Low desulfurization efficiency impedes the wide application of dry desulfurization technology,which is a low-cost and simple process,and one significant solution is the development and manufacture of high-performance ...Low desulfurization efficiency impedes the wide application of dry desulfurization technology,which is a low-cost and simple process,and one significant solution is the development and manufacture of high-performance desulfurizers.In this study,firstly,a steam jet mill was used to digest quicklime;then,we utilized numerical simulation to study the flow field distribution and analyze the driving factors of quicklime digestion;and lastly,the desulfurization performance of the desulfurizer was evaluated under different relative humidities.The results show that the desulfurizer prepared via the steam jet mill had better apparent activity than traditional desulfurizers.Also,the entire jet flow field of the steam jet mill is in a supersonic and highly turbulent flow state,with high crushing intensity and good particle acceleration performance.Sufficient contact with the nascent surface maximizes the formation of slaked lime.The experiments demonstrated that the operating time with 100%desulfurization efficiency and the“break-through”time for the desulfurizer prepared via the steam jet mill is longer than that of traditional desulfurizers,and has significant advantages,especially at low flue gas relative humidity.Compared with traditional desulfurizers,the desulfurizer prepared via steam jet mill expands the range of acceptable flue gas temperature,and the failure temperature is 1.625 times that of traditional desulfurizers.This work breaks through the technical bottleneck of low dry desulfurization efficiency,which is an important step in pushing forward the application of dry desulfurization.展开更多
Ce-doped nanosized ZnO desulfurizer was prepared by homogeneous precipitation,and its desulfurization efficiency at ambient temperature was investigated through dynamic experiments.The results showed that the desulfur...Ce-doped nanosized ZnO desulfurizer was prepared by homogeneous precipitation,and its desulfurization efficiency at ambient temperature was investigated through dynamic experiments.The results showed that the desulfurization activity of nanosized Ce-ZnO had improved greatly,compared to nanosized ZnO desulfurizer.Nanosized Ce-ZnO desulfurizer was characterized by XRD,TPD-MS,XPS,and TEM.The research results indicated that doping Ce decreased the particle size of the nanosized ZnO desulfurizer and ZnS was the principal desulfurization product.There were adsorption complexes of HS and S on the surface of desulfurizer as well.Only a small amount of vapor appeared in the tail gas on the condition of meeting the precision of desulfurization.展开更多
CaO-Al2O3-SiO2-CaF2-MgO was selected as the slag system for desulfurization in LF process.The reaction between steel and slag during desulfurization has been simulated by using Factsage software to study the influence...CaO-Al2O3-SiO2-CaF2-MgO was selected as the slag system for desulfurization in LF process.The reaction between steel and slag during desulfurization has been simulated by using Factsage software to study the influence of component on the sulfur distribution ratio.In order to research the influence of CaO content,aluminum powder content and its granularity on desulfurization,laboratory experiments have been carried out in a 200 kg inductive furnace.Results showed that the optimal composition of deep desulfurizer is wCaO=64% and aluminium powder 10% with a granularity of 30 μm.Industrial trials showed that the main composition range of final slag in LF process is wCaO=53.0%-57.0%,wAl2O3=23.4%-25.1%,wSiO2=8.1%-10.0%,and wCaF2=3.2%-4.7%.The sulfur mass percent in steel is lower than 0.0008% with a desulfurization rate above 89%.According to the result of industrial production,this desulfurizer could meet the production requirement for ultra-low sulfur steel,of which sulfur mass percent is under 0.0015%展开更多
In this experiment,an EG/ChCl deep eutectic solvent(DES)was synthesized using choline chloride(ChCl)and ethylene glycol(EG)as the raw materials.The synthesized DES was characterized by Fourier transform infrared spect...In this experiment,an EG/ChCl deep eutectic solvent(DES)was synthesized using choline chloride(ChCl)and ethylene glycol(EG)as the raw materials.The synthesized DES was characterized by Fourier transform infrared spectroscopy and thermogravimetric analysis.The results demonstrate the successful synthesis of DES.A certain amount of FeCl_(3) and CuSO_(4) was added to the DES to promote the absorption of H_(2)S;thus,a Fe(Ⅲ)-Cu(Ⅱ)coupled DES desulfurization system was obtained.The effects of DES raw materials’ratio,FeCl_(3) concentration,water content,CuSO_(4) concentration,and reaction temperature on the desulfurization efficiency and the regeneration conditions were studied.The results show that ChCl/EG DES with a molar ratio of 1:2 has a better desulfurization effect,and the addition of an appropriate amount of water can effectively promote the dissolution of CuSO_(4) and the absorption of H_(2)S.An appropriate increase in reaction temperature and CuSO_(4) concentration would also promote the absorption of H_(2)S.When the concentration of CuSO_(4) in DES desulfurizer was 0.15 mol/L,the gas speed was 20 mL/min,and the sulfur capacity could reach 10.23 g/L.The desulfurizer could be regenerated by passing O_(2),and the desulfurization efficiency did not change much after repeated use of desulfurization-regeneration many times.The desulfurization product was characterized by XRD as rhombohedral sulfur.展开更多
This paper has investigated a new desulfurizer for iron and steel industry to make up the lackness of magnesium-based desulfurizer.In order to explore the desulfurization process of hot metal by the new desulfurizer,b...This paper has investigated a new desulfurizer for iron and steel industry to make up the lackness of magnesium-based desulfurizer.In order to explore the desulfurization process of hot metal by the new desulfurizer,both the thermodynamics and experiments have been studied..The results of thermodynamics indicated that,under the standard condition,the lowest reaction temperatures of MgO+C and MgO+Si were 1846℃and 2132℃and the pressure of Mg vapor at the hot metal temperature were 0.2-0.5kPa and 0.005-0.01kPa,respectively.In the case of reaction between MgO and Al,the calculated starting reaction temperature under standard condition was 1475℃,and the pressure of Mg vapor was distributed from 27 kPa to 45kPa at the hot metal temperature,showing that it was easy to happen the reaction of MgO+Al.The experimental results displayed that the desulfurization efficiency was only 42.31%by the desulfurizer of MgO and C,while the effect of MgO+Al and MgO+Al-Si was good,since the desulfurization efficiencies were above 85%,and the lowest sulfur content was below 40×10-6.展开更多
