was more stable than that in the FB and SFB reactors.The effects of some parameters of MDARS on the CH_4conversion and product selectivity were investigated.To verify the feasibility and reliability of the MDARS,an eight-hour long-term test was carried out,which demonstrated that the operation of the MDARS was stable and that the catalytic activity remained stable throughout the entire experimental period.展开更多
The catalytic cracking of coal tar asphaltene(CTA)pyrolysis vapors was carried out over transition metalion modified zeolites to promote the generation of light aromatic hydrocarbons(L-ArHs)in a pyrolysisgas chromatog...The catalytic cracking of coal tar asphaltene(CTA)pyrolysis vapors was carried out over transition metalion modified zeolites to promote the generation of light aromatic hydrocarbons(L-ArHs)in a pyrolysisgas chromatography/mass spectrometry(Py-GC/MS)micro-reactor system.The effects of ultra stable Y(USY),Co/USY and Mo/USY on the selectivity and yield of L-ArHs products and the extent of deoxygenation(Edeoxygenation),lightweight(Elightweight)from CTA pyrolysis volatiles were investigated.Results showed that the yields of L-ArHs are mainly controlled by the acid sites and specific surface area of the catalysts,while the deoxygenation effect is determined by theirs pore size.The Eligltweight of CTA pyrolysis volatiles over USY is 9.65%,while the Edeoxygenation of CTA pyrolysis volatiles over Mo/USY reaches 20.85%.Additionally,the modified zeolites(Mo/USY and Co/USY)exhibit better performance than USY on L-ArHs production,owing to the synergistic effect of metal ions(Mo,Co)and acid sites of USY.Compared with the non-catalytic fast pyrolysis of CTA,the total yield of L-ArHs obtained over USY(4032 mg·kg^(-1)),Co/USY(4363 mg·kg^(-1))and Mo/USY(4953 mg·kg^(-1))were increased by 27.03%,38.19%and 54.78%,respectively.Furthermore,the possible catalytic conversion mechanism of transition metal ion(Co and Mo)modified zeolites was proposed based on the distribution of products and the characterizations of catalysts.展开更多
A facile approach was developed for the preparation of nano-sized HZSM-5 with a hierarchical mesoporous structure by adding imidazole into conventional zeolite synthesis precursor solution. The physicochemical propert...A facile approach was developed for the preparation of nano-sized HZSM-5 with a hierarchical mesoporous structure by adding imidazole into conventional zeolite synthesis precursor solution. The physicochemical properties of modified HZSM-5 were characterized by X-ray diffraction(XRD), N_2 adsorption–desorption isotherms, scanning electron microscopy(SEM), NH_3-temperature-programmed desorption(NH_3-TPD) and pyridine adsorption infrared spectroscopy(Py-IR). The coke in spent catalysts was characterized by thermogravimetry(TG). The results showed that hierarchical HZSM-5 zeolites with excellent textural properties, such as abundant porous structure, uniform particle size and suitable acidity, could be synthesized by the recipe of one-pot synthesis routes. Moreover, the obtained HZSM-5 exhibited higher selectivity of total aromatics as well as longer lifetime in the catalytic conversion of methanol to aromatics, comparing with conventional HZSM-5. It is expected that the synthesis approach demonstrated here will be applicable to other zeolites with particular textural properties and controllable particle sizes, facilitating the emergence of new-type porous materials and their related applications in catalysis and separation.展开更多
As a potential methane efficient conversion process,non-oxidative aromatization of methane in fluidized bed requires a catalyst with good attrition resistance,especially in the states of high temperature,longtime rapi...As a potential methane efficient conversion process,non-oxidative aromatization of methane in fluidized bed requires a catalyst with good attrition resistance,especially in the states of high temperature,longtime rapid movement and chemical reaction.Existing evaluation methods for attrition resistance,such as ASTM D5757 and Jet Cup test,are targeted for fresh catalysts at ambient temperature,which cannot well reflect the real process.In this study,spherical-shaped Mo/HZSM-5 catalyst prepared by dipping and spray drying was placed in a self-made apparatus for attrition testing,in which the catalyst attrition under different system temperatures,running time and process factors was investigated with percent mass loss(PML),particle size-mass distribution(PSMD)and scanning electron microscope(SEM).Carbon deposition on the catalyst before and after activation,aromatization and regeneration was analyzed by thermogravimetry(TG),and the attrited catalysts were evaluated for methane dehydro-aromatization(MDA).The results show that the surface abrasion and body breakage of catalyst particles occur continuously,with the increase of system temperature and running time,and make the PML rise gradually.The process factors of activation,aromatization and regeneration can cause the catalyst attrition and carbon deposits,which broaden the PSMD in varying degrees,and the carbon-substances on catalysts greatly improve their attrition resistance at high temperature.Catalyst attrition has a certain influence on its catalytic performance,and the main reasons point to particle breakage and fine powder escape.展开更多
The structure and composition of coal determine its fast pyrolysis characteristics,and the study of the relationship between them can play an important role in the efficient and clean utilization of coal.So,in this wo...The structure and composition of coal determine its fast pyrolysis characteristics,and the study of the relationship between them can play an important role in the efficient and clean utilization of coal.So,in this work,hydrothermal pretreatment was used to artificially change the structure and composition of Sheng Li(SL)lignite,which was used to investigate the influence of structural changes on pyrolysis.The physicochemical structure and composition of samples were characterized by X-ray diffraction,specific surface area and porosity analyzer,solid-state 13C nuclear magnetic resonance,Fourier transform infrared spectroscopy,and elemental analyzer.Pyrolysis experiments were carried out in a powderparticle fluidized bed reactor,and the distribution and composition of the pyrolysis products were analyzed.The gasification activity of char was investigated by thermogravimetric analysis with a CO_(2) atmosphere.The results show that hydrothermal pretreatment(HTP)can destroy the cross-linking structure of SL lignite,and affect its aromaticity,pore structure,functional group,and carbon structure to change the distribution and composition of pyrolysis products of SL lignite,especially the composition of tar.Finally,the structure–activity relationship between the structure,composition,and pyrolysis characteristics of coal was comprehensively studied.展开更多
