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
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
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 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
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
As a pyrometallurgical process,circulating fluidized bed(CFB) roasting has good potential for application in desulfurization of high-sulfur bauxite.The gas-solid distribution and reaction during CFB roasting of high-s...As a pyrometallurgical process,circulating fluidized bed(CFB) roasting has good potential for application in desulfurization of high-sulfur bauxite.The gas-solid distribution and reaction during CFB roasting of high-sulfur bauxite were simulated using the computational particle fluid dynamics(CPFD) method.The effect of primary air flow velocity on particle velocity,particle volume distribution,furnace temperature distribution and pressure distribution were investigated.Under the condition of the same total flow of natural gas,the impact of the number of inlets on the desulfurization efficiency,atmosphere mass fraction distribution and temperature distribution in the furnace was further investigated.展开更多
The development of highly active functionalized ionic liquids(ILs)as both extractants and catalysts for use in achieving deep desulfurization continues to pose challenges.In this study,a highly efficient oxidative des...The development of highly active functionalized ionic liquids(ILs)as both extractants and catalysts for use in achieving deep desulfurization continues to pose challenges.In this study,a highly efficient oxidative desulfurization system was constructed,composed of dual-acidic ionic liquids(DILs)and H_(2)O_(2)-AcOH.The investigation results of four DILs prepared from different metal chlorides([HSO_(3)C_(3)NEt_(3)]Cl-MnCl_(n),MnCl_(n)=AlCl_(3),ZnCl_(2),CuCl_(2),FeCl_(3))in oxidative desulfurization showed that[HSO_(3)C_(3)NEt_(3)]Cl-AlCl_(3)had an outstanding catalytic effect and significantly promoted the oxidation of sulfides.With a 0.2 g[HSO_(3)C_(3)NEt_(3)]Cl-AlCl_(3),the removal rate of dibenzothiophene(DBT)reached 100%in 10 mL model oil under mild conditions at 55℃for 20 min.The key is its ability to induce the dismutation of su-peroxide anions(·O_(2)^(-)),which facilitates the generation of singlet oxygen(1 O_(2)).The efficient oxidation of DBT is accomplished through a predominantly^(1)O_(2)-mediated_(n)on-radical mechanism.[HSO_(3)C_(3)NEt_(3)]Cl-AlCl_(3)serves as a favorable medium for contact to be made between^(1)O_(2)and sulfides,which indicates an efficient catalytic-adsorption synergy.展开更多
Practical applications of desulfurization gypsum are limited owing to its brittleness and low strength.To overcome these challenges,researchers have developed engineered desulfurization gypsum composites(EDGCs)by inco...Practical applications of desulfurization gypsum are limited owing to its brittleness and low strength.To overcome these challenges,researchers have developed engineered desulfurization gypsum composites(EDGCs)by incorporating ultrahigh molecular weight polyethylene(UHMWPE)fiber and sulfoaluminate cement(SAC).The mix ratio was optimized using response surface methodology(RSM).Experimental testing of EDGC under compressive and tensile loads led to the creation of a regression model that investigates the influence of variables and their interactions on the material’s compressive and tensile strengths.Additionally,microscopic morphology and hydration product composition were analyzed to explore the influence mechanism.The results indicated that EDGC’s compressive strength increased by up to 38.4%owing to a decreased water-binder ratio and higher SAC content.Similarly,tensile strength increased by up to 38.6%owing to increased SAC and fiber content.Moreover,EDGC demonstrated excellent strain-hardening behavior and multiple cracking characteristics,achieving a maximum tensile strain of nearly 3%.The research findings provide valuable insights for optimizing the performance of desulfurization gypsum.展开更多
Desulfurization technology is rather difficult and urgently needed for carbon dioxide(CO_(2))utilization in industry.A new Cu(I)-based adsorbent was synthesized and examined for the capacity of removing carbonyl sulfi...Desulfurization technology is rather difficult and urgently needed for carbon dioxide(CO_(2))utilization in industry.A new Cu(I)-based adsorbent was synthesized and examined for the capacity of removing carbonyl sulfide(COS)from a CO_(2)stream in an effort to solve the competitive adsorption between CO_(2)and COS and to seek opportunity to advance adsorption capacity.A wide range of character-ization techniques were used to investigate the physicochemical properties of the synthesized Cu(I)adsorbent featuringπ-complexation and their correlations with the adsorption