The compound nano-ZnO modified with Ce was prepared by homogeneous precipitation.IR,XRD and dynamic experiments show that the crystal size of nano-ZnO desulfurizer is decreased after being modified with Ce and its des...The compound nano-ZnO modified with Ce was prepared by homogeneous precipitation.IR,XRD and dynamic experiments show that the crystal size of nano-ZnO desulfurizer is decreased after being modified with Ce and its desulfurization activities are improved greatly.When calcined at 270 ℃,Ce distributes evenly on the ZnO particle surface as amorphous state oxides,and the amorphous ZnO·H2O also exists;when the calcining temperature is 570 ℃,the crystal CeO2 separates out and the amorphous structure of zinc oxide disappears,at the same time,the crystal is perfect and its size increases,but the desulfurization activities decrease.The desulfurization product of nano-ZnO modified with Ce was analyzed with XPS.The results show that the adsorption compound of HS,S and ZnS exists on the surface of the desulfurizer.展开更多
Sulfur dioxide is one of the major pollutants resulting from fuel combustion. In this study, CaO and attapulgite were utilized as raw material for synthesizing CaO/attapulgite (CaO/ATP) desulfurizer. The physicochemic...Sulfur dioxide is one of the major pollutants resulting from fuel combustion. In this study, CaO and attapulgite were utilized as raw material for synthesizing CaO/attapulgite (CaO/ATP) desulfurizer. The physicochemical characteristics of CaO/ATP desulfurizer were evaluated by various techniques such as XRD, SEM, FT-IR. The performance of samples was studied in dynamic conditions. Major factors affecting on desulfurization such as weight ratio of CaO to total, types of modifiers, roasting time and temperature were investigated. The desulfurization agent synthesized under optimal synthesis conditions with CaO content of 30 wt% and NaOH modifier, and the desulfurization roasting time of 2 hours and roasting temperature of 600°C, exhibit sulfur tolerance of 10.15 wt%. This desulfurizer with excellent absorbency and catalysis of desulfurization, economical and?environment-friendly, could be especially useful in industrial applications.展开更多
Desulfurization of CaO–Al_(2)O_(3) particles in molten steel was observed in situ using high-temperature confocal scanning laser microscopy.The effects of the aluminum and silicon contents of molten steel on desulfur...Desulfurization of CaO–Al_(2)O_(3) particles in molten steel was observed in situ using high-temperature confocal scanning laser microscopy.The effects of the aluminum and silicon contents of molten steel on desulfurization were analyzed.When the total aluminum content in the steel increased from 6 to 1100 ppm,the CaS content in CaO–Al_(2)O_(3) particles increased from 2.1wt%to 84.84wt%after the reaction for 90 s.Furthermore,when the silicon content in the steel increased from 0.01wt%to 2.20wt%,the CaS content in CaO–Al_(2)O_(3) particles increased from 1.53wt%to 79.01wt%after the reaction for 90 s.This indicates that the increase in the aluminum and silicon contents of the steel promoted the desulfurization of CaO–Al_(2)O_(3) particles.A kinetic model was established to predict the CaO–Al_(2)O_(3) particles composition,and the diffusion coefficient of sulfur in CaO–Al_(2)O_(3) particles was 9.375×10^(−10)m^(2)·s^(−1) at 1600℃,which provided a new method for the calculation of diffusion coefficient.展开更多
In order to realize the OY Smelting Furnace disposal of solid waste,municipal waste,form a model of steel enterprises and urban integration,through the production practice of smelting furnace,analyzes the mechanism of...In order to realize the OY Smelting Furnace disposal of solid waste,municipal waste,form a model of steel enterprises and urban integration,through the production practice of smelting furnace,analyzes the mechanism of solid waste disposal,and proposed the disposal of solid waste desulfurization agent and disposal method:According to the theory to guide the actual production process,the test ton of iron with 10-15kg of desulfurizer in the production process does not affect the quality of molten iron and slag quality.展开更多
Blast furnace gas(BFG)is an important by-product energy for the iron and steel industry and has been widely used for heating or electricity generation.However,the undesirable contaminants in BFG(especially H_(2)S)gene...Blast furnace gas(BFG)is an important by-product energy for the iron and steel industry and has been widely used for heating or electricity generation.However,the undesirable contaminants in BFG(especially H_(2)S)generate harmful environmental emissions.The desulfurization of BFG is urgent for integrated steel plants due to the stringent ultra-low emission standards.Compared with other desulfurization materials,zeolite-based adsorbents represent a viable option with low costs and long service life.In this study,an ammonia-induced CuO modified 13X adsorbent(NH_(3)–CuO/13X)was prepared for H_(2)S removal from simulated BFG at low temperature.The XRD,H_(2)-TPR and TEM analysis proved that smaller CuO particles were formed and the dispersion of Cu on the surface of 13X zeolite was improved via the induction of ammonia.Evaluation on H_(2)S adsorption performance of the adsorbent was carried out using simulated BFG,and the results showed that NH_(3)–CuO/13X-3 has better breakthrough sulfur capacity,which was more than twice the sulfur capacity of CuO/13X.It is proposed that the enhanced desulfurization performance of NH_(3)–CuO/13X is attributed to an abundant pore of 13X,and combined action of 13X and CuO.This work provided an effective way to improve the sulfur capacity of zeolite-based adsorbents via impregnation method by ammonia induction.展开更多
Catalytic oxidation desulfurization(CODS)technology has shown great promise for diesel desulfurization by virtue of its low cost,mild reaction conditions,and superior desulfurization performance.Herein,a series of FeM...Catalytic oxidation desulfurization(CODS)technology has shown great promise for diesel desulfurization by virtue of its low cost,mild reaction conditions,and superior desulfurization performance.Herein,a series of FeMoO_(x)/LaTiO_(y)-z samples with diverse Fe/Mo ratios were prepared via a facile citric acid-assisted method.The impact of Fe incorporation on the dispersion and surface elemental states of Mo species,as well as oxygen species content of the synthesized FeMoO_(x)/LaTiO_(y)-z catalysts were systematically characterized using TEM,BET,UV-vis DRS,XPS,XANES,and reaction kinetics,and their CODS performances were examined for 4,6-DMDBT removal.Experimental results demonstrated that Fe/Mo ratio significantly affected the Ti−O bond strength,surface dispersion and electronic structure of Mo O_(2)species on FeMoO_(x)/LaTiO_(y)-z catalysts.FeMoO_(x)/LaTiO_(y)-2 catalyst showed outstanding cycling durability and the best CODS performance with almost 100%removal of 4,6-DMDBT from model oil within 75 min due to its proper MoO3 dispersion,optimal redox property,and the most oxygen vacancy concentration.Nevertheless,further enhancing Fe content led to the increased dispersion of Mo species,while the decrease active Mo species as well as the increase of steric effect for 4,6-DMDBT accessing to the catalytic reactive sites considerably increase the apparent activation energy of FeMoO_(x)/LaTiO_(y)-z(z>2)catalysts during the CODS process,thereby seriously suppressing their CODS performances.Moreover,Radical trapping experiments reveal that the·,generated by the activation of O_(2)at the active sites,catalytic oxidized 4,6-DMDBT to the product of 4,6-DMDBTO_(2),thereby enabling both deep desulfurization and recovery of high-value 4,6-DMDBTO_(2).These findings offer an alternative strategy to achieve ultra deep desulfurization as well as separate and recover high economic value sulfone substances from diesel.展开更多