In this paper,using the computational fluid dynamics based on Euler Lagrange and the commercial software Barracuda VR,the gas-particle hydrodynamics and the erosion of particles on the inner wall and internal componen...In this paper,using the computational fluid dynamics based on Euler Lagrange and the commercial software Barracuda VR,the gas-particle hydrodynamics and the erosion of particles on the inner wall and internal components of the spouted bed in the integrated multi-jet swirling spout-fluidized bed(IMSSFB)are studied.Erosion experiments have obtained the characterization of particle erosion on internal components and verified the relevant numerical models.The results show that:the particle distribution within the IMSSFB is uneven due to the cyclonic effect of the axial swirl vane(ASV),resulting in particle erosion for the ASV being concentrated on one side;when the gas reaches the top,too high an erosion gas velocity leads to gas backflow.As the filling height increases,there is a tendency for the erosion position of the particles on the ASV to expand upwards.However,the effect of increasing gas velocity on the erosion position is insignificant.展开更多
The development of intensification technology for spouted beds has become a current research focus,and an effective way to improve the efficiency of spouted beds is to reform their structure.Although numerous studies ...The development of intensification technology for spouted beds has become a current research focus,and an effective way to improve the efficiency of spouted beds is to reform their structure.Although numerous studies have been conducted on conventional beds,there are few reviews on the comprehensive application of intensification technology for spouted beds.In this paper,we comprehensively review the role of intensification technology in spouted beds for use in hydrodynamics,drying,desulfurization,pyrolysis,coating,biomass and waste gasification,and biomass drying from the perspective of experiment and simulation.Finally,potential problems and challenges in current spouted-bed research are summarized.展开更多
CaO-based sorbent is considered to be a promising candidate for capturing CO_2 at high temperature. However,the adsorption capacity of CaO decreases sharply with the increase of the carbonation/calcination cycles. In ...CaO-based sorbent is considered to be a promising candidate for capturing CO_2 at high temperature. However,the adsorption capacity of CaO decreases sharply with the increase of the carbonation/calcination cycles. In this study, CaO was derived from calcium acetate(CaAc_2), which was doped with different elements(Mg, Al,Ce, Zr and La) to improve the cyclic stability. The carbonation conversion and cyclic stability of sorbents were tested by thermogravimetric analyzer(TGA). The sorbents were characterized by N_2 isothermal adsorption measurements, scanning electron microscopy(SEM) and X-ray diffraction(XRD). The results showed that the cyclic stabilities of all modified sorbents were improved by doping elements, while the carbonation conversions of sorbents in the 1st cycle were not increased by doping different elements. After 22 cycles, the cyclic stabilities of CaO–Al, CaO–Ce and CaO–La were above 96.2%. After 110 cycles, the cyclic stability of CaO–Al was still as high as 87.1%. Furthermore, the carbonation conversion was closely related to the critical time and specific surface area.展开更多
A new method for nitric oxide(NO)removal was developed by combining dielectric barrier discharge(DBD)and negative pulse corona(NPC).The effects of gas composition(O2,CO2,and H2 O)on NO removal were investigated with t...A new method for nitric oxide(NO)removal was developed by combining dielectric barrier discharge(DBD)and negative pulse corona(NPC).The effects of gas composition(O2,CO2,and H2 O)on NO removal were investigated with this method,and the effect of alcohols(methanol and ethanol)addition on NO removal was also investigated as well as the reaction mechanisms to enhance the NO removal efficiency.The experimental results showed that O2,CO2,and H2 O had obvious inhibition effects on NO removal,and the negative effects were in the following order:O2>CO2>H2 O.The addition of methanol or ethanol in the reaction system could mitigate the negative effects of O2,CO2 and H2 O on NO removal,and also eliminated the production of N02.The positive effect of alcohols addition with DBD-NPC denitration method was also validated in the simulated flue gas,in which the NOx(NO,NO2)was mainly converted into N2.展开更多
Nitric oxide(NO) removal and sulfur dioxide(SO_2) removal by sodium persulfate(Na_2S_2O_8) were studied in a Bubble Column Reactor. The proposed reaction pathways of NO and SO_2 removal are discussed. The effects of t...Nitric oxide(NO) removal and sulfur dioxide(SO_2) removal by sodium persulfate(Na_2S_2O_8) were studied in a Bubble Column Reactor. The proposed reaction pathways of NO and SO_2 removal are discussed. The effects of temperatures(35–90 °C), Na_2S_2O_8(0.05–0.5 mol·L^(-1)), Fe SO4(0.5–5.0 m mol·L^(-1)) and H_2O_2(0.25 mol·L^(-1))on NO and SO_2 removal were investigated. The results indicated that increased persulfate concentration led to increase in NO removal at various temperatures. SO_2 was almost completely removed in the temperature range of 55–85 °C. Fe^(2+)accelerated persulfate activation and enhanced NO removal efficiency. At 0.2 mol·L^(-1) Na_2S_2O_8 and 0.5–1.0 mmol·L^(-1) Fe^(2+), NO removal of 93.5%–99% was obtained at 75–90 °C, SO_2 removal was higher than 99% at all temperatures. The addition of 0.25 mol·L^(-1) H_2O_2 into 0.2 mol·L^(-1) Na_2S_2O_8 solution promoted NO removal efficiency apparently until utterly decomposition of H2 O2, the SO_2 removal was as high as98.4% separately at 35 °C and 80 °C.展开更多
The selective catalytic hydrogenation of naphthalene to high-value tetralin was systematically investigated.A series of Al2O3 catalysts containing different active metals(Co,Mo,Ni,W)were prepared by incipient wetness ...The selective catalytic hydrogenation of naphthalene to high-value tetralin was systematically investigated.A series of Al2O3 catalysts containing different active metals(Co,Mo,Ni,W)were prepared by incipient wetness impregnation.The effects of different active metals forms(oxidation,reduction,sulfuration)and reaction conditions on naphthalene hydrogenation were investigated and the catalysts were characterized by XRD,XPS,BET,NH3-TPD and SEM.Especially,Ni-Mo/Al2O3 was first used in this reactive system.The results show that the oxidative4%Ni O-20%MoO3/Al2O3 is the best catalyst for the preparation of tetralin.The conversion of naphthalene and the selectivity of tetralin can reach 95.62%and 99.75%respectively at 200℃,8 h and 6 MPa.Compared with reduced and sulfureted 4%Ni O-20%MoO3/Al2O3 catalysts,oxidative 4%Ni O-20%MoO3/Al2O3 has a well dispersed and uniform monolayer of the active metals,larger pore volume and size,and larger total acidity.NiO-MoO3/Al2O3 has a synergistic effect between NiO activity and MoO3 selectivity.展开更多
