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
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
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
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
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
An efficient mass transfer process is a critical factor for regulating catalytic activity in a photocatalytic desulfurization system.Herein,a phosphotungstic acid(HPW)active center is successfully composited with a qu...An efficient mass transfer process is a critical factor for regulating catalytic activity in a photocatalytic desulfurization system.Herein,a phosphotungstic acid(HPW)active center is successfully composited with a quaternary ammonium phosphotungstate-based hexadecyltrimethylammonium chloride ionic liquid(CTAC-HPW)by the ion exchange method for the photocatalytic oxidative desulfurization of dibenzothiophene sulfide.The keggin structure of HPW and highly mass transfer performance of organic cations synergistically enhanced the photocatalytic activity towards the effective convertion of dibenzothiophene(DBT)with the excitation of visible light.The deep desulfurization(<10 mg·kg^(-1))is attained within 30 min,and well stability is demonstrated within 25 cycles.Moreover,the CTAC-HPW photocatalyst projects well selectivity to interference from coexisting compounds such as olefins and aromatic hydrocarbons and universality of dibenzothiophenes,for example,4-methyldibenzothiophene(4-MDBT)and 4,6-dimethyldibenzothiophene(4,6-DMDBT).Ultimately,a possible photocatalytic desulfurization mechanism is proposed according to the Gaschromatography-mass spectrometry(GC-MS),proving that the final product is the corresponding sulfone.The trapping experiment and electron spin resonance(ESR)analysis confirmed that h^(+)and,COOH played critical roles in the oxidation process.The work offers a practicable strategy for efficiently converting DBT to DBTO_(2) with added value.展开更多
Synergic catalytic effect between active sites and supports greatly determines the catalytic activity for the aerobic oxidative desulfurization of fuel oils.In this work,Ni-doped Co-based bimetallic metal-organic fram...Synergic catalytic effect between active sites and supports greatly determines the catalytic activity for the aerobic oxidative desulfurization of fuel oils.In this work,Ni-doped Co-based bimetallic metal-organic framework(CoNi-MOF)is fabricated to disperse N-hydroxyphthalimide(NHPI),in which the whole catalyst provides plentiful synergic catalytic effect to improve the performance of oxidative desulfurization(ODS).As a bimetallic MOF,the second metal Ni doping results in the flower-like morphology and the modification of electronic properties,which ensure the exposure of NHPI and strengthen the synergistic effect of the overall catalyst.Compared with the monometallic Co-MOF and naked NHPI,the NHPI@CoNi-MOF triggers the efficient activation of molecular oxygen and improves the ODS performance without an initiator.The sulfur removal of dibenzothiophene-based model oil reaches 96.4%over the NHPI@CoNi-MOF catalyst in 8 h of reaction.Furthermore,the catalytic product of this aerobic ODS reaction is sulfone,which is adsorbed on the catalyst surface due to the difference in polarity.This work provides new insight and strategy for the design of a strong synergic catalytic effect between NHPI and bimetallic supports toward high-activity aerobic ODS materials.展开更多
Polyurethane/desulfurization ash(PU/DA)composites were synthesized using"one-pot method",with the incorporation of a silane coupling agent(KH550)as a"molecular bridge"to facilitate the integration ...Polyurethane/desulfurization ash(PU/DA)composites were synthesized using"one-pot method",with the incorporation of a silane coupling agent(KH550)as a"molecular bridge"to facilitate the integration of DA as hard segments into the PU molecular chain.The effects of DA content(φ)on the mechanical properties,thermal stability,and hydrophobicity of PU,both before and after the addition of KH550,were thoroughly examined.The results of microscopic mechanism analysis confirmed that KH550 chemically modified the surface of DA,facilitating its incorporation into the polyurethane molecular chain,thereby significantly enhancing the compatibility and dispersion of DA within the PU matrix.When the mass fraction of modified DA(MDA)reached 12%,the mechanical properties,thermal stability,and hydrophobicity of the composites were substantially improved,with the tensile strength reaching 14.9 MPa,and the contact angle measuring 100.6°.展开更多