performance.Meanwhile,the first principal calculation software CP2K was used to develop an understanding of the adsorption mechanism,which can offer useful guidance for the adsorbent regeneration.The synthesized Cu(I)adsorbent,prepared by using copper citrate and citric acid on the ZSM-5(SiO_(2)/Al_(2)O_(3)=25)carrier,outperformed other adsorbents with varying formulations and carriers in adsorption capacities.Through optimization of the preparation and adsorption conditions for various adsorbents,the breakthrough adsorption capacity(Qb)for COS was further enhanced from 2.19 mg/g to 15.36 mg/g.The formed stableπ-complex bonds between COS and Cu(I),as confirmed by density func-tional theory calculations,were verified by the significant improvement in the adsorption capacity after regeneration at 600°C.The above advantages render the novel synthesized Cu(I)adsorbent a promising candidate featuring cost-effectiveness,high efficacy and good regenerability for desulfurization from a CO_(2)stream.展开更多
Development of clean desulfurization process that combines both efficient and environmentally friendly remains a significant challenge for diesel production.The photocatalytic oxidation desulfurization technology is r...Development of clean desulfurization process that combines both efficient and environmentally friendly remains a significant challenge for diesel production.The photocatalytic oxidation desulfurization technology is regarded as a promising process depending on the superior electron transfer and visible light utilization of photocatalyst.Herein,the nonstoichiometry MoO_(3-x)with outstanding photoresponse ability is prepared and modified by imidazole-based ionic liquid[C_(12)mim]Cl to upgrade electronic structure.The interface H-bonding between MoO_(3-x)and[C_(12)mim]Cl regard as electronic transfer channel and the recombination of e^(-)-h^(+)pairs is effectively inhibited with the modification of[C_(12)mim]Cl.Deep desulfurization rate of 96.6%can be reached within 60 min and the MoO_(3-x)/[C_(12)mim]Cl(MoC_(12))photocatalyst demonstrated outstanding cyclic stability within 7 cycles in an extraction coupled photocatalytic oxidation desulfurization(ECPODS)system.The study provides a new perspective on enhancing photocatalytic desulfurization through defect engineering and surface modification.展开更多
For the treatment of the mixed flue gas desulfurization wastewater with high salinity by the biological fluidized bed process,the optimum temperature was 25-35℃,and the optimum hydraulic retention time was 10 h.When ...For the treatment of the mixed flue gas desulfurization wastewater with high salinity by the biological fluidized bed process,the optimum temperature was 25-35℃,and the optimum hydraulic retention time was 10 h.When the influent quality was stable,the average concentration of COD,NH_(4)^(+)-N and TN in the inlet water was 210,11 and 16.3 mg/L,respectively,and their average concentration in the effluent was 54,0.32 and 4.09 mg/L,respectively.The treatment effect was good.When the incoming water quality of flue gas desulfurization wastewater fluctuated greatly,the effluent quality was still relatively stable after being treated by the biological fluidized bed,indicating that the biological fluidized bed process had a good ability to resist the impact of water quality in the treatment of high-salinity flue gas desulfurization wastewater.At the same time,the biological fluidized bed process provides a reference for high-salinity wastewater that is difficult to be biologically treated.展开更多
The instantaneous desulfurization of CaO-Al_(2)O_(3)-SiO_(2)slag particles in the molten steel was in situ observed using a high-temperature confocal scanning laser microscope.The desulfurization effect of CaO-Al_(2)O...The instantaneous desulfurization of CaO-Al_(2)O_(3)-SiO_(2)slag particles in the molten steel was in situ observed using a high-temperature confocal scanning laser microscope.The desulfurization effect of CaO-Al_(2)O_(3)-SiO_(2)slags with different compositions was discussed.The influence of CaO/Al_(2)O_(3)and CaO/SiO_(2)on the desulfurization effect was analyzed.It was shown that in the liquid phase range,the higher CaO/SiO_(2)and CaO/Al_(2)O_(3)can significantly improve the desulfurization effect of the slag.A dimensionless desulfurization index Sindex was introduced to evaluate the desulfurization ability of CaO-Al_(2)O_(3)-SiO_(2)slags quantitatively.The Sindex values of CaO-Al_(2)O_(3)-SiO_(2)with different compositions at 1550°C were calculated.It was suggested to use(65%-75%)CaO-(0-20%)SiO_(2)-(20%-40%)Al_(2)O_(3)slags to improve the molten steel desulfurization.展开更多