The chemical composition of seawater affects the desulfurization of chalcopyrite in flotation.In this study,desulfurization experiments of chalcopyrite were conducted in both deionized(DI)water and seawater.The result...The chemical composition of seawater affects the desulfurization of chalcopyrite in flotation.In this study,desulfurization experiments of chalcopyrite were conducted in both deionized(DI)water and seawater.The results showed that,the copper grade of the concentrate obtained from seawater flotation decreased to 24.30%,compared to 24.60%in DI water.Concurrently,the recovery of chalcopyrite decreased from 51.39%to 38.67%,while the selectivity index(SI)also had a reduction from 2.006 to 1.798.The incorporation of ethylene diamine tetraacetic acid(EDTA),sodium silicate(SS),and sodium hexametaphosphate(SHMP)yielded an enhancement in the SI value,elevating it from 1.798 to 1.897,2.250 and 2.153,separately.It is particularly noteworthy that an excess of EDTA resulted in a SI value of merely 1.831.The mechanism of action was elucidated through analysis of surface charge measurements,X-ray photoelectron spectroscopy(XPS),Fourier transform infrared spectroscopy(FT-IR),extended Derjaguin-Landau Verwey-Overbeek(E-DLVO)theory,and density functional theory(DFT)calculations.展开更多
This study explores a hydrogen-assisted mineral phase transformation process with synergistic desulfurization for the efficient recovery of iron from the high-pressure acid leach(HPAL)tailings of laterite nickel ore.H...This study explores a hydrogen-assisted mineral phase transformation process with synergistic desulfurization for the efficient recovery of iron from the high-pressure acid leach(HPAL)tailings of laterite nickel ore.HPAL tailings containing 51.50wt%iron and 2.09wt%sulfur present environmental challenges due to their sulfur content.Pre-treatment at 950℃ for 15 min successfully reduced the sulfur content to 0.295wt%and increased the iron grade to 57.66wt%.Further hydrogen-assisted mineral phase transformation at 520℃ for 30 min,using 40vol%hydrogen and a gas flow rate of 600 mL·min^(-1),resulted in a product with an iron grade of 61.00wt%and 90.11%iron recovery.The overall desulfurization rate reached 85.83%when wet scrubbing and limestone were used to capture the sulfur.This study demonstrates the efficiency of this hydrogen-assisted process for sustainable iron recovery and sulfur removal from laterite nickel ore tailings,with potential for industrial applications.展开更多
In petroleum,mercaptan impurities generate malodorous fumes that pose risks to both human health and the environment,and leading to substandard oil quality.Lye desulfurization is a widely employed technique for elimin...In petroleum,mercaptan impurities generate malodorous fumes that pose risks to both human health and the environment,and leading to substandard oil quality.Lye desulfurization is a widely employed technique for eliminating mercaptans from oil.In traditional scrubber towers,lye and oil are poorly mixed,the desulfurization efficiency is low,and the lye consumption is high.To enhance washing efficiency,a droplet micromixer and corresponding fiber coalescence separator were developed.By optimizing the structure and operating parameters,more effective mixing and separation were achieved,and both caustic washing and desulfurization were enhanced.The proposed mixer/separator outperforms the industry standard by reducing the caustic loading by 30%and offers superior economic and engineering performances.The results of this study offer a direction for designing and optimizing a mercaptan removal unit to enhance the scrubbing effectiveness and decrease expenses to achieve more efficient and green production process.展开更多
The oxidation characteristics of sulfite and thiosulfate were examined by using thermodynamic calculations and simulated desulfurization solution experiments to investigate their difference.Subsequently,a new multista...The oxidation characteristics of sulfite and thiosulfate were examined by using thermodynamic calculations and simulated desulfurization solution experiments to investigate their difference.Subsequently,a new multistage oxidation method using oxygen−ammonium persulfate was presented and applied to the oxidation of a real desulfurization solution.The results show that the concentrations of thiosulfate and sulfite in the real desulfurization solution decrease from 48.76 and 61.76 g/L to 2.24 and 0.02 g/L,respectively,and the ammonium sulfate products obtained are white with uniform particles.In addition,compared with ammonium persulfate alone,the multistage oxidation method can reduce the ammonium persulfate addition by 37.56%and treatment cost by 28.13%.展开更多
With the acceleration of industrialization,the pollution problem of sulfur dioxide(SO_(2))emitted from coal-fired power plants has become increasingly severe.Although wet flue gas desulfurization(FGD)technology can re...With the acceleration of industrialization,the pollution problem of sulfur dioxide(SO_(2))emitted from coal-fired power plants has become increasingly severe.Although wet flue gas desulfurization(FGD)technology can remove about 95%of SO_(2),its high energy consumption and the corrosion risk of downstream equipment caused by residual SO_(2)(500–3000 ppm)still need to be addressed[1].Previous porous materials(such as MOFs)achieve selective adsorption of SO_(2) through open metal sites,M–OH sites or functional organic groups,but the problem of CO_(2) co-adsorption limits their practical application[2].In recent years,hydrogen-bonded organic frameworks(HOFs)have emerged as a research hotspot due to their reversible hydrogen-bonding networks and flexible structures[3],but their stability under extreme conditions and efficient separation performance still need to be improved[4].展开更多
Sulfuric acid slag,a common byproduct with high iron content,poses challenges due to its high levels of harmful impurities and is often discarded as solid waste,leading to significant environmental and water pollution...Sulfuric acid slag,a common byproduct with high iron content,poses challenges due to its high levels of harmful impurities and is often discarded as solid waste,leading to significant environmental and water pollution.To address this issue and improve resource utilization,the preparation process of oxidized pellets from sulfuric acid slag was studied,exploring suitable pelletizing systems and thermal parameters.Additionally,the removal of harmful elements and the consolidation mechanism were established during the oxidation roasting process.The findings revealed that sulfuric acid slag along with specific processing conditions,such as using two high-pressure grinding rolls and adding 1.25 wt.%bentonite,resulted in the production of qualified green pellets with desirable physical properties.Through a thermal treatment process involving preheating and roasting,the desulfurization rate of the pellets reached 95.55%and the removal efficiency of arsenic achieved 27.11%.Hematite recrystallizes,shrinks,and forms a reticulated structure with Fe2O3 recrystallization as the backbone,resulting in higher consolidation strength.展开更多