A few-layered hexagonal boron nitride nanosheets stabilized platinum nanoparticles(Pt/h-BNNS)is engineered for oxidation-promoted adsorptive desulfurization(OPADS)of fuel oil.It was found that the few-layered structur...A few-layered hexagonal boron nitride nanosheets stabilized platinum nanoparticles(Pt/h-BNNS)is engineered for oxidation-promoted adsorptive desulfurization(OPADS)of fuel oil.It was found that the few-layered structure and the defective sites of h-BNNS not only are beneficial to the stabilization of Pt NPs but also favor the adsorption of aromatic sulfides.By employing Pt/h-BNNS with a Pt loading amount of 1.19 wt%as the active adsorbent and air as an oxidant,a 98.0%sulfur removal over dibenzothiophene(DBT)is achieved along with a total conversion of the DBT to the corresponding sulfones(DBTO_(2)).Detailed experiments show that the excellent desulfurization activity originates from the few-layered structure of h-BNNS and the high catalytic activity of Pt NPs.In addition,the OPADS system with Pt/h-BNNS as the active adsorbent shows remarkable stability in desulfurization performance with the existence of different interferents such as olefin,and aromatic hydrocarbons.Besides,the Pt/h-BNNS can be recycled 12 times without a significant decrease in desulfurization performance.Also,a process flow diagram is proposed for deep desulfurization of fuel oil and recovery of high value-added products,which would promote the industrial application of such OPADS strategy.展开更多
An in-process technology approach is proposed to identify the source of acid mine drainage(AMD)generation and prevent its formation in a porphyry copper waste rock(WR).Adopting actions before stockpiling the WR enable...An in-process technology approach is proposed to identify the source of acid mine drainage(AMD)generation and prevent its formation in a porphyry copper waste rock(WR).Adopting actions before stockpiling the WR enables the establishment of potential contaminants and predicts the more convenient method for AMD prevention.A WR sample was separated into size fractions,and the WR’s net acidgenerating potential was quantified using chemical and mineralogical characterization.The diameter of physical locking of sulfides(DPLS)was determined,and the fractions below the DPLS were desulfurized using flotation.Finally,the WR fractions and tailing from the flotation test were submitted to acid-base accounting and weathering tests to evaluate their acid-generating potential.Results show that the WR’s main sulfide mineral is pyrite,and the DPLS was defined as 850μm.A sulfide recovery of 91%was achieved using a combination of HydroFloat^(®)and Denver cells for a size fraction lower than DPLS.No grinding was conducted.The results show that size fractions greater than DPLS and the desulfurized WR are unlikely to produce AMD.The outcomes show that in-processing technology can be a more proactive approach and an effective tool for avoiding AMD in a porphyry copper WR.展开更多
Porous ionic liquids have demonstrated excellent performance in the field of separation,attributed to their high specific surface area and efficient mass transfer.Herein,task-specific protic porous ionic liquids(PPILs...Porous ionic liquids have demonstrated excellent performance in the field of separation,attributed to their high specific surface area and efficient mass transfer.Herein,task-specific protic porous ionic liquids(PPILs)were prepared by employing a novel one-step coupling neutralization reaction strategy for extractive desulfurization.The single-extraction efficiency of PPILs reached 75.0%for dibenzothiophene.Moreover,adding aromatic hydrocarbon interferents resulted in a slight decrease in the extraction efficiency of PPILs(from 45.2%to 37.3%,37.9%,and 33.5%),indicating the excellent extraction selectivity of PPILs.The experimental measurements and density functional theory calculations reveal that the surface channels of porous structures can selectively capture dibenzothiophene by the stronger electrophilicity(Eint(HS surface channel/DBT)=-39.8 kcal mol^(-1)),and the multiple extraction sites of ion pairs can effectively enrich and transport dibenzothiophene from the oil phase into PPILs throughπ...π,C-H...πand hydrogen bonds interactions.Furthermore,this straightforward synthetic strategy can be employed in preparing porous liquids,offering new possibilities for synthesizing PPILs with tailored functionalities.展开更多