Electroslag remelting(ESR) gives a combination of liquid metal refining and solidification structure control.One of the typical aspects of liquid metal refining during ESR for the advanced steel and alloy production i...Electroslag remelting(ESR) gives a combination of liquid metal refining and solidification structure control.One of the typical aspects of liquid metal refining during ESR for the advanced steel and alloy production is desulfurization.It involves two patterns, i.e., slag–metal reaction and gas–slag reaction(gasifying desulfurization).In this paper, the advances in desulfurization practices of ESR are reviewed.The effects of processing parameters, including the initial sulfur level of consumable electrode, remelting atmosphere, deoxidation schemes of ESR,slag composition, melting rate, and electrical parameters on the desulfurization in ESR are assessed.The interrelation between desulfurization and sulfide inclusion evolution during ESR is discussed, and advancements in the production of sulfur-bearing steel at a high-sulfur level during ESR are described.The remaining challenges for future work are also proposed.展开更多
A series of functional,tungsten-containing mesoporous silica materials（W-SiO2） have been fabricated directly from an ionic liquid that contained imidazole and polyoxometalate,which acted as mesoporous template and m...A series of functional,tungsten-containing mesoporous silica materials（W-SiO2） have been fabricated directly from an ionic liquid that contained imidazole and polyoxometalate,which acted as mesoporous template and metal source respectively.These materials were then characterized through X-ray diffraction（XRD）,transmission electron microscopy（TEM）,Raman spectroscopy,Fourier transform infrared spectra（FTIR）,diffuse reflectance spectra（DRS）,and N2 adsorption-desorption,which were found to contain tungsten species that were effectively dispersed throughout the structure.The as-prepared materials W-SiO2 were also found to possess a mesoporous structure.The pore diameters of the respective sample W-SiO2-20 determined from the TEM images ranged from 2 to 4 nm,which was close to the average pore size determined from the nitrogen desorption isotherm（2.9 nm）.The materials were evaluated as catalysts for the heterogeneous oxidative desulfurization of dibenzothiophene（DBT）,which is able to achieve deep desulfurization within 40 min under the optimal conditions（Catalyst（W-SiO2-20）= 0.01 g,temperature = 60℃,oxidant（H2O2）= 20 μL）.For the removal of different organic sulfur compounds within oil,the ability of the catalyst（W-SiO2-20） under the same conditions to remove sulfur compounds decreased in the order：4,6-dimethyldibenzothiophene Dibenzothiophene Benzothiophene 1-dodecanethiol.Additionally,they did not require organic solvents as an extractant in the heterogeneous oxidative desulfurization process.After seven separate catalytic cycles,the desulfurization efficiency was still as high as 90.3%.From the gas chromatography-mass spectrometer analysis,DBT was entirely oxidized to its corresponding sulfone DBTO2 after reaction.A mechanism for the heterogeneous desulfurization reaction was proposed.展开更多
A highly active catalyst of phosphomolybdic acid ~HPMo） was prepared and applied in the catalytic oxidative desulfurization （CODS） system. The catalyst was characterized by FT-IR, XRD, XPS and superconducting NMR. ...A highly active catalyst of phosphomolybdic acid ~HPMo） was prepared and applied in the catalytic oxidative desulfurization （CODS） system. The catalyst was characterized by FT-IR, XRD, XPS and superconducting NMR. The influences of rn（catalyst）/m（oil）, V（H202）fV（oil）, reaction temperature and reaction time on the fractional conversion of benzothiophene （BT） and dibenzothiophene （DBT） were investigated. GC-MS and micra-coulometric methods were employed to investigate the reaction. The catalyst has high desulfurization activity in the removal of BT and DBT under mild conditions. The recycling experiments indicated that DBT and BT removal could still reach 95.2% and 95.7% after 10 cycles.展开更多
Sulfur in transportation fuels is a major source of air pollution. New strategies for the desulfurization of fuels have been explored to meet the urgent need to produce cleaner gasoline. Adsorptive desulfurization（AD...Sulfur in transportation fuels is a major source of air pollution. New strategies for the desulfurization of fuels have been explored to meet the urgent need to produce cleaner gasoline. Adsorptive desulfurization（ADS） is one of the most promising complementary and alternative methods. Herein,nanocrystalline ferrite adsorbents were synthesized from metal nitrates and urea using a microwave assisted combustion method. A series of ADS experiments were performed using a fixed‐bed reactor to evaluate the ADS reactivity over the ferrites, which was found to have the order MgFe2O4〉NiFe2O4〉CuZnFe2O4〉ZnFe2O4〉CoFe2O4. This effect is explained by the fact that the low degree of alloying of Mg‐Fe and the doped Mg increased the interaction between Fe and S compounds,leading to a significant improvement in the desulfurization capability of the adsorbent.Additionally, Mg can dramatically promote the decomposition of thiophene. X‐ray diffraction and Mosbauer spectroscopy were used to characterize the fresh, regenerated, and sulfided adsorbents.Although the ferrite adsorbents were partially sulfided to bimetallic sulfides during the adsorption process, they were successfully regenerated after calcining at 500 °C in air.展开更多