Designing efficient adsorbents for the deep removal of refractory dibenzothiophene(DBT)from fuel oil is vital for addressing environmental issues such as acid rain.Herein,zinc gluconate and urea-derived porous carbons...Designing efficient adsorbents for the deep removal of refractory dibenzothiophene(DBT)from fuel oil is vital for addressing environmental issues such as acid rain.Herein,zinc gluconate and urea-derived porous carbons SF-ZnNC-T(T represents the carbonization temperature)were synthesized without solvents.Through a temperature-controlled process of“melting the zinc gluconate and urea mixture,forming H-bonded polymers,and carbonizing the polymers,”the optimal carbon,SF-ZnNC-900,was obtained with a large surface area(2280 m^(2)g^(-1),highly dispersed Zn sites,and hierarchical pore structures.Consequently,SF-ZnNC-900 demonstrated significantly higher DBT adsorption capacity of43.2 mg S g^(-1),compared to just 4.3 mg S g^(-1)for the precursor.It also demonstrated good reusability,fast adsorption rate,and the ability for ultra-deep desulfurization.The superior DBT adsorption performance resulted from the evaporation of residual zinc species,which generated abundant mesopores that facilitated DBT transformation,as well as the formation of Zn-N_(x) sites that strengthened the host-vip interaction(ΔE=-1.466 e V).The solvent-free synthesized highly dispersed Zn-doped carbon shows great potential for producing sulfur-free fuel oil and for designing metal-loaded carbon adsorbents.展开更多
An in-depth understanding of the competition mechanism between olefins and different types of sulfides in gasoline is essential to improve the desulfurization selectivity of the adsorption desulfurization process(ADS)...An in-depth understanding of the competition mechanism between olefins and different types of sulfides in gasoline is essential to improve the desulfurization selectivity of the adsorption desulfurization process(ADS).In this study,the competitive adsorption and diffusion mechanism of two systems,diethyl sulfide/cyclohexene and n-butyl mercaptan/cyclohexene,with different adsorption amounts in siliceous faujasite zeolite(FAU) were investigated by Monte Carlo(MC) and molecular dynamics(MD).The systems exhibited a two-stage loading-dependent competitive adsorption and diffusion mechanism,with an inflection point of 32 molecule/UC(moleculers per microcoulomb).Before the inflection point(4-32molecule/UC),the competition mechanism of the two systems was the "optimal-displacement" mechanism.After the inflection point,the mechanism of the diethyl sulfide/cyclohexene changed to "relocation-displacement",while that of the n-butyl mercaptan/cyclohexene system changed to "dominantdisplacement".Compared to ether functional groups,the alcohol functional group has higher polarity and stronger adsorption stability,thus occupying more favorable adsorption sites within the supercages(SCs),while ethyl sulfide shifts outward to other sites within other SCs.In addition,the diffusion performance of adsorbent is related to the adsorption energy.The lower the adsorption energy,the weaker the diffusion ability.Meanwhile,the diffusion performance of adsorbates is better at high temperatures and low adsorption capacity.The effect of temperatu re on the desulfu rization selectivity was determined.A lower temperature is favorable for the adsorption capacity of the two systems and the removal selectivity of sulfides.This study provides fundamental insights into the competitive adsorption and diffusion mechanisms among sulfides,mercaptans and olefins,offering theoretical guidance for adsorbent design and reaction temperature optimization.展开更多
The development of an efficient dual-function catalytic-sorption system,which seamlessly integrates reaction and separation into a single step for extractant-free systems,represents a transformative advancement in oxi...The development of an efficient dual-function catalytic-sorption system,which seamlessly integrates reaction and separation into a single step for extractant-free systems,represents a transformative advancement in oxidative desulfurization(ODS)process.In this work,we introduce a novel dualfunction amphiphilic biochar(Mo/CBC)catalyst,functionalized with MoO_(3-x)featuring abundant oxygen vacancies,for highly effective extractant-free ODS.The polarity of the biochar was precisely tailored by varying the amount of KOH,leading to the creation of amphiphilic carriers.Subsequent ball milling facilitated the successful loading of MoO_(3-x)onto the biochar surface via an impregnation-calcination route leveraging carbon reduction,resulting in the synthesis of amphiphilic Mo/CBC catalysts.The amphiphilic nature of these catalysts ensures their stable dispersion within the oil phase,while also facilitating their interaction with the oxidant H2O2 and the adsorption of sulfur-containing oxidation products.Characterization techniques,including EPR,XPS,and in situ XRD,verified the existence of abundant oxygen vacancies obtained by carbon reduction on the amphiphilic Mo/CBC catalysts,which significantly boosted their activity in an extractant-free ODs system.Remarkably,the amphiphilic Mo/CBC catalyst displayed exceptional catalytic performance,achieving a desulfurization efficiency of 99.6%in just 10 min without extraction solvent.DFT theoretical calculations further revealed that H_(2)O_(2)readily dissociates into two OH radicals on the O_(vac)-MoO_(3),overcoming a low energy barrier.This process was identified as a key contributor to the catalyst's outstanding ODS performance.Furthermore,other biochar sources,such as rice straw,bamboo,rapeseed oil cake,and walnut oil cake,were investigated to produce Mo-based amphiphilic biochar catalysts,which all showed excellent desulfurization performance.This work establishes a versatile and highly efficient dual-function catalytic-sorption system by designing amphiphilic biochar catalysts enriched with oxygen vacancies,paving the way for the development of universally applicable ODS catalysts for industrial applications.展开更多
基金supported by the Southwest University of Science and Technology(No.22zx7168)the Sichuan Science and Technology Program(No.2020YFG0186)。
文摘Low desulfurization efficiency impedes the wide application of dry desulfurization technology,which is a low-cost and simple process,and one significant solution is the development and manufacture of high-performance desulfurizers.In this study,firstly,a steam jet mill was used to digest quicklime;then,we utilized numerical simulation to study the flow field distribution and analyze the driving factors of quicklime digestion;and lastly,the desulfurization performance of the desulfurizer was evaluated under different relative humidities.The results show that the desulfurizer prepared via the steam jet mill had better apparent activity than traditional desulfurizers.Also,the entire jet flow field of the steam jet mill is in a supersonic and highly turbulent flow state,with high crushing intensity and good particle acceleration performance.Sufficient contact with the nascent surface maximizes the formation of slaked lime.The experiments demonstrated that the operating time with 100%desulfurization efficiency and the“break-through”time for the desulfurizer prepared via the steam jet mill is longer than that of traditional desulfurizers,and has significant advantages,especially at low flue gas relative humidity.Compared with traditional desulfurizers,the desulfurizer prepared via steam jet mill expands the range of acceptable flue gas temperature,and the failure temperature is 1.625 times that of traditional desulfurizers.This work breaks through the technical bottleneck of low dry desulfurization efficiency,which is an important step in pushing forward the application of dry desulfurization.