In order to reduce the sulfur compounds in diesel fuel,boron nitride(BN)has been used as a novel metal-free catalyst in the present research.This nanocatalyst was synthesized via template-free approach followed by hea...In order to reduce the sulfur compounds in diesel fuel,boron nitride(BN)has been used as a novel metal-free catalyst in the present research.This nanocatalyst was synthesized via template-free approach followed by heating treatment at 900℃ in nitrogen atmosphere that the characteristics of the sample were identified by the X-ray diffraction,Fourier-transform infrared spectroscopy,Raman spectroscopy,field emission scanning electron microscopy,transmission electron microscopy,atomic force microscopy,and N2 adsorption-desorption isotherms.The results of structural and morphological analysis represented that BN has been successfully synthesized.The efficacy of the main operating parameters on the process was studied by using response surface methodology based on the Box-Behnken design method.The prepared catalyst showed high efficiency in oxidative desulfurization of diesel fuel with initial sulfur content of 8040 mg·kg^(-1)S.From statistical analysis,a significant quadratic model was obtained to predict the sulfur removal as a function of efficient parameters.The maximum efficiency of 72.4%was achieved under optimized conditions at oxidant/sulfur molar ratio of 10.2,temperature of 71℃,reaction time of 113 min,and catalyst dosage of 0.36 g.Also,the reusability of the BN was studied,and the result showed little reduction in activity of the catalyst after 10 times regeneration.Moreover,a plausible mechanism was proposed for oxidation of sulfur compounds on the surface of the catalyst.The present study shows that BN materials can be selected as promising metal-free catalysts for desulfurization process.展开更多
A series of Lewis-acid deep eutectic solvents (DESs) were synthesized by stirring phosphoric acid and zincchloride as raw materials at 80℃ to form H_(3)PO_(4)/nZnCl_(2) (n = 0.1, 0.25, 0.5, 0.75, 1). The DESs were ch...A series of Lewis-acid deep eutectic solvents (DESs) were synthesized by stirring phosphoric acid and zincchloride as raw materials at 80℃ to form H_(3)PO_(4)/nZnCl_(2) (n = 0.1, 0.25, 0.5, 0.75, 1). The DESs were characterized byFourier transform infrared spectrophotometry (FT-IR), thermogravimetry/differential thermogravimetry (TG/DTG), andelectron spray ionization mass spectrometry (ESI-MS). The DESs were used as both extractants and catalysts to removedibenzothiophene from fuels via oxidative desulfurization (ODS). Experiments were performed to investigated the influenceof factors such as composition of DES, temperature, oxidant dosage (molar ratio of O:S), DES dosage (volume ratio ofDES:oil), and number of cycles on desulfurization rate. The results indicated that the removal rate of dibenzothiophene (DBT)was affected by the Lewis acidic DESs, with that of H_(3)PO_(4)/0.25∙ZnCl_(2) reaching 96.4% under optimal conditions (Voil=5 mL,VDES=1 mL, an oxidant dosage of 6, T=50 ℃). After six cycles, the desulfurization rate of H_(3)PO_(4)/0.25∙ZnCl_(2) remained above94.1%. The apparent activation energy of dibenzothiophene (DBT) removal reaction was determined by a pseudo-first orderkinetic equation according to the Arrhenius equation to be 32.34 kJ/mol, as estimated. A reaction mechanism is proposedbased on the experimental data and characterization results.展开更多
The synergistic impact of mechanical ball milling and flue gas desulfurization(FGD)gypsum on the dealkalization of bauxite residue was investigated through integrated analyses of solution chemistry,mineralogy,and micr...The synergistic impact of mechanical ball milling and flue gas desulfurization(FGD)gypsum on the dealkalization of bauxite residue was investigated through integrated analyses of solution chemistry,mineralogy,and microtopography.The results showed a significant decrease in Na_(2)O content(>30 wt.%)of FGD gypsum-treated bauxite residue after 30 min of mechanical ball milling.Mechanical ball milling resulted in differentiation of the elemental distribution,modification of the minerals in crystalline structure,and promotion in the dissolution of alkaline minerals,thus enhancing the acid neutralization capacity of bauxite residue.5 wt.%FGD gypsum combined with 30 min mechanical ball milling was optimal for the dealkalization of bauxite residue.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