In the present work,the effect of pre-calcination on carbonation conversion and cyclic stability of modi fied CaObased sorbent was investigated by thermogravimetric analyzer(TGA).The modi fied CaO-based sorbents with ...In the present work,the effect of pre-calcination on carbonation conversion and cyclic stability of modi fied CaObased sorbent was investigated by thermogravimetric analyzer(TGA).The modi fied CaO-based sorbents with CaAc_2 as precursor were respectively doped with different elements(Mg,Al,Ce,Zr and La).The speci fic surface area,pore volume and pore size distribution were tested by N_2 isothermal adsorption measurements.The phase compositions of sorbents were characterized by X-ray diffraction(XRD).The results showed that the cyclic stabilities of the sorbents were improved by pre-calcination.The pre-calcination was conducted at 900°C for 5 h in air by the muf fle furnace.With pre-calcination,the cyclic stabilities of sorbents could be as high as 96% after 22 cycles,such as CaO-Al,CaO-Ce and CaO-La.After contact with air,the carbonation conversions of spent sorbents with pre-calcination suddenly increased by about one-sixth due to the change of channel structure by hydration.Both the cyclic stability of sorbent and the durability of reactivation were related to the structural stability of sample,especially the stability of mesopores between 2 nm and 5.5 nm.The present work also provided an easy and low-cost method for reactivating the spent CaO-based sorbents.展开更多
A series of ZnO-ZrO_(2) solid solutions with different Zn contents were synthesized by the urea coprecipitation method,which were coupled with H-ZSM-5 zeolite to form bifunctional catalysts.As a new benzene alkylation...A series of ZnO-ZrO_(2) solid solutions with different Zn contents were synthesized by the urea coprecipitation method,which were coupled with H-ZSM-5 zeolite to form bifunctional catalysts.As a new benzene alkylation reagent,syngas was used instead of methanol to realize the efficient conversion of syngas and benzene into toluene and xylene.A suitable ratio of ZnO-ZrO_(2) led to the significant improvement in the catalytic performance,and a suitable amount of acid helped to increase the selectivity of toluene/xylene and reduce the selectivity of the by-products ethylbenzene and C^(9+) aromatics.The highest benzene conversion of 89.2%and toluene/xylene selectivity of 88.7%were achieved over 10%ZnO-ZrO_(2)&H-ZSM-5(Si/Al=23)at a pressure of 3 MPa and a temperature of 450℃.In addition,the effect of the zeolite framework structure on product distribution was examined.Similar to the molecular dynamics of aromatic hydrocarbons,H-ZSM-5 zeolites comprise 10-membered-ring pores,which are beneficial to the activation of benzene;hence,the conversion of benzene is higher.H-ZSM-35 and HMOR zeolites exhibited small eight-membered-ring channels,which were not conducive to the passage of benzene;hence,the by-product ethylbenzene exhibits a higher selectivity.The distance between the active centers of the bifunctional catalysts was the main factor affecting the catalytic performance,and the powder mixing method was more conducive to the conversion of syngas and benzene.展开更多
To reasonably utilize the coal direct liquefaction residue(DLR), contrasting research on the co-pyrolysis between different low-rank coals and DLR was investigated using a TGA coupled with an FT-IR spectrophotometer a...To reasonably utilize the coal direct liquefaction residue(DLR), contrasting research on the co-pyrolysis between different low-rank coals and DLR was investigated using a TGA coupled with an FT-IR spectrophotometer and a fixed-bed reactor. GC–MS, FTIR, and XRD were used to explore the reaction mechanisms of the various co-pyrolysis processes. Based on the TGA results, it was confirmed that the tetrahydrofuran insoluble fraction of DLR helped to catalyze the conversion reaction of lignite. Also, the addition of DLR improved the yield of tar in the fixed-bed, with altering the composition of the tar. Moreover, a kinetic analysis during the co-pyrolysis was conducted using a distributed activation energy model. The co-pyrolysis reactions showed an approximate double-Gaussian distribution.展开更多
HZSM-5 zeolites with Si/Al ratios of 20,35,50 and 65 were prepared by the directing crystallization process of silicalite-1 seeds.The influence of Si/Al ratios on the production of benzene,toluene,xylene and naphthale...HZSM-5 zeolites with Si/Al ratios of 20,35,50 and 65 were prepared by the directing crystallization process of silicalite-1 seeds.The influence of Si/Al ratios on the production of benzene,toluene,xylene and naphthalene(BTXN)originated from asphaltenes catalytic pyrolysis was explored by adopting Py-GC/MS.Modified Z5-50 zeolites were prepared by various metal ions(Ni^(2+),Mo^(6+),Fe^(3+),and Co^(2+))with different loading rates(3%(mass),5%(mass),7%(mass),and 9%(mass))and the physical and chemical properties of these zeolites were characterized by XRD,SEM,ICP-OES,XPS,NH_(3)-TPD,FTIR,Py-IR and N_(2)adsorption-desorption isotherm.In addition,they were employed to catalyze the conversion of asphaltenes pyrolysis production to BTXN using Py-GC/MS.Results show that the highest relative content of aromatics has been obtained over HZSM-5 with Si/Al ratio of 50(Z5-50),reaching 61.87%.Besides,the loading of Ni,Mo,Fe,and Co on Z5-50 leads to an increase of acid strength and provides new active sites.The relative content of BTXN increases by 3.17%over 3Ni-Z5,which may be ascribed to that Ni promoted the conversion of polycyclic aromatic hydrocarbons(PAHs)to monocyclic aromatics due to the cracking of aliphatic side chains of PAHs and the decrease of phenolic activation energy.While under the catalysis of 5Mo-Z5,the relative content of aromatics and BTXN augmented by 5.75%and 4.02%,respectively.In addition,the highest relative content of aromatics reaches 70.09%when the loading rate of Fe was 7%(mass),and the relative content of BTXN increases from 25.87%to 29.42%.The results demonstrate that the active sites provided by different metal species expressed diverse effects on BTXN.Although the Bronsted/Lewis acid ratios of HZSM-5 modified by metal decreased,the acid strength and the relative content of BTXN both increased,which illustrated that there is a synergistic catalysis with the Bronsted acid sites and Lewis acid sites provided by metal species.In general,the performance of the catalyst is affected by the pore structure,acidity and metal active sites.Moreover,the possible formation mechanism of BTXN derived from asphaltenes catalytic pyrolysis was proposed on the basis of structural features and catalytic performances of a series of zeolites.展开更多