基金Project supported by the National Natural Science Foundation of China(50478026)
文摘Ce-doped nanosized ZnO desulfurizer was prepared by homogeneous precipitation,and its desulfurization efficiency at ambient temperature was investigated through dynamic experiments.The results showed that the desulfurization activity of nanosized Ce-ZnO had improved greatly,compared to nanosized ZnO desulfurizer.Nanosized Ce-ZnO desulfurizer was characterized by XRD,TPD-MS,XPS,and TEM.The research results indicated that doping Ce decreased the particle size of the nanosized ZnO desulfurizer and ZnS was the principal desulfurization product.There were adsorption complexes of HS and S on the surface of desulfurizer as well.Only a small amount of vapor appeared in the tail gas on the condition of meeting the precision of desulfurization.
基金Sponsored by National Key Technology Research and Development Program in 11th Five-Year Plan of China(2007BAF08B01-03)
文摘CaO-Al2O3-SiO2-CaF2-MgO was selected as the slag system for desulfurization in LF process.The reaction between steel and slag during desulfurization has been simulated by using Factsage software to study the influence of component on the sulfur distribution ratio.In order to research the influence of CaO content,aluminum powder content and its granularity on desulfurization,laboratory experiments have been carried out in a 200 kg inductive furnace.Results showed that the optimal composition of deep desulfurizer is wCaO=64% and aluminium powder 10% with a granularity of 30 μm.Industrial trials showed that the main composition range of final slag in LF process is wCaO=53.0%-57.0%,wAl2O3=23.4%-25.1%,wSiO2=8.1%-10.0%,and wCaF2=3.2%-4.7%.The sulfur mass percent in steel is lower than 0.0008% with a desulfurization rate above 89%.According to the result of industrial production,this desulfurizer could meet the production requirement for ultra-low sulfur steel,of which sulfur mass percent is under 0.0015%
基金China National Science and Technology Major Project(2016ZX05017)Sinopec Group Corporation 2020 Science and Technology Project“Organic Sulfur Catalytic Hydrolysis Technology Improves Quality Research”(No.120049-1).
文摘In this experiment,an EG/ChCl deep eutectic solvent(DES)was synthesized using choline chloride(ChCl)and ethylene glycol(EG)as the raw materials.The synthesized DES was characterized by Fourier transform infrared spectroscopy and thermogravimetric analysis.The results demonstrate the successful synthesis of DES.A certain amount of FeCl_(3) and CuSO_(4) was added to the DES to promote the absorption of H_(2)S;thus,a Fe(Ⅲ)-Cu(Ⅱ)coupled DES desulfurization system was obtained.The effects of DES raw materials’ratio,FeCl_(3) concentration,water content,CuSO_(4) concentration,and reaction temperature on the desulfurization efficiency and the regeneration conditions were studied.The results show that ChCl/EG DES with a molar ratio of 1:2 has a better desulfurization effect,and the addition of an appropriate amount of water can effectively promote the dissolution of CuSO_(4) and the absorption of H_(2)S.An appropriate increase in reaction temperature and CuSO_(4) concentration would also promote the absorption of H_(2)S.When the concentration of CuSO_(4) in DES desulfurizer was 0.15 mol/L,the gas speed was 20 mL/min,and the sulfur capacity could reach 10.23 g/L.The desulfurizer could be regenerated by passing O_(2),and the desulfurization efficiency did not change much after repeated use of desulfurization-regeneration many times.The desulfurization product was characterized by XRD as rhombohedral sulfur.
基金supported by the National Natural Science Foundation of China(No.50974035)National Natural Science Foundation of China(No.51074047)+2 种基金the doctoral fund of EDU gov(20090407)China Postdoctoral Science Foundation,(20090451277)Key scientific and technological program in Liaoning Province(200921007)
文摘This paper has investigated a new desulfurizer for iron and steel industry to make up the lackness of magnesium-based desulfurizer.In order to explore the desulfurization process of hot metal by the new desulfurizer,both the thermodynamics and experiments have been studied..The results of thermodynamics indicated that,under the standard condition,the lowest reaction temperatures of MgO+C and MgO+Si were 1846℃and 2132℃and the pressure of Mg vapor at the hot metal temperature were 0.2-0.5kPa and 0.005-0.01kPa,respectively.In the case of reaction between MgO and Al,the calculated starting reaction temperature under standard condition was 1475℃,and the pressure of Mg vapor was distributed from 27 kPa to 45kPa at the hot metal temperature,showing that it was easy to happen the reaction of MgO+Al.The experimental results displayed that the desulfurization efficiency was only 42.31%by the desulfurizer of MgO and C,while the effect of MgO+Al and MgO+Al-Si was good,since the desulfurization efficiencies were above 85%,and the lowest sulfur content was below 40×10-6.