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,...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 exploration of highly efficient catalysts based on nano-sized Ti-rich titanosilicate zeolites with controllable active titanium species is of great importance in zeolite catalytic reactions.Herein,we reported an e...The exploration of highly efficient catalysts based on nano-sized Ti-rich titanosilicate zeolites with controllable active titanium species is of great importance in zeolite catalytic reactions.Herein,we reported an efficient and facile synthesis of nano-sized Ti-rich TS-1(MFI)zeolites by replacing tetrabutyl orthotitanate(TBOT)with tetrabutyl orthotitanate tetramer(TBOT-tetramer)as the titanium source.The introduced TBOT-tetramer slowed down the zeolite crystallization process,and accordingly balanced the rate of incorporating Ti and the crystal growth and inhibited the massive formation of anatase species.Notably,the prepared Ti-rich TS-1 zeolite sample had a Si/Ti as low as 27.6 in contrast to conventional one with a molar ratio of 40.The TBOT-tetramer endowed the titanosilicate zeolites with enriched active titanium species and enlarged external surface area.It also impeded the formation of anatase species,resulting in superior catalytic behavior toward the oxidative desulfurization of dibenzothiophene compared with the conventional TS-1 zeolite counterpart prepared with TBOT.展开更多
Hydrogen sulfide(H_(2)S)is an industrial exhausted gas that is highly toxic to humans and the environment.Combining desulfurization and fabrication of cathode materials for lithium-sulfur batteries(LSBs)can solve this...Hydrogen sulfide(H_(2)S)is an industrial exhausted gas that is highly toxic to humans and the environment.Combining desulfurization and fabrication of cathode materials for lithium-sulfur batteries(LSBs)can solve this issue with a double benefit.Herein,the amino-functionalized lotus root-like carbon nanofibers(NH_(2)-PLCNFs)are prepared by the amination of electrospinning carbon nanofibers under dielectric barrier discharge plasma.Selective catalytic oxidation of H_(2)S to elemental sulfur(S)is achieved over the metalfree NH_(2)-PLCNFs catalyst,and the obtained composite S@NH_(2)-PLCNFs is further used as cathode in LSBs.NH_(2)-PLCNFs enable efficient desulfurization(removal capacity as high as 3.46 g H_(2)S g^(−1) catalyst)and strongly covalent stabilization of S on modified carbon nanofibers.LSBs equipped with S@NH_(2)-PLCNFs deliver a high specific capacity of 705.8 mA h g^(−1) at 1 C after 1000 cycles based on the spatial confinement and the covalent stabilization of electroactive materials on amino-functionalized porous carbon matrix.It is revealed that S@NH_(2)-PLCNFs obtained by this kind of chemical vapor deposition leads to a more homogeneous S distribution and superior electrochemical performance to the sample S/NH_(2)-PLCNF-M prepared by the traditional molten infusion.This work opens a new avenue for the combination of environment protection and energy storage.展开更多
The ultra-deep desulfurization of oil needs to be solved urgently due to various problems,including environmental pollution and environmental protection requirements.Oxidative desulfurization(ODS)was considered to be ...The ultra-deep desulfurization of oil needs to be solved urgently due to various problems,including environmental pollution and environmental protection requirements.Oxidative desulfurization(ODS)was considered to be the most promising technology.The facile synthesis of highly efficient and stable HPW-based heterogeneous catalysts for oxidative desulfurization is still a challenging task.In this paper,pentamethylene hexamine(PEHA)and phosphotungstic acid(HPW)were combined by a simple one-step method to prepare a heterogeneous catalyst of PEHA-HPW for the production of ultra-deep desulfurization fuel oil.The composite material exhibited excellent catalytic activity and high recyclability,which could reach a 100% dibenzothiophene(DBT)removal rate in 30 min and be recycled at least 5 times.Experiments and DFT simulations were used to better examine the ODS mechanism of PEHA-HPW.It was proved that the rich amino groups on the surface of PEHA-HPW play a crucial role.This work provides a simple and feasible way for the manufacture of efficient HPW-based catalysts.展开更多