Application of particle image velocity (PIV) techniques for measuringparticle size distribution and total number in an activation chamber of desulfurization system isintroduced. Watersheld algorithm is used to choose ...Application of particle image velocity (PIV) techniques for measuringparticle size distribution and total number in an activation chamber of desulfurization system isintroduced. Watersheld algorithm is used to choose the suitable initial gray level threshold whichis used to change the gray level images taken by PIV to black and white ones, then every particle inan image is isolated totally. For every isolating particle, its contour is tracked by the edgeenhancement filter function and kept by Freeman s chain code. Based on a set of particle s chincode, its size and size distribution are calculated and sorted. Finally, the experimental data ofcalcium particles and water drops, separately injected into the activation chamber, and the erroranalysis of data are given out.展开更多
Zn-based sorbent （Z20SC） prepared through semi-coke support in 20 wt% zinc nitrate solution by high-pressure impregnation presents an excellent desulfurization capacity in hot coal gas,in which H2 S can not be nearl...Zn-based sorbent （Z20SC） prepared through semi-coke support in 20 wt% zinc nitrate solution by high-pressure impregnation presents an excellent desulfurization capacity in hot coal gas,in which H2 S can not be nearly detected in the outlet gas before 20 h breakthrough time.The effects of the main operational conditions and the particle size of Z20SC sorbent on its desulfurization performances sorbent were investigated in a fixed-bed reactor and the desulfurization kinetics of Z20SC sorbent removing H2 S from hot coal gas was calculated based on experimental data.Results showed that the conversion of Z20SC sorbent desulfurization reaction increased with the decrease of the particle size of the sorbent and the increases of gas volumetric flow rate,reaction temperature and H 2 S content in inlet gas.Z20SC sorbent obtained from hydrothermal synthesis by high-pressure impregnation possessed much larger surface area and pore volume than semi-coke support,and they were significantly reduced after the desulfurization reaction.The equivalent grain model was reasonably used to analyze experimental data,in which k s=4.382×10-3 exp（-8.270×103/RgT） and Dep=1.262×10-4exp（1.522×104/RgT）.It suggests that the desulfurization reaction of the Z20SC sorbent is mainly controlled by the chemical reaction in the initial stage and later by the diffusion through the reacted sorbent layer.展开更多
Calcium-based desulfurization ash(CDA)is mainly produced in dry and semi-dry flue gas desulfurization processes.The property of CDA is extremely unstable because its main component,calcium sulfite,makes it difficult t...Calcium-based desulfurization ash(CDA)is mainly produced in dry and semi-dry flue gas desulfurization processes.The property of CDA is extremely unstable because its main component,calcium sulfite,makes it difficult to be directly applied to the field of building materials.The modification of desulfurization ash can be realized by high-temperature oxidation and wet oxidation.After modification,CDA can be widely used in building materials.Hydrothermal oxidation has broad development prospects because it can complete the oxidation of CDA and the removal of impurity elements at the same time.CDA can be used to prepare high value-added products of calcium sulfate whiskers and ecological rubber fillers.展开更多
Vortexing limestone injection into furnace combined with calcium lime hydration in the downstream is the most promising technology for controlling SO 2 emission. Particle imaging velocimetry (PIV) is used to measure ...Vortexing limestone injection into furnace combined with calcium lime hydration in the downstream is the most promising technology for controlling SO 2 emission. Particle imaging velocimetry (PIV) is used to measure the gas liquid solid three phase flow field in a reactor. By image processing based on newly developed software, the number concentrations of sorbent particles and water droplets are presented. The measuring results are very helpful for better understanding the desulfurization mechanism and optimizing configurational and operational parameters in the hydration reactor.展开更多
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.