基金the National Natural Science Foundation of China(Grant No.50478026)the Science Foundation for Young Scientists of Harbin University of Science and Technology(Grant No.2008XQJZ039)
文摘The compound nano-ZnO modified with Ce was prepared by homogeneous precipitation.IR,XRD and dynamic experiments show that the crystal size of nano-ZnO desulfurizer is decreased after being modified with Ce and its desulfurization activities are improved greatly.When calcined at 270 ℃,Ce distributes evenly on the ZnO particle surface as amorphous state oxides,and the amorphous ZnO·H2O also exists;when the calcining temperature is 570 ℃,the crystal CeO2 separates out and the amorphous structure of zinc oxide disappears,at the same time,the crystal is perfect and its size increases,but the desulfurization activities decrease.The desulfurization product of nano-ZnO modified with Ce was analyzed with XPS.The results show that the adsorption compound of HS,S and ZnS exists on the surface of the desulfurizer.
文摘Sulfur dioxide is one of the major pollutants resulting from fuel combustion. In this study, CaO and attapulgite were utilized as raw material for synthesizing CaO/attapulgite (CaO/ATP) desulfurizer. The physicochemical characteristics of CaO/ATP desulfurizer were evaluated by various techniques such as XRD, SEM, FT-IR. The performance of samples was studied in dynamic conditions. Major factors affecting on desulfurization such as weight ratio of CaO to total, types of modifiers, roasting time and temperature were investigated. The desulfurization agent synthesized under optimal synthesis conditions with CaO content of 30 wt% and NaOH modifier, and the desulfurization roasting time of 2 hours and roasting temperature of 600°C, exhibit sulfur tolerance of 10.15 wt%. This desulfurizer with excellent absorbency and catalysis of desulfurization, economical and?environment-friendly, could be especially useful in industrial applications.
基金supported by the National Key R&D Program of China(No.2023YFB3709900)the National Nature Science Foundation of China(No.U22A20171)+1 种基金the China Baowu Low Carbon Metallurgy Innovation Foundation(No.BWLCF202315)the High Steel Center(HSC)at North China University of Technology and University of Science and Technology Beijing,China.
文摘Desulfurization of CaO–Al_(2)O_(3) particles in molten steel was observed in situ using high-temperature confocal scanning laser microscopy.The effects of the aluminum and silicon contents of molten steel on desulfurization were analyzed.When the total aluminum content in the steel increased from 6 to 1100 ppm,the CaS content in CaO–Al_(2)O_(3) particles increased from 2.1wt%to 84.84wt%after the reaction for 90 s.Furthermore,when the silicon content in the steel increased from 0.01wt%to 2.20wt%,the CaS content in CaO–Al_(2)O_(3) particles increased from 1.53wt%to 79.01wt%after the reaction for 90 s.This indicates that the increase in the aluminum and silicon contents of the steel promoted the desulfurization of CaO–Al_(2)O_(3) particles.A kinetic model was established to predict the CaO–Al_(2)O_(3) particles composition,and the diffusion coefficient of sulfur in CaO–Al_(2)O_(3) particles was 9.375×10^(−10)m^(2)·s^(−1) at 1600℃,which provided a new method for the calculation of diffusion coefficient.
文摘In order to realize the OY Smelting Furnace disposal of solid waste,municipal waste,form a model of steel enterprises and urban integration,through the production practice of smelting furnace,analyzes the mechanism of solid waste disposal,and proposed the disposal of solid waste desulfurization agent and disposal method:According to the theory to guide the actual production process,the test ton of iron with 10-15kg of desulfurizer in the production process does not affect the quality of molten iron and slag quality.
基金financially supported by National Natural Science Foundation of China(Grant.22076189)National Key Research and Development Program of China(No.2023YFC3707003)the Joint Fund of Yulin University and Dalian National Laboratory for Clean Energy(Grant.YLU-DNL Fund 2022003).
文摘Blast furnace gas(BFG)is an important by-product energy for the iron and steel industry and has been widely used for heating or electricity generation.However,the undesirable contaminants in BFG(especially H_(2)S)generate harmful environmental emissions.The desulfurization of BFG is urgent for integrated steel plants due to the stringent ultra-low emission standards.Compared with other desulfurization materials,zeolite-based adsorbents represent a viable option with low costs and long service life.In this study,an ammonia-induced CuO modified 13X adsorbent(NH_(3)–CuO/13X)was prepared for H_(2)S removal from simulated BFG at low temperature.The XRD,H_(2)-TPR and TEM analysis proved that smaller CuO particles were formed and the dispersion of Cu on the surface of 13X zeolite was improved via the induction of ammonia.Evaluation on H_(2)S adsorption performance of the adsorbent was carried out using simulated BFG,and the results showed that NH_(3)–CuO/13X-3 has better breakthrough sulfur capacity,which was more than twice the sulfur capacity of CuO/13X.It is proposed that the enhanced desulfurization performance of NH_(3)–CuO/13X is attributed to an abundant pore of 13X,and combined action of 13X and CuO.This work provided an effective way to improve the sulfur capacity of zeolite-based adsorbents via impregnation method by ammonia induction.
基金supported by the Natural Science Foundation of Guangdong Province(2024A1515010908,2025A1515011103)Opening Project of Hubei Key Laboratory of Plasma Chemistry and Advanced Materials(2024P11)+2 种基金Postdoctoral Fellowship Program of CPSF(GZC20233104)National Natural Science Foundation of China(22202087)Opening Project of Hubei Key Laboratory of Biomass Fibers and Eco-Dyeing&Finishing(STRZ202418)。
文摘Catalytic oxidation desulfurization(CODS)technology has shown great promise for diesel desulfurization by virtue of its low cost,mild reaction conditions,and superior desulfurization performance.Herein,a series of FeMoO_(x)/LaTiO_(y)-z samples with diverse Fe/Mo ratios were prepared via a facile citric acid-assisted method.The impact of Fe incorporation on the dispersion and surface elemental states of Mo species,as well as oxygen species content of the synthesized FeMoO_(x)/LaTiO_(y)-z catalysts were systematically characterized using TEM,BET,UV-vis DRS,XPS,XANES,and reaction kinetics,and their CODS performances were examined for 4,6-DMDBT removal.Experimental results demonstrated that Fe/Mo ratio significantly affected the Ti−O bond strength,surface dispersion and electronic structure of Mo O_(2)species on FeMoO_(x)/LaTiO_(y)-z catalysts.FeMoO_(x)/LaTiO_(y)-2 catalyst showed outstanding cycling durability and the best CODS performance with almost 100%removal of 4,6-DMDBT from model oil within 75 min due to its proper MoO3 dispersion,optimal redox property,and the most oxygen vacancy concentration.Nevertheless,further enhancing Fe content led to the increased dispersion of Mo species,while the decrease active Mo species as well as the increase of steric effect for 4,6-DMDBT accessing to the catalytic reactive sites considerably increase the apparent activation energy of FeMoO_(x)/LaTiO_(y)-z(z>2)catalysts during the CODS process,thereby seriously suppressing their CODS performances.Moreover,Radical trapping experiments reveal that the·,generated by the activation of O_(2)at the active sites,catalytic oxidized 4,6-DMDBT to the product of 4,6-DMDBTO_(2),thereby enabling both deep desulfurization and recovery of high-value 4,6-DMDBTO_(2).These findings offer an alternative strategy to achieve ultra deep desulfurization as well as separate and recover high economic value sulfone substances from diesel.