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 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the financial supports from National Natural Science Foundation of China(22172066,22378176)supported by State Key Laboratory of Heavy Oil ProcessingSupported by Jiangsu Collaborative Innovation Center of Technology and Material of Water Treatment,Suzhou University of Science and Technology。
文摘An efficient mass transfer process is a critical factor for regulating catalytic activity in a photocatalytic desulfurization system.Herein,a phosphotungstic acid(HPW)active center is successfully composited with a quaternary ammonium phosphotungstate-based hexadecyltrimethylammonium chloride ionic liquid(CTAC-HPW)by the ion exchange method for the photocatalytic oxidative desulfurization of dibenzothiophene sulfide.The keggin structure of HPW and highly mass transfer performance of organic cations synergistically enhanced the photocatalytic activity towards the effective convertion of dibenzothiophene(DBT)with the excitation of visible light.The deep desulfurization(<10 mg·kg^(-1))is attained within 30 min,and well stability is demonstrated within 25 cycles.Moreover,the CTAC-HPW photocatalyst projects well selectivity to interference from coexisting compounds such as olefins and aromatic hydrocarbons and universality of dibenzothiophenes,for example,4-methyldibenzothiophene(4-MDBT)and 4,6-dimethyldibenzothiophene(4,6-DMDBT).Ultimately,a possible photocatalytic desulfurization mechanism is proposed according to the Gaschromatography-mass spectrometry(GC-MS),proving that the final product is the corresponding sulfone.The trapping experiment and electron spin resonance(ESR)analysis confirmed that h^(+)and,COOH played critical roles in the oxidation process.The work offers a practicable strategy for efficiently converting DBT to DBTO_(2) with added value.
基金This work was financially supported by the National Natural Science Foundation of China(Nos.21978119,22202088)Key Research and Development Plan of Hainan Province(ZDYF2022SHFZ285)Jiangsu Funding Program for Excellent Postdoctoral Talent(2022ZB636)。
文摘Synergic catalytic effect between active sites and supports greatly determines the catalytic activity for the aerobic oxidative desulfurization of fuel oils.In this work,Ni-doped Co-based bimetallic metal-organic framework(CoNi-MOF)is fabricated to disperse N-hydroxyphthalimide(NHPI),in which the whole catalyst provides plentiful synergic catalytic effect to improve the performance of oxidative desulfurization(ODS).As a bimetallic MOF,the second metal Ni doping results in the flower-like morphology and the modification of electronic properties,which ensure the exposure of NHPI and strengthen the synergistic effect of the overall catalyst.Compared with the monometallic Co-MOF and naked NHPI,the NHPI@CoNi-MOF triggers the efficient activation of molecular oxygen and improves the ODS performance without an initiator.The sulfur removal of dibenzothiophene-based model oil reaches 96.4%over the NHPI@CoNi-MOF catalyst in 8 h of reaction.Furthermore,the catalytic product of this aerobic ODS reaction is sulfone,which is adsorbed on the catalyst surface due to the difference in polarity.This work provides new insight and strategy for the design of a strong synergic catalytic effect between NHPI and bimetallic supports toward high-activity aerobic ODS materials.
基金Funded by the National Key Research and Development Project(No.2019YFC1908204)the Guiding Projects in Fujian Province(No.2023H0023)the Fuzhou Science and Technology Plan Project(No.2022-P-012)。
文摘Polyurethane/desulfurization ash(PU/DA)composites were synthesized using"one-pot method",with the incorporation of a silane coupling agent(KH550)as a"molecular bridge"to facilitate the integration of DA as hard segments into the PU molecular chain.The effects of DA content(φ)on the mechanical properties,thermal stability,and hydrophobicity of PU,both before and after the addition of KH550,were thoroughly examined.The results of microscopic mechanism analysis confirmed that KH550 chemically modified the surface of DA,facilitating its incorporation into the polyurethane molecular chain,thereby significantly enhancing the compatibility and dispersion of DA within the PU matrix.When the mass fraction of modified DA(MDA)reached 12%,the mechanical properties,thermal stability,and hydrophobicity of the composites were substantially improved,with the tensile strength reaching 14.9 MPa,and the contact angle measuring 100.6°.