基金supported by the National Key Research and Development Program of China(2022YFC2904400)Guangxi Science and Technology Major Project(Gui Ke AA23023033)。
文摘As a pyrometallurgical process,circulating fluidized bed(CFB) roasting has good potential for application in desulfurization of high-sulfur bauxite.The gas-solid distribution and reaction during CFB roasting of high-sulfur bauxite were simulated using the computational particle fluid dynamics(CPFD) method.The effect of primary air flow velocity on particle velocity,particle volume distribution,furnace temperature distribution and pressure distribution were investigated.Under the condition of the same total flow of natural gas,the impact of the number of inlets on the desulfurization efficiency,atmosphere mass fraction distribution and temperature distribution in the furnace was further investigated.
基金support provided by South Africa National Research Foundation(UID 95983,113648,137947)Foundation for Innovative Research Groups of the Natural Science Foundation of Hebei Province(no.B2021208005).
文摘The development of highly active functionalized ionic liquids(ILs)as both extractants and catalysts for use in achieving deep desulfurization continues to pose challenges.In this study,a highly efficient oxidative desulfurization system was constructed,composed of dual-acidic ionic liquids(DILs)and H_(2)O_(2)-AcOH.The investigation results of four DILs prepared from different metal chlorides([HSO_(3)C_(3)NEt_(3)]Cl-MnCl_(n),MnCl_(n)=AlCl_(3),ZnCl_(2),CuCl_(2),FeCl_(3))in oxidative desulfurization showed that[HSO_(3)C_(3)NEt_(3)]Cl-AlCl_(3)had an outstanding catalytic effect and significantly promoted the oxidation of sulfides.With a 0.2 g[HSO_(3)C_(3)NEt_(3)]Cl-AlCl_(3),the removal rate of dibenzothiophene(DBT)reached 100%in 10 mL model oil under mild conditions at 55℃for 20 min.The key is its ability to induce the dismutation of su-peroxide anions(·O_(2)^(-)),which facilitates the generation of singlet oxygen(1 O_(2)).The efficient oxidation of DBT is accomplished through a predominantly^(1)O_(2)-mediated_(n)on-radical mechanism.[HSO_(3)C_(3)NEt_(3)]Cl-AlCl_(3)serves as a favorable medium for contact to be made between^(1)O_(2)and sulfides,which indicates an efficient catalytic-adsorption synergy.
基金The National Natural Science Foundation of China(No.51978504).
文摘Practical applications of desulfurization gypsum are limited owing to its brittleness and low strength.To overcome these challenges,researchers have developed engineered desulfurization gypsum composites(EDGCs)by incorporating ultrahigh molecular weight polyethylene(UHMWPE)fiber and sulfoaluminate cement(SAC).The mix ratio was optimized using response surface methodology(RSM).Experimental testing of EDGC under compressive and tensile loads led to the creation of a regression model that investigates the influence of variables and their interactions on the material’s compressive and tensile strengths.Additionally,microscopic morphology and hydration product composition were analyzed to explore the influence mechanism.The results indicated that EDGC’s compressive strength increased by up to 38.4%owing to a decreased water-binder ratio and higher SAC content.Similarly,tensile strength increased by up to 38.6%owing to increased SAC and fiber content.Moreover,EDGC demonstrated excellent strain-hardening behavior and multiple cracking characteristics,achieving a maximum tensile strain of nearly 3%.The research findings provide valuable insights for optimizing the performance of desulfurization gypsum.