HFC-134a is a widely used environment-friendly refrigerant.At present,China is the largest producer of HFC-134a in the world.The production of HFC-134a in China mainly adopts the calcium carbide acetylene route.Howeve...HFC-134a is a widely used environment-friendly refrigerant.At present,China is the largest producer of HFC-134a in the world.The production of HFC-134a in China mainly adopts the calcium carbide acetylene route.However,the production route has high resource and energy consumption and large waste emission,and few of the studies addressed on the environmental performance of its production process.This study quantified the environmental performance of HFC-134a production by calcium carbide route via carrying out a life cycle assessment(LCA)using the CML 2001 method.And uncertainty analysis by Monte-Carlo simulation was also carried out.The results showed that electricity had the most impact on the environment,followed by steam,hydrogen fluoride and chlorine,and the impact of direct CO_(2) emissions in calcium carbide production stage on the global warming effect also could not be ignored.Therefore,the clean energy(e.g.,wind,solar,biomass,and natural gas)was used to replace coal-based electricity and coal-fired steam in this study,showing considerable environmental benefits.At the same time,the use of advanced production technologies could also improve environmental benefits,and the environmental impact of the global warming category could be reduced by 4.1%via using CO_(2) capture and purification technology.The Chinese database of HFC-134a production established in this study provides convenience for the relevant study of scholars.For the production of HFC-134a,this study helps to better identify the specific environmental hotspots and proposes useful ways to improve the environmental benefits.展开更多
This paper developed a new clean continuous process for the hydrogenation of 3,5-dimethylpyridine(DPY)to 3,5-dimethylpiperidine(DPI)without solvent.A series of Ru/C catalysts were prepared by impregnation method,which...This paper developed a new clean continuous process for the hydrogenation of 3,5-dimethylpyridine(DPY)to 3,5-dimethylpiperidine(DPI)without solvent.A series of Ru/C catalysts were prepared by impregnation method,which were characterized by the BET,ICP,CO chemisorptions,XRD,SEM,EDS,TEM and TG.The effect of active species,loading,catalyst support,reaction temperature and pressure on the catalytic performance was investigated.The influence of internal and external diffusion in the trickle-bed reactor(TBR)was basically eliminated by adjusting the particle size and dosage of the Ru/C catalyst.The reaction performance of the hydrogenation of DPY to DPI in the TBR and kettle reactor(KR)was compared,and the superiority of the TBR process was analyzed.The results show that this new continuous process developed in this study is an efficient way to realize the hydrogenation of DPY to DPI,and has a good industrial application prospect.展开更多
Regulable loading of Ni(OH)_(2) crystals by using three dimensionally ordered mesoporous carbon(3DOMC)as a support is achieved through a confined growth strategy accompanied by steam-assisted crystallization.Dual form...Regulable loading of Ni(OH)_(2) crystals by using three dimensionally ordered mesoporous carbon(3DOMC)as a support is achieved through a confined growth strategy accompanied by steam-assisted crystallization.Dual forms of high-crystalline nanosheet-like Ni(OH)_(2) severally distribute within mesopores or over the outer surface of 3DOMC particles depending on the loading amount(3%^(−1)5%)of Ni(OH)_(2).Benefitted from the highly hybrid combination and efficient electrolyte diffusion,the obtained Ni(OH)_(2)/carbon nanocomposites exhibit an excellent electrochemical performance,and the optimal sample of 6%_Ni(OH)_(2)/3DOMC with confined extrasmall Ni(OH)_(2) nanosheets as dominant shows the highest specific capacitance of 552.5F.g^(−1) at 1.0A⋅g^(−1),which is 330%higher than the contrast sample by using actived carbon as the support.Furthermore,the assembled hybrid supercapacitor by using 6%_Ni(OH)_(2)/3DOMC and 3DOMC as positive and negative electrodes displays an energy density of 11.7 Wh.kg^(−1) at 288.1 W.kg^(−1) and a superior charge/discharge stability.It is expected that the flexible component,well-defined structure,and superior electrochemical performance could promote a great application potential of Ni(OH)_(2)/3DOMC nanocomposites as supercapacitor electrodes and in other energy storage devices.展开更多
基金financed by the project supported by the National Natural Science Foundation of China(22078266,21908180,22178289,22278338)the Key Research and Development Program of Shaanxi(2020ZDLGY11-02,2021GY-136)the Special Fund for High-level Scholars of China(XJ21B10)。
文摘The low temperature coal tar(CT)is taken as the raw material,and the extraction and column chromatography are used for detailed and accurate characterization in this paper.The n-heptane soluble fraction(CT-HS)and insoluble fraction(CT-HI)were obtained by n-heptane Soxhlet extraction.The extraction rate of CT-HS reached 92.79%(mass),which indicated that there are few heavy compounds in it.Further,different solvents(methylbenzene,benzene,ethyl acetate,methylbenzene-ethanol)were used to elute CT-HS by chromatographic column to obtain five fractions(saturates,aromatics,heteroatoms,phenolics and resins,named CT-SA,CT-AR,CT-HE,CT-PH,CT-RE,respectively).The yields of CTSA,CT-AR,CT-HE,CT-PH,CT-RE are 42.12%,10.43%,2.19%,9.50%and 6.63%(mass),respectively.Gas chromatography-mass spectrometry analysis of eluting components show that alkanes are the main components in CT,followed by polycyclic aromatics,and the corresponding fractions are CT-SA and CT-AR,respectively.The relative content of aliphatics in CT-SA is 76.93%,and the relative content of aromatics in CT-AR is 75.05%.This separation technology effectively separates and enriches different components in CT,and the activation energy required for the pyrolysis process of a single eluting fraction is lower than that of CT,which is expected to provide an important reference for the separation,analysis and conversion of complex oil products such as coal-oil co-processing products,coal tar and other complex heavy carbon oil products.