基金financial support from the National Natural Science Foundation of China(22178154,22008094,21908082,21878133)Natural Science Foundation of Jiangsu Province(BK20190852,BK20190854)Natural Science Foundation for Jiangsu Colleges and Universities(19KJB530005).
文摘A few-layered hexagonal boron nitride nanosheets stabilized platinum nanoparticles(Pt/h-BNNS)is engineered for oxidation-promoted adsorptive desulfurization(OPADS)of fuel oil.It was found that the few-layered structure and the defective sites of h-BNNS not only are beneficial to the stabilization of Pt NPs but also favor the adsorption of aromatic sulfides.By employing Pt/h-BNNS with a Pt loading amount of 1.19 wt%as the active adsorbent and air as an oxidant,a 98.0%sulfur removal over dibenzothiophene(DBT)is achieved along with a total conversion of the DBT to the corresponding sulfones(DBTO_(2)).Detailed experiments show that the excellent desulfurization activity originates from the few-layered structure of h-BNNS and the high catalytic activity of Pt NPs.In addition,the OPADS system with Pt/h-BNNS as the active adsorbent shows remarkable stability in desulfurization performance with the existence of different interferents such as olefin,and aromatic hydrocarbons.Besides,the Pt/h-BNNS can be recycled 12 times without a significant decrease in desulfurization performance.Also,a process flow diagram is proposed for deep desulfurization of fuel oil and recovery of high value-added products,which would promote the industrial application of such OPADS strategy.
基金supported by Agencia Nacional de Investigación y Desarrollo de Chile(ANID)Anillo-Grant ANID/ACT210027,Fondecyt 1211498,and ANID/AFB230001+1 种基金the ANID scholarship Grant 21210801partially performed by Luis Cisternas during the visit to the Universitédu Québec,supported by MINEDUC-UA project,code ANT1999.
文摘An in-process technology approach is proposed to identify the source of acid mine drainage(AMD)generation and prevent its formation in a porphyry copper waste rock(WR).Adopting actions before stockpiling the WR enables the establishment of potential contaminants and predicts the more convenient method for AMD prevention.A WR sample was separated into size fractions,and the WR’s net acidgenerating potential was quantified using chemical and mineralogical characterization.The diameter of physical locking of sulfides(DPLS)was determined,and the fractions below the DPLS were desulfurized using flotation.Finally,the WR fractions and tailing from the flotation test were submitted to acid-base accounting and weathering tests to evaluate their acid-generating potential.Results show that the WR’s main sulfide mineral is pyrite,and the DPLS was defined as 850μm.A sulfide recovery of 91%was achieved using a combination of HydroFloat^(®)and Denver cells for a size fraction lower than DPLS.No grinding was conducted.The results show that size fractions greater than DPLS and the desulfurized WR are unlikely to produce AMD.The outcomes show that in-processing technology can be a more proactive approach and an effective tool for avoiding AMD in a porphyry copper WR.
基金financially supported by the National Natural Science Foundation of China (Nos.22078135,21808092,21978119,22202088)。
文摘Porous ionic liquids have demonstrated excellent performance in the field of separation,attributed to their high specific surface area and efficient mass transfer.Herein,task-specific protic porous ionic liquids(PPILs)were prepared by employing a novel one-step coupling neutralization reaction strategy for extractive desulfurization.The single-extraction efficiency of PPILs reached 75.0%for dibenzothiophene.Moreover,adding aromatic hydrocarbon interferents resulted in a slight decrease in the extraction efficiency of PPILs(from 45.2%to 37.3%,37.9%,and 33.5%),indicating the excellent extraction selectivity of PPILs.The experimental measurements and density functional theory calculations reveal that the surface channels of porous structures can selectively capture dibenzothiophene by the stronger electrophilicity(Eint(HS surface channel/DBT)=-39.8 kcal mol^(-1)),and the multiple extraction sites of ion pairs can effectively enrich and transport dibenzothiophene from the oil phase into PPILs throughπ...π,C-H...πand hydrogen bonds interactions.Furthermore,this straightforward synthetic strategy can be employed in preparing porous liquids,offering new possibilities for synthesizing PPILs with tailored functionalities.