基金supported by the National Key Research and Development Program of China(2022YFA1504402)National Energy R&D Center of Petroleum Refining Technology(RIPP,SINOPEC)+2 种基金the National Natural Science Foundation of China(22472016 and U23B20169)Key R&D Program of Ningbo(No.2023Z144)the Fundamental Research Funds for the Central Universities(DUT22LAB601).
文摘Desulfurization technology is rather difficult and urgently needed for carbon dioxide(CO_(2))utilization in industry.A new Cu(I)-based adsorbent was synthesized and examined for the capacity of removing carbonyl sulfide(COS)from a CO_(2)stream in an effort to solve the competitive adsorption between CO_(2)and COS and to seek opportunity to advance adsorption capacity.A wide range of character-ization techniques were used to investigate the physicochemical properties of the synthesized Cu(I)adsorbent featuringπ-complexation and their correlations with the adsorption performance.Meanwhile,the first principal calculation software CP2K was used to develop an understanding of the adsorption mechanism,which can offer useful guidance for the adsorbent regeneration.The synthesized Cu(I)adsorbent,prepared by using copper citrate and citric acid on the ZSM-5(SiO_(2)/Al_(2)O_(3)=25)carrier,outperformed other adsorbents with varying formulations and carriers in adsorption capacities.Through optimization of the preparation and adsorption conditions for various adsorbents,the breakthrough adsorption capacity(Qb)for COS was further enhanced from 2.19 mg/g to 15.36 mg/g.The formed stableπ-complex bonds between COS and Cu(I),as confirmed by density func-tional theory calculations,were verified by the significant improvement in the adsorption capacity after regeneration at 600°C.The above advantages render the novel synthesized Cu(I)adsorbent a promising candidate featuring cost-effectiveness,high efficacy and good regenerability for desulfurization from a CO_(2)stream.
基金supports from National Natural Science Foundation of China(Nos.22172066,22378176)supported by State Key Laboratory of Heavy Oil Processing.Supported by Jiangsu Collaborative Innovation Center of TechnologyMaterial of Water Treatment,Suzhou University of Science and Technology.
文摘Development of clean desulfurization process that combines both efficient and environmentally friendly remains a significant challenge for diesel production.The photocatalytic oxidation desulfurization technology is regarded as a promising process depending on the superior electron transfer and visible light utilization of photocatalyst.Herein,the nonstoichiometry MoO_(3-x)with outstanding photoresponse ability is prepared and modified by imidazole-based ionic liquid[C_(12)mim]Cl to upgrade electronic structure.The interface H-bonding between MoO_(3-x)and[C_(12)mim]Cl regard as electronic transfer channel and the recombination of e^(-)-h^(+)pairs is effectively inhibited with the modification of[C_(12)mim]Cl.Deep desulfurization rate of 96.6%can be reached within 60 min and the MoO_(3-x)/[C_(12)mim]Cl(MoC_(12))photocatalyst demonstrated outstanding cyclic stability within 7 cycles in an extraction coupled photocatalytic oxidation desulfurization(ECPODS)system.The study provides a new perspective on enhancing photocatalytic desulfurization through defect engineering and surface modification.
文摘For the treatment of the mixed flue gas desulfurization wastewater with high salinity by the biological fluidized bed process,the optimum temperature was 25-35℃,and the optimum hydraulic retention time was 10 h.When the influent quality was stable,the average concentration of COD,NH_(4)^(+)-N and TN in the inlet water was 210,11 and 16.3 mg/L,respectively,and their average concentration in the effluent was 54,0.32 and 4.09 mg/L,respectively.The treatment effect was good.When the incoming water quality of flue gas desulfurization wastewater fluctuated greatly,the effluent quality was still relatively stable after being treated by the biological fluidized bed,indicating that the biological fluidized bed process had a good ability to resist the impact of water quality in the treatment of high-salinity flue gas desulfurization wastewater.At the same time,the biological fluidized bed process provides a reference for high-salinity wastewater that is difficult to be biologically treated.
基金support from the National Key R&D Program(No.2023YFB3709901)the National Natural Science Foundation of China(Grant No.U22A20171)China Baowu Low Carbon Metallurgy Innovation Foundation(BWLCF202315).