基金Supported by Hydrocarbon High-efficiency Utilization Technology Research Center of Yanchang Petroleum(Group)Co.Ltd.,China(ycsy2013ky-A-30)
文摘An experimental study on co-pyrolysis of bituminous coal and biomass was performed in a pressured fluidized bed reactor.The blend ratio of biomass in the mixture was varied between 0 and 100 wt%,and the temperature was over a range of 550–650℃ under 1.0 MPa pressure with different atmospheres.On the basis of the individual pyrolysis behavior of bituminous coal and biomass,the influences of the biomass blending ratio,temperature,pressure and atmosphere on the product distribution were investigated.The results indicated that there existed a synergetic effect in the co-pyrolysis of bituminous coal and biomass in this pressured fluidized bed reactor,especially when the condition of bituminous coal and biomass blend ratio of 70:30(w/w),600℃,and 0.3 MPa was applied.The addition of biomass influenced the tar and char yields and gas and tar composition during co-pyrolysis.The tar yields were higher than the calculated values from individual pyrolysis of each fuel,and consequently the char yields were lower.The experimental results showed that the composition of the gaseous products was not in accordance with those of their individual fuel.The improvement of composition in tar also indicated synergistic effect in the co-pyrolysis.
基金Supported by Hydrocarbon High-efficiency Utilization Technology Research Center of Yanchang Petroleum(Group)Co.Ltd,China(Contract No.HCRC-C13-010)by the National Natural Science Foundation of China(21536009)
文摘A pilot-scale methane dehydroaromatization–H_2regeneration fluidized bed system(MDARS)was developed.In the MDARS,the catalyst circulation between a fluidized bed reactor and a fluidized bed regenerator with the help of a catalyst feeder allowed methane dehydroaromatization(MDA)and H_2regeneration to be carried out simultaneously,which is good for maintaining a stable MDA catalytic activity.A fixed bed reactor(FB)and a single fluidized bed reactor(SFB)were also used for a comparative study.The experimental results showed that the catalytic activity in the MDARS was more stable than that in the FB and SFB reactors.The effects of some parameters of MDARS on the CH_4conversion and product selectivity were investigated.To verify the feasibility and reliability of the MDARS,an eight-hour long-term test was carried out,which demonstrated that the operation of the MDARS was stable and that the catalytic activity remained stable throughout the entire experimental period.
基金financed by the projects of the National Natural Science Foundation of China(21776229,21908180,22078266)the National Key Research&Development Program of China(2018YFB0604603)the Key Research and Development Program of Shaanxi(2020ZDLGY11-02,2018ZDXM-GY-167)。
文摘The catalytic cracking of coal tar asphaltene(CTA)pyrolysis vapors was carried out over transition metalion modified zeolites to promote the generation of light aromatic hydrocarbons(L-ArHs)in a pyrolysisgas chromatography/mass spectrometry(Py-GC/MS)micro-reactor system.The effects of ultra stable Y(USY),Co/USY and Mo/USY on the selectivity and yield of L-ArHs products and the extent of deoxygenation(Edeoxygenation),lightweight(Elightweight)from CTA pyrolysis volatiles were investigated.Results showed that the yields of L-ArHs are mainly controlled by the acid sites and specific surface area of the catalysts,while the deoxygenation effect is determined by theirs pore size.The Eligltweight of CTA pyrolysis volatiles over USY is 9.65%,while the Edeoxygenation of CTA pyrolysis volatiles over Mo/USY reaches 20.85%.Additionally,the modified zeolites(Mo/USY and Co/USY)exhibit better performance than USY on L-ArHs production,owing to the synergistic effect of metal ions(Mo,Co)and acid sites of USY.Compared with the non-catalytic fast pyrolysis of CTA,the total yield of L-ArHs obtained over USY(4032 mg·kg^(-1)),Co/USY(4363 mg·kg^(-1))and Mo/USY(4953 mg·kg^(-1))were increased by 27.03%,38.19%and 54.78%,respectively.Furthermore,the possible catalytic conversion mechanism of transition metal ion(Co and Mo)modified zeolites was proposed based on the distribution of products and the characterizations of catalysts.
基金the financial support of National Natural Science Foundation of China(NO.21536009)the National High Technology Research and Development Program of China(Grant No.2011AA05A2021)Science and Technology Innovation Planning Project of Shaanxi Province,China(NO.2012KTDZ0101-04)
文摘A facile approach was developed for the preparation of nano-sized HZSM-5 with a hierarchical mesoporous structure by adding imidazole into conventional zeolite synthesis precursor solution. The physicochemical properties of modified HZSM-5 were characterized by X-ray diffraction(XRD), N_2 adsorption–desorption isotherms, scanning electron microscopy(SEM), NH_3-temperature-programmed desorption(NH_3-TPD) and pyridine adsorption infrared spectroscopy(Py-IR). The coke in spent catalysts was characterized by thermogravimetry(TG). The results showed that hierarchical HZSM-5 zeolites with excellent textural properties, such as abundant porous structure, uniform particle size and suitable acidity, could be synthesized by the recipe of one-pot synthesis routes. Moreover, the obtained HZSM-5 exhibited higher selectivity of total aromatics as well as longer lifetime in the catalytic conversion of methanol to aromatics, comparing with conventional HZSM-5. It is expected that the synthesis approach demonstrated here will be applicable to other zeolites with particular textural properties and controllable particle sizes, facilitating the emergence of new-type porous materials and their related applications in catalysis and separation.
基金supported by Hydrocarbon High-efficiency Utilization Technology Research Center of Shaanxi Yanchang Petroleum(Group)Co.,Ltd.,China(Contract No.HCRC-C13-010)the National Natural Science Foundation of China(No.21536009)。
文摘As a potential methane efficient conversion process,non-oxidative aromatization of methane in fluidized bed requires a catalyst with good attrition resistance,especially in the states of high temperature,longtime rapid movement and chemical reaction.Existing evaluation methods for attrition resistance,such as ASTM D5757 and Jet Cup test,are targeted for fresh catalysts at ambient temperature,which cannot well reflect the real process.In this study,spherical-shaped Mo/HZSM-5 catalyst prepared by dipping and spray drying was placed in a self-made apparatus for attrition testing,in which the catalyst attrition under different system temperatures,running time and process factors was investigated with percent mass loss(PML),particle size-mass distribution(PSMD)and scanning electron microscope(SEM).Carbon deposition on the catalyst before and after activation,aromatization and regeneration was analyzed by thermogravimetry(TG),and the attrited catalysts were evaluated for methane dehydro-aromatization(MDA).The results show that the surface abrasion and body breakage of catalyst particles occur continuously,with the increase of system temperature and running time,and make the PML rise gradually.The process factors of activation,aromatization and regeneration can cause the catalyst attrition and carbon deposits,which broaden the PSMD in varying degrees,and the carbon-substances on catalysts greatly improve their attrition resistance at high temperature.Catalyst attrition has a certain influence on its catalytic performance,and the main reasons point to particle breakage and fine powder escape.