文摘In order to reduce the sulfur compounds in diesel fuel,boron nitride(BN)has been used as a novel metal-free catalyst in the present research.This nanocatalyst was synthesized via template-free approach followed by heating treatment at 900℃ in nitrogen atmosphere that the characteristics of the sample were identified by the X-ray diffraction,Fourier-transform infrared spectroscopy,Raman spectroscopy,field emission scanning electron microscopy,transmission electron microscopy,atomic force microscopy,and N2 adsorption-desorption isotherms.The results of structural and morphological analysis represented that BN has been successfully synthesized.The efficacy of the main operating parameters on the process was studied by using response surface methodology based on the Box-Behnken design method.The prepared catalyst showed high efficiency in oxidative desulfurization of diesel fuel with initial sulfur content of 8040 mg·kg^(-1)S.From statistical analysis,a significant quadratic model was obtained to predict the sulfur removal as a function of efficient parameters.The maximum efficiency of 72.4%was achieved under optimized conditions at oxidant/sulfur molar ratio of 10.2,temperature of 71℃,reaction time of 113 min,and catalyst dosage of 0.36 g.Also,the reusability of the BN was studied,and the result showed little reduction in activity of the catalyst after 10 times regeneration.Moreover,a plausible mechanism was proposed for oxidation of sulfur compounds on the surface of the catalyst.The present study shows that BN materials can be selected as promising metal-free catalysts for desulfurization process.
基金the College Student Innovation and Entrepreneurship Training Program Project of Liaoning Province(202310148016)Doctoral Fund of Liaoning Province(201501105).
文摘A series of Lewis-acid deep eutectic solvents (DESs) were synthesized by stirring phosphoric acid and zincchloride as raw materials at 80℃ to form H_(3)PO_(4)/nZnCl_(2) (n = 0.1, 0.25, 0.5, 0.75, 1). The DESs were characterized byFourier transform infrared spectrophotometry (FT-IR), thermogravimetry/differential thermogravimetry (TG/DTG), andelectron spray ionization mass spectrometry (ESI-MS). The DESs were used as both extractants and catalysts to removedibenzothiophene from fuels via oxidative desulfurization (ODS). Experiments were performed to investigated the influenceof factors such as composition of DES, temperature, oxidant dosage (molar ratio of O:S), DES dosage (volume ratio ofDES:oil), and number of cycles on desulfurization rate. The results indicated that the removal rate of dibenzothiophene (DBT)was affected by the Lewis acidic DESs, with that of H_(3)PO_(4)/0.25∙ZnCl_(2) reaching 96.4% under optimal conditions (Voil=5 mL,VDES=1 mL, an oxidant dosage of 6, T=50 ℃). After six cycles, the desulfurization rate of H_(3)PO_(4)/0.25∙ZnCl_(2) remained above94.1%. The apparent activation energy of dibenzothiophene (DBT) removal reaction was determined by a pseudo-first orderkinetic equation according to the Arrhenius equation to be 32.34 kJ/mol, as estimated. A reaction mechanism is proposedbased on the experimental data and characterization results.
基金the National Natural Science Foundation of China(Nos.42177391,42077379)the Natural Science Foundation of Hunan Province,China(No.2022JJ20060)+1 种基金the Central South University Innovation-driven Research Program,China(No.2023CXQD065)the Fundamental Research Funds for the Central Universities of Central South University,China(No.2023ZZTS0800).
文摘The synergistic impact of mechanical ball milling and flue gas desulfurization(FGD)gypsum on the dealkalization of bauxite residue was investigated through integrated analyses of solution chemistry,mineralogy,and microtopography.The results showed a significant decrease in Na_(2)O content(>30 wt.%)of FGD gypsum-treated bauxite residue after 30 min of mechanical ball milling.Mechanical ball milling resulted in differentiation of the elemental distribution,modification of the minerals in crystalline structure,and promotion in the dissolution of alkaline minerals,thus enhancing the acid neutralization capacity of bauxite residue.5 wt.%FGD gypsum combined with 30 min mechanical ball milling was optimal for the dealkalization of bauxite residue.