基金Project(52174239)supported by the National Natural Science Foundation of ChinaProject(2021YFC2902400)supported by the National Key R&D Program of China。
文摘The chemical composition of seawater affects the desulfurization of chalcopyrite in flotation.In this study,desulfurization experiments of chalcopyrite were conducted in both deionized(DI)water and seawater.The results showed that,the copper grade of the concentrate obtained from seawater flotation decreased to 24.30%,compared to 24.60%in DI water.Concurrently,the recovery of chalcopyrite decreased from 51.39%to 38.67%,while the selectivity index(SI)also had a reduction from 2.006 to 1.798.The incorporation of ethylene diamine tetraacetic acid(EDTA),sodium silicate(SS),and sodium hexametaphosphate(SHMP)yielded an enhancement in the SI value,elevating it from 1.798 to 1.897,2.250 and 2.153,separately.It is particularly noteworthy that an excess of EDTA resulted in a SI value of merely 1.831.The mechanism of action was elucidated through analysis of surface charge measurements,X-ray photoelectron spectroscopy(XPS),Fourier transform infrared spectroscopy(FT-IR),extended Derjaguin-Landau Verwey-Overbeek(E-DLVO)theory,and density functional theory(DFT)calculations.
基金support from the National Key Research and Development Program of China(No.2021YFC2901000)the National Natural Science Foundation of China(No.U23A20603)+1 种基金China Nonferrous Metal Mining(Group)Co.,Ltd.,Technology Research and Development Project(No.2022_2_KJJH01)the Fundamental Research Funds for the Central Universities,China(No.N25ZLV006).
文摘This study explores a hydrogen-assisted mineral phase transformation process with synergistic desulfurization for the efficient recovery of iron from the high-pressure acid leach(HPAL)tailings of laterite nickel ore.HPAL tailings containing 51.50wt%iron and 2.09wt%sulfur present environmental challenges due to their sulfur content.Pre-treatment at 950℃ for 15 min successfully reduced the sulfur content to 0.295wt%and increased the iron grade to 57.66wt%.Further hydrogen-assisted mineral phase transformation at 520℃ for 30 min,using 40vol%hydrogen and a gas flow rate of 600 mL·min^(-1),resulted in a product with an iron grade of 61.00wt%and 90.11%iron recovery.The overall desulfurization rate reached 85.83%when wet scrubbing and limestone were used to capture the sulfur.This study demonstrates the efficiency of this hydrogen-assisted process for sustainable iron recovery and sulfur removal from laterite nickel ore tailings,with potential for industrial applications.
基金supported by the National Natural Science Foundation of China(52025103)the Xplorer Prize(XPLORER-2022-1034).
文摘In petroleum,mercaptan impurities generate malodorous fumes that pose risks to both human health and the environment,and leading to substandard oil quality.Lye desulfurization is a widely employed technique for eliminating mercaptans from oil.In traditional scrubber towers,lye and oil are poorly mixed,the desulfurization efficiency is low,and the lye consumption is high.To enhance washing efficiency,a droplet micromixer and corresponding fiber coalescence separator were developed.By optimizing the structure and operating parameters,more effective mixing and separation were achieved,and both caustic washing and desulfurization were enhanced.The proposed mixer/separator outperforms the industry standard by reducing the caustic loading by 30%and offers superior economic and engineering performances.The results of this study offer a direction for designing and optimizing a mercaptan removal unit to enhance the scrubbing effectiveness and decrease expenses to achieve more efficient and green production process.
基金financial support of the Yunnan Major Scientific and Technological Project,China(No.202302AG050008)Yunnan Fundamental Research Project,China(No.202101BE070001-023)“Yunnan Revitalization Talents Support Plan”High-End Foreign Talents Program,China。
文摘The oxidation characteristics of sulfite and thiosulfate were examined by using thermodynamic calculations and simulated desulfurization solution experiments to investigate their difference.Subsequently,a new multistage oxidation method using oxygen−ammonium persulfate was presented and applied to the oxidation of a real desulfurization solution.The results show that the concentrations of thiosulfate and sulfite in the real desulfurization solution decrease from 48.76 and 61.76 g/L to 2.24 and 0.02 g/L,respectively,and the ammonium sulfate products obtained are white with uniform particles.In addition,compared with ammonium persulfate alone,the multistage oxidation method can reduce the ammonium persulfate addition by 37.56%and treatment cost by 28.13%.
基金the support of the National Natural Science Foundation of China(Nos.22205207 and 22378369).
文摘With the acceleration of industrialization,the pollution problem of sulfur dioxide(SO_(2))emitted from coal-fired power plants has become increasingly severe.Although wet flue gas desulfurization(FGD)technology can remove about 95%of SO_(2),its high energy consumption and the corrosion risk of downstream equipment caused by residual SO_(2)(500–3000 ppm)still need to be addressed[1].Previous porous materials(such as MOFs)achieve selective adsorption of SO_(2) through open metal sites,M–OH sites or functional organic groups,but the problem of CO_(2) co-adsorption limits their practical application[2].In recent years,hydrogen-bonded organic frameworks(HOFs)have emerged as a research hotspot due to their reversible hydrogen-bonding networks and flexible structures[3],but their stability under extreme conditions and efficient separation performance still need to be improved[4].
基金financially supported by the Fundamental Research Funds for the Central Universities of Central South University(2023ZZTS0506).