基金supported by the National Natural Science Foundation of China(21536009)Science and Technology Plan Projects of Shaanxi Province(2017ZDCXL-GY-10-03)。
文摘The structure and composition of coal determine its fast pyrolysis characteristics,and the study of the relationship between them can play an important role in the efficient and clean utilization of coal.So,in this work,hydrothermal pretreatment was used to artificially change the structure and composition of Sheng Li(SL)lignite,which was used to investigate the influence of structural changes on pyrolysis.The physicochemical structure and composition of samples were characterized by X-ray diffraction,specific surface area and porosity analyzer,solid-state 13C nuclear magnetic resonance,Fourier transform infrared spectroscopy,and elemental analyzer.Pyrolysis experiments were carried out in a powderparticle fluidized bed reactor,and the distribution and composition of the pyrolysis products were analyzed.The gasification activity of char was investigated by thermogravimetric analysis with a CO_(2) atmosphere.The results show that hydrothermal pretreatment(HTP)can destroy the cross-linking structure of SL lignite,and affect its aromaticity,pore structure,functional group,and carbon structure to change the distribution and composition of pyrolysis products of SL lignite,especially the composition of tar.Finally,the structure–activity relationship between the structure,composition,and pyrolysis characteristics of coal was comprehensively studied.
基金supported by the National Natural Science Foundation of China(22178286)Shaanxi Qin Chuangyuan“scientist and engineer”team construction project(2022KXJ-041)。
文摘In this paper,using the computational fluid dynamics based on Euler Lagrange and the commercial software Barracuda VR,the gas-particle hydrodynamics and the erosion of particles on the inner wall and internal components of the spouted bed in the integrated multi-jet swirling spout-fluidized bed(IMSSFB)are studied.Erosion experiments have obtained the characterization of particle erosion on internal components and verified the relevant numerical models.The results show that:the particle distribution within the IMSSFB is uneven due to the cyclonic effect of the axial swirl vane(ASV),resulting in particle erosion for the ASV being concentrated on one side;when the gas reaches the top,too high an erosion gas velocity leads to gas backflow.As the filling height increases,there is a tendency for the erosion position of the particles on the ASV to expand upwards.However,the effect of increasing gas velocity on the erosion position is insignificant.
基金supported by the National Natural Science Foundation of China(22178286)Shaanxi Qin Chuangyuan“scientist and engineer”team construction project(2022KXJ-041).
文摘The development of intensification technology for spouted beds has become a current research focus,and an effective way to improve the efficiency of spouted beds is to reform their structure.Although numerous studies have been conducted on conventional beds,there are few reviews on the comprehensive application of intensification technology for spouted beds.In this paper,we comprehensively review the role of intensification technology in spouted beds for use in hydrodynamics,drying,desulfurization,pyrolysis,coating,biomass and waste gasification,and biomass drying from the perspective of experiment and simulation.Finally,potential problems and challenges in current spouted-bed research are summarized.
基金Supported by Capture CO_2 and Storage Technology Jointly Studied by USA and China(2013DFB60140-04)Northwest University Graduate Innovative Talent Training Project(YZZ12036)
文摘CaO-based sorbent is considered to be a promising candidate for capturing CO_2 at high temperature. However,the adsorption capacity of CaO decreases sharply with the increase of the carbonation/calcination cycles. In this study, CaO was derived from calcium acetate(CaAc_2), which was doped with different elements(Mg, Al,Ce, Zr and La) to improve the cyclic stability. The carbonation conversion and cyclic stability of sorbents were tested by thermogravimetric analyzer(TGA). The sorbents were characterized by N_2 isothermal adsorption measurements, scanning electron microscopy(SEM) and X-ray diffraction(XRD). The results showed that the cyclic stabilities of all modified sorbents were improved by doping elements, while the carbonation conversions of sorbents in the 1st cycle were not increased by doping different elements. After 22 cycles, the cyclic stabilities of CaO–Al, CaO–Ce and CaO–La were above 96.2%. After 110 cycles, the cyclic stability of CaO–Al was still as high as 87.1%. Furthermore, the carbonation conversion was closely related to the critical time and specific surface area.
基金Supported by the National Natural Science Foundation of China(21536009)the Science and Technology Plan Projects of Shaanxi Province(2017ZDCXL-GY-10-03).
文摘A new method for nitric oxide(NO)removal was developed by combining dielectric barrier discharge(DBD)and negative pulse corona(NPC).The effects of gas composition(O2,CO2,and H2 O)on NO removal were investigated with this method,and the effect of alcohols(methanol and ethanol)addition on NO removal was also investigated as well as the reaction mechanisms to enhance the NO removal efficiency.The experimental results showed that O2,CO2,and H2 O had obvious inhibition effects on NO removal,and the negative effects were in the following order:O2>CO2>H2 O.The addition of methanol or ethanol in the reaction system could mitigate the negative effects of O2,CO2 and H2 O on NO removal,and also eliminated the production of N02.The positive effect of alcohols addition with DBD-NPC denitration method was also validated in the simulated flue gas,in which the NOx(NO,NO2)was mainly converted into N2.
基金Supported by the National Natural Science Foundation of China(21536009)Science and Technology Plan Projects of Shaanxi Province(2017ZDCXL-GY-10-03)
文摘Nitric oxide(NO) removal and sulfur dioxide(SO_2) removal by sodium persulfate(Na_2S_2O_8) were studied in a Bubble Column Reactor. The proposed reaction pathways of NO and SO_2 removal are discussed. The effects of temperatures(35–90 °C), Na_2S_2O_8(0.05–0.5 mol·L^(-1)), Fe SO4(0.5–5.0 m mol·L^(-1)) and H_2O_2(0.25 mol·L^(-1))on NO and SO_2 removal were investigated. The results indicated that increased persulfate concentration led to increase in NO removal at various temperatures. SO_2 was almost completely removed in the temperature range of 55–85 °C. Fe^(2+)accelerated persulfate activation and enhanced NO removal efficiency. At 0.2 mol·L^(-1) Na_2S_2O_8 and 0.5–1.0 mmol·L^(-1) Fe^(2+), NO removal of 93.5%–99% was obtained at 75–90 °C, SO_2 removal was higher than 99% at all temperatures. The addition of 0.25 mol·L^(-1) H_2O_2 into 0.2 mol·L^(-1) Na_2S_2O_8 solution promoted NO removal efficiency apparently until utterly decomposition of H2 O2, the SO_2 removal was as high as98.4% separately at 35 °C and 80 °C.