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, China (Grant 21920102005, 22288101, and 21835002)the 111 Project, China (B17020)+2 种基金the European Union through the European Research Council, European Union (grant ERC-AdG-2014-671093, SynCatMatch)the Spanish Government through “Severo Ochoa”, Spain (SEV2016-0683, MINECO) for supporting this workthe financial support from China Scholarship Council, China
文摘The exploration of highly efficient catalysts based on nano-sized Ti-rich titanosilicate zeolites with controllable active titanium species is of great importance in zeolite catalytic reactions.Herein,we reported an efficient and facile synthesis of nano-sized Ti-rich TS-1(MFI)zeolites by replacing tetrabutyl orthotitanate(TBOT)with tetrabutyl orthotitanate tetramer(TBOT-tetramer)as the titanium source.The introduced TBOT-tetramer slowed down the zeolite crystallization process,and accordingly balanced the rate of incorporating Ti and the crystal growth and inhibited the massive formation of anatase species.Notably,the prepared Ti-rich TS-1 zeolite sample had a Si/Ti as low as 27.6 in contrast to conventional one with a molar ratio of 40.The TBOT-tetramer endowed the titanosilicate zeolites with enriched active titanium species and enlarged external surface area.It also impeded the formation of anatase species,resulting in superior catalytic behavior toward the oxidative desulfurization of dibenzothiophene compared with the conventional TS-1 zeolite counterpart prepared with TBOT.
基金financial support from projects funded by the National Natural Science Foundation of China(22179017,52172038).
文摘Hydrogen sulfide(H_(2)S)is an industrial exhausted gas that is highly toxic to humans and the environment.Combining desulfurization and fabrication of cathode materials for lithium-sulfur batteries(LSBs)can solve this issue with a double benefit.Herein,the amino-functionalized lotus root-like carbon nanofibers(NH_(2)-PLCNFs)are prepared by the amination of electrospinning carbon nanofibers under dielectric barrier discharge plasma.Selective catalytic oxidation of H_(2)S to elemental sulfur(S)is achieved over the metalfree NH_(2)-PLCNFs catalyst,and the obtained composite S@NH_(2)-PLCNFs is further used as cathode in LSBs.NH_(2)-PLCNFs enable efficient desulfurization(removal capacity as high as 3.46 g H_(2)S g^(−1) catalyst)and strongly covalent stabilization of S on modified carbon nanofibers.LSBs equipped with S@NH_(2)-PLCNFs deliver a high specific capacity of 705.8 mA h g^(−1) at 1 C after 1000 cycles based on the spatial confinement and the covalent stabilization of electroactive materials on amino-functionalized porous carbon matrix.It is revealed that S@NH_(2)-PLCNFs obtained by this kind of chemical vapor deposition leads to a more homogeneous S distribution and superior electrochemical performance to the sample S/NH_(2)-PLCNF-M prepared by the traditional molten infusion.This work opens a new avenue for the combination of environment protection and energy storage.
基金supported by the National Natural Science Foundation of China(22378065,22278077)the Fujian Province Department of Science&Technology,China(2019YZ017001)。
文摘The ultra-deep desulfurization of oil needs to be solved urgently due to various problems,including environmental pollution and environmental protection requirements.Oxidative desulfurization(ODS)was considered to be the most promising technology.The facile synthesis of highly efficient and stable HPW-based heterogeneous catalysts for oxidative desulfurization is still a challenging task.In this paper,pentamethylene hexamine(PEHA)and phosphotungstic acid(HPW)were combined by a simple one-step method to prepare a heterogeneous catalyst of PEHA-HPW for the production of ultra-deep desulfurization fuel oil.The composite material exhibited excellent catalytic activity and high recyclability,which could reach a 100% dibenzothiophene(DBT)removal rate in 30 min and be recycled at least 5 times.Experiments and DFT simulations were used to better examine the ODS mechanism of PEHA-HPW.It was proved that the rich amino groups on the surface of PEHA-HPW play a crucial role.This work provides a simple and feasible way for the manufacture of efficient HPW-based catalysts.