文摘Sulfuric acid slag,a common byproduct with high iron content,poses challenges due to its high levels of harmful impurities and is often discarded as solid waste,leading to significant environmental and water pollution.To address this issue and improve resource utilization,the preparation process of oxidized pellets from sulfuric acid slag was studied,exploring suitable pelletizing systems and thermal parameters.Additionally,the removal of harmful elements and the consolidation mechanism were established during the oxidation roasting process.The findings revealed that sulfuric acid slag along with specific processing conditions,such as using two high-pressure grinding rolls and adding 1.25 wt.%bentonite,resulted in the production of qualified green pellets with desirable physical properties.Through a thermal treatment process involving preheating and roasting,the desulfurization rate of the pellets reached 95.55%and the removal efficiency of arsenic achieved 27.11%.Hematite recrystallizes,shrinks,and forms a reticulated structure with Fe2O3 recrystallization as the backbone,resulting in higher consolidation strength.
基金supported by the National Natural Science Foundation of China(Grant No.22378065,22278077,22278076)。
文摘Designing efficient adsorbents for the deep removal of refractory dibenzothiophene(DBT)from fuel oil is vital for addressing environmental issues such as acid rain.Herein,zinc gluconate and urea-derived porous carbons SF-ZnNC-T(T represents the carbonization temperature)were synthesized without solvents.Through a temperature-controlled process of“melting the zinc gluconate and urea mixture,forming H-bonded polymers,and carbonizing the polymers,”the optimal carbon,SF-ZnNC-900,was obtained with a large surface area(2280 m^(2)g^(-1),highly dispersed Zn sites,and hierarchical pore structures.Consequently,SF-ZnNC-900 demonstrated significantly higher DBT adsorption capacity of43.2 mg S g^(-1),compared to just 4.3 mg S g^(-1)for the precursor.It also demonstrated good reusability,fast adsorption rate,and the ability for ultra-deep desulfurization.The superior DBT adsorption performance resulted from the evaporation of residual zinc species,which generated abundant mesopores that facilitated DBT transformation,as well as the formation of Zn-N_(x) sites that strengthened the host-vip interaction(ΔE=-1.466 e V).The solvent-free synthesized highly dispersed Zn-doped carbon shows great potential for producing sulfur-free fuel oil and for designing metal-loaded carbon adsorbents.
基金support from the National Natural Science Foundation of China (22325808,U22B20140,22021004)。
文摘An in-depth understanding of the competition mechanism between olefins and different types of sulfides in gasoline is essential to improve the desulfurization selectivity of the adsorption desulfurization process(ADS).In this study,the competitive adsorption and diffusion mechanism of two systems,diethyl sulfide/cyclohexene and n-butyl mercaptan/cyclohexene,with different adsorption amounts in siliceous faujasite zeolite(FAU) were investigated by Monte Carlo(MC) and molecular dynamics(MD).The systems exhibited a two-stage loading-dependent competitive adsorption and diffusion mechanism,with an inflection point of 32 molecule/UC(moleculers per microcoulomb).Before the inflection point(4-32molecule/UC),the competition mechanism of the two systems was the "optimal-displacement" mechanism.After the inflection point,the mechanism of the diethyl sulfide/cyclohexene changed to "relocation-displacement",while that of the n-butyl mercaptan/cyclohexene system changed to "dominantdisplacement".Compared to ether functional groups,the alcohol functional group has higher polarity and stronger adsorption stability,thus occupying more favorable adsorption sites within the supercages(SCs),while ethyl sulfide shifts outward to other sites within other SCs.In addition,the diffusion performance of adsorbent is related to the adsorption energy.The lower the adsorption energy,the weaker the diffusion ability.Meanwhile,the diffusion performance of adsorbates is better at high temperatures and low adsorption capacity.The effect of temperatu re on the desulfu rization selectivity was determined.A lower temperature is favorable for the adsorption capacity of the two systems and the removal selectivity of sulfides.This study provides fundamental insights into the competitive adsorption and diffusion mechanisms among sulfides,mercaptans and olefins,offering theoretical guidance for adsorbent design and reaction temperature optimization.
基金supported by the National Natural Science Foundation of China(22162008)the Science and Technology Supporting Project of Guizhou Province([2022]208)+1 种基金the Guizhou Province Local Government Overseas Study Programthe open project of Guizhou Provincial Double Carbon and Renewable Energy Technology Innovation Research Institute.
文摘The development of an efficient dual-function catalytic-sorption system,which seamlessly integrates reaction and separation into a single step for extractant-free systems,represents a transformative advancement in oxidative desulfurization(ODS)process.In this work,we introduce a novel dualfunction amphiphilic biochar(Mo/CBC)catalyst,functionalized with MoO_(3-x)featuring abundant oxygen vacancies,for highly effective extractant-free ODS.The polarity of the biochar was precisely tailored by varying the amount of KOH,leading to the creation of amphiphilic carriers.Subsequent ball milling facilitated the successful loading of MoO_(3-x)onto the biochar surface via an impregnation-calcination route leveraging carbon reduction,resulting in the synthesis of amphiphilic Mo/CBC catalysts.The amphiphilic nature of these catalysts ensures their stable dispersion within the oil phase,while also facilitating their interaction with the oxidant H2O2 and the adsorption of sulfur-containing oxidation products.Characterization techniques,including EPR,XPS,and in situ XRD,verified the existence of abundant oxygen vacancies obtained by carbon reduction on the amphiphilic Mo/CBC catalysts,which significantly boosted their activity in an extractant-free ODs system.Remarkably,the amphiphilic Mo/CBC catalyst displayed exceptional catalytic performance,achieving a desulfurization efficiency of 99.6%in just 10 min without extraction solvent.DFT theoretical calculations further revealed that H_(2)O_(2)readily dissociates into two OH radicals on the O_(vac)-MoO_(3),overcoming a low energy barrier.This process was identified as a key contributor to the catalyst's outstanding ODS performance.Furthermore,other biochar sources,such as rice straw,bamboo,rapeseed oil cake,and walnut oil cake,were investigated to produce Mo-based amphiphilic biochar catalysts,which all showed excellent desulfurization performance.This work establishes a versatile and highly efficient dual-function catalytic-sorption system by designing amphiphilic biochar catalysts enriched with oxygen vacancies,paving the way for the development of universally applicable ODS catalysts for industrial applications.