基金supported by the Joint Funds of National Key R&D Program of China(2018YFB0604603)the National Natural Science Foundation of China(21536009,21776229)+2 种基金Science and Technology Plan Projects of Shaanxi Province(2017ZDCXL-GY-10-03,2018ZDXMGY-167)The Young Science and Technology Star Project of Shaanxi Province(2017KJXX-62)Science and Technology Program of Yulin(2018-2-22)。
文摘The selective catalytic hydrogenation of naphthalene to high-value tetralin was systematically investigated.A series of Al2O3 catalysts containing different active metals(Co,Mo,Ni,W)were prepared by incipient wetness impregnation.The effects of different active metals forms(oxidation,reduction,sulfuration)and reaction conditions on naphthalene hydrogenation were investigated and the catalysts were characterized by XRD,XPS,BET,NH3-TPD and SEM.Especially,Ni-Mo/Al2O3 was first used in this reactive system.The results show that the oxidative4%Ni O-20%MoO3/Al2O3 is the best catalyst for the preparation of tetralin.The conversion of naphthalene and the selectivity of tetralin can reach 95.62%and 99.75%respectively at 200℃,8 h and 6 MPa.Compared with reduced and sulfureted 4%Ni O-20%MoO3/Al2O3 catalysts,oxidative 4%Ni O-20%MoO3/Al2O3 has a well dispersed and uniform monolayer of the active metals,larger pore volume and size,and larger total acidity.NiO-MoO3/Al2O3 has a synergistic effect between NiO activity and MoO3 selectivity.
基金Supported by Capture CO2 and Storage Technology Jointly Studied by USA and China(2013DFB60140-04)Key Program of National Natural Science Foundation of China(No.21536009)
文摘In the present work,the effect of pre-calcination on carbonation conversion and cyclic stability of modi fied CaObased sorbent was investigated by thermogravimetric analyzer(TGA).The modi fied CaO-based sorbents with CaAc_2 as precursor were respectively doped with different elements(Mg,Al,Ce,Zr and La).The speci fic surface area,pore volume and pore size distribution were tested by N_2 isothermal adsorption measurements.The phase compositions of sorbents were characterized by X-ray diffraction(XRD).The results showed that the cyclic stabilities of the sorbents were improved by pre-calcination.The pre-calcination was conducted at 900°C for 5 h in air by the muf fle furnace.With pre-calcination,the cyclic stabilities of sorbents could be as high as 96% after 22 cycles,such as CaO-Al,CaO-Ce and CaO-La.After contact with air,the carbonation conversions of spent sorbents with pre-calcination suddenly increased by about one-sixth due to the change of channel structure by hydration.Both the cyclic stability of sorbent and the durability of reactivation were related to the structural stability of sample,especially the stability of mesopores between 2 nm and 5.5 nm.The present work also provided an easy and low-cost method for reactivating the spent CaO-based sorbents.
基金financial support from the National Key Research&Development Program of China(2018YFB0604901)the National Natural Science Foundation of China(21706210)the Key Research&Development Program of Shaanxi Province(2020ZDLGY11-06)。
文摘A series of ZnO-ZrO_(2) solid solutions with different Zn contents were synthesized by the urea coprecipitation method,which were coupled with H-ZSM-5 zeolite to form bifunctional catalysts.As a new benzene alkylation reagent,syngas was used instead of methanol to realize the efficient conversion of syngas and benzene into toluene and xylene.A suitable ratio of ZnO-ZrO_(2) led to the significant improvement in the catalytic performance,and a suitable amount of acid helped to increase the selectivity of toluene/xylene and reduce the selectivity of the by-products ethylbenzene and C^(9+) aromatics.The highest benzene conversion of 89.2%and toluene/xylene selectivity of 88.7%were achieved over 10%ZnO-ZrO_(2)&H-ZSM-5(Si/Al=23)at a pressure of 3 MPa and a temperature of 450℃.In addition,the effect of the zeolite framework structure on product distribution was examined.Similar to the molecular dynamics of aromatic hydrocarbons,H-ZSM-5 zeolites comprise 10-membered-ring pores,which are beneficial to the activation of benzene;hence,the conversion of benzene is higher.H-ZSM-35 and HMOR zeolites exhibited small eight-membered-ring channels,which were not conducive to the passage of benzene;hence,the by-product ethylbenzene exhibits a higher selectivity.The distance between the active centers of the bifunctional catalysts was the main factor affecting the catalytic performance,and the powder mixing method was more conducive to the conversion of syngas and benzene.
基金Supported by National High-tech Research and Development Program of China(2011AA05A2021)the National Natural Science Foundation of China(21536009)Science and Technology Plan Projects of Shaanxi Province(2017ZDCXL-GY-10-03).
文摘To reasonably utilize the coal direct liquefaction residue(DLR), contrasting research on the co-pyrolysis between different low-rank coals and DLR was investigated using a TGA coupled with an FT-IR spectrophotometer and a fixed-bed reactor. GC–MS, FTIR, and XRD were used to explore the reaction mechanisms of the various co-pyrolysis processes. Based on the TGA results, it was confirmed that the tetrahydrofuran insoluble fraction of DLR helped to catalyze the conversion reaction of lignite. Also, the addition of DLR improved the yield of tar in the fixed-bed, with altering the composition of the tar. Moreover, a kinetic analysis during the co-pyrolysis was conducted using a distributed activation energy model. The co-pyrolysis reactions showed an approximate double-Gaussian distribution.
基金financed by the project supported by the National Natural Science Foundation of China(21776229,21908180)National Key Research and Developent Program of China(2018YFB0604603)+2 种基金Key Research and Development Program of Shaanxi,China(2020ZDLGY11-02,2018ZDXM-GY-167)the project funded by China Postdoctoral Science Foundation(2019M653718,2020T130530)the project supported by Science and Technology Project of Yulin,China(2018-2-22)。
文摘HZSM-5 zeolites with Si/Al ratios of 20,35,50 and 65 were prepared by the directing crystallization process of silicalite-1 seeds.The influence of Si/Al ratios on the production of benzene,toluene,xylene and naphthalene(BTXN)originated from asphaltenes catalytic pyrolysis was explored by adopting Py-GC/MS.Modified Z5-50 zeolites were prepared by various metal ions(Ni^(2+),Mo^(6+),Fe^(3+),and Co^(2+))with different loading rates(3%(mass),5%(mass),7%(mass),and 9%(mass))and the physical and chemical properties of these zeolites were characterized by XRD,SEM,ICP-OES,XPS,NH_(3)-TPD,FTIR,Py-IR and N_(2)adsorption-desorption isotherm.In addition,they were employed to catalyze the conversion of asphaltenes pyrolysis production to BTXN using Py-GC/MS.Results show that the highest relative content of aromatics has been obtained over HZSM-5 with Si/Al ratio of 50(Z5-50),reaching 61.87%.Besides,the loading of Ni,Mo,Fe,and Co on Z5-50 leads to an increase of acid strength and provides new active sites.The relative content of BTXN increases by 3.17%over 3Ni-Z5,which may be ascribed to that Ni promoted the conversion of polycyclic aromatic hydrocarbons(PAHs)to monocyclic aromatics due to the cracking of aliphatic side chains of PAHs and the decrease of phenolic activation energy.While under the catalysis of 5Mo-Z5,the relative content of aromatics and BTXN augmented by 5.75%and 4.02%,respectively.In addition,the highest relative content of aromatics reaches 70.09%when the loading rate of Fe was 7%(mass),and the relative content of BTXN increases from 25.87%to 29.42%.The results demonstrate that the active sites provided by different metal species expressed diverse effects on BTXN.Although the Bronsted/Lewis acid ratios of HZSM-5 modified by metal decreased,the acid strength and the relative content of BTXN both increased,which illustrated that there is a synergistic catalysis with the Bronsted acid sites and Lewis acid sites provided by metal species.In general,the performance of the catalyst is affected by the pore structure,acidity and metal active sites.Moreover,the possible formation mechanism of BTXN derived from asphaltenes catalytic pyrolysis was proposed on the basis of structural features and catalytic performances of a series of zeolites.
基金supported by the National Natural Science Foun-dation of China(22008198)and(21536009)Science and Technol-ogy Plan Projects of Shaanxi Province,China(2017ZDCXL-GY-10-03)Industrialization Cultivation Project of Education Ministry of Shaanxi province,China(19JK0854).
文摘HFC-134a is a widely used environment-friendly refrigerant.At present,China is the largest producer of HFC-134a in the world.The production of HFC-134a in China mainly adopts the calcium carbide acetylene route.However,the production route has high resource and energy consumption and large waste emission,and few of the studies addressed on the environmental performance of its production process.This study quantified the environmental performance of HFC-134a production by calcium carbide route via carrying out a life cycle assessment(LCA)using the CML 2001 method.And uncertainty analysis by Monte-Carlo simulation was also carried out.The results showed that electricity had the most impact on the environment,followed by steam,hydrogen fluoride and chlorine,and the impact of direct CO_(2) emissions in calcium carbide production stage on the global warming effect also could not be ignored.Therefore,the clean energy(e.g.,wind,solar,biomass,and natural gas)was used to replace coal-based electricity and coal-fired steam in this study,showing considerable environmental benefits.At the same time,the use of advanced production technologies could also improve environmental benefits,and the environmental impact of the global warming category could be reduced by 4.1%via using CO_(2) capture and purification technology.The Chinese database of HFC-134a production established in this study provides convenience for the relevant study of scholars.For the production of HFC-134a,this study helps to better identify the specific environmental hotspots and proposes useful ways to improve the environmental benefits.
基金supported by the National Natural Science Foun-dation of China(21536009)the Science and Technology Plan Projects of Shaanxi Province(2017ZDCXL-GY-10-03).
文摘This paper developed a new clean continuous process for the hydrogenation of 3,5-dimethylpyridine(DPY)to 3,5-dimethylpiperidine(DPI)without solvent.A series of Ru/C catalysts were prepared by impregnation method,which were characterized by the BET,ICP,CO chemisorptions,XRD,SEM,EDS,TEM and TG.The effect of active species,loading,catalyst support,reaction temperature and pressure on the catalytic performance was investigated.The influence of internal and external diffusion in the trickle-bed reactor(TBR)was basically eliminated by adjusting the particle size and dosage of the Ru/C catalyst.The reaction performance of the hydrogenation of DPY to DPI in the TBR and kettle reactor(KR)was compared,and the superiority of the TBR process was analyzed.The results show that this new continuous process developed in this study is an efficient way to realize the hydrogenation of DPY to DPI,and has a good industrial application prospect.
基金the National Natural Science Foundation of China(Nos.21978238,21878248,and 21978055)Natural Science Foundation of Shaanxi Provincial Department of Education(No.21JY041).
文摘Regulable loading of Ni(OH)_(2) crystals by using three dimensionally ordered mesoporous carbon(3DOMC)as a support is achieved through a confined growth strategy accompanied by steam-assisted crystallization.Dual forms of high-crystalline nanosheet-like Ni(OH)_(2) severally distribute within mesopores or over the outer surface of 3DOMC particles depending on the loading amount(3%^(−1)5%)of Ni(OH)_(2).Benefitted from the highly hybrid combination and efficient electrolyte diffusion,the obtained Ni(OH)_(2)/carbon nanocomposites exhibit an excellent electrochemical performance,and the optimal sample of 6%_Ni(OH)_(2)/3DOMC with confined extrasmall Ni(OH)_(2) nanosheets as dominant shows the highest specific capacitance of 552.5F.g^(−1) at 1.0A⋅g^(−1),which is 330%higher than the contrast sample by using actived carbon as the support.Furthermore,the assembled hybrid supercapacitor by using 6%_Ni(OH)_(2)/3DOMC and 3DOMC as positive and negative electrodes displays an energy density of 11.7 Wh.kg^(−1) at 288.1 W.kg^(−1) and a superior charge/discharge stability.It is expected that the flexible component,well-defined structure,and superior electrochemical performance could promote a great application potential of Ni(OH)_(2)/3DOMC nanocomposites as supercapacitor electrodes and in other energy storage devices.