文摘The instantaneous desulfurization of CaO-Al_(2)O_(3)-SiO_(2)slag particles in the molten steel was in situ observed using a high-temperature confocal scanning laser microscope.The desulfurization effect of CaO-Al_(2)O_(3)-SiO_(2)slags with different compositions was discussed.The influence of CaO/Al_(2)O_(3)and CaO/SiO_(2)on the desulfurization effect was analyzed.It was shown that in the liquid phase range,the higher CaO/SiO_(2)and CaO/Al_(2)O_(3)can significantly improve the desulfurization effect of the slag.A dimensionless desulfurization index Sindex was introduced to evaluate the desulfurization ability of CaO-Al_(2)O_(3)-SiO_(2)slags quantitatively.The Sindex values of CaO-Al_(2)O_(3)-SiO_(2)with different compositions at 1550°C were calculated.It was suggested to use(65%-75%)CaO-(0-20%)SiO_(2)-(20%-40%)Al_(2)O_(3)slags to improve the molten steel desulfurization.
基金financially supported by the National Natural Science Foundation of China (Nos.51874026 and 52074027)the Fundamental Research Funds for the Central Universities (No.FRF-TP-18-004A3)the State Key Laboratory of Advanced Metallurgy of China (No.41619019)。
文摘Electroslag remelting(ESR) gives a combination of liquid metal refining and solidification structure control.One of the typical aspects of liquid metal refining during ESR for the advanced steel and alloy production is desulfurization.It involves two patterns, i.e., slag–metal reaction and gas–slag reaction(gasifying desulfurization).In this paper, the advances in desulfurization practices of ESR are reviewed.The effects of processing parameters, including the initial sulfur level of consumable electrode, remelting atmosphere, deoxidation schemes of ESR,slag composition, melting rate, and electrical parameters on the desulfurization in ESR are assessed.The interrelation between desulfurization and sulfide inclusion evolution during ESR is discussed, and advancements in the production of sulfur-bearing steel at a high-sulfur level during ESR are described.The remaining challenges for future work are also proposed.
基金supported by the National Nature Science Foundation of China(21276117,21376111,21406092)~~
文摘A series of functional,tungsten-containing mesoporous silica materials（W-SiO2） have been fabricated directly from an ionic liquid that contained imidazole and polyoxometalate,which acted as mesoporous template and metal source respectively.These materials were then characterized through X-ray diffraction（XRD）,transmission electron microscopy（TEM）,Raman spectroscopy,Fourier transform infrared spectra（FTIR）,diffuse reflectance spectra（DRS）,and N2 adsorption-desorption,which were found to contain tungsten species that were effectively dispersed throughout the structure.The as-prepared materials W-SiO2 were also found to possess a mesoporous structure.The pore diameters of the respective sample W-SiO2-20 determined from the TEM images ranged from 2 to 4 nm,which was close to the average pore size determined from the nitrogen desorption isotherm（2.9 nm）.The materials were evaluated as catalysts for the heterogeneous oxidative desulfurization of dibenzothiophene（DBT）,which is able to achieve deep desulfurization within 40 min under the optimal conditions（Catalyst（W-SiO2-20）= 0.01 g,temperature = 60℃,oxidant（H2O2）= 20 μL）.For the removal of different organic sulfur compounds within oil,the ability of the catalyst（W-SiO2-20） under the same conditions to remove sulfur compounds decreased in the order：4,6-dimethyldibenzothiophene Dibenzothiophene Benzothiophene 1-dodecanethiol.Additionally,they did not require organic solvents as an extractant in the heterogeneous oxidative desulfurization process.After seven separate catalytic cycles,the desulfurization efficiency was still as high as 90.3%.From the gas chromatography-mass spectrometer analysis,DBT was entirely oxidized to its corresponding sulfone DBTO2 after reaction.A mechanism for the heterogeneous desulfurization reaction was proposed.
基金supported by the National Natural Science Foundation of China (21473126)~~
文摘A highly active catalyst of phosphomolybdic acid ~HPMo） was prepared and applied in the catalytic oxidative desulfurization （CODS） system. The catalyst was characterized by FT-IR, XRD, XPS and superconducting NMR. The influences of rn（catalyst）/m（oil）, V（H202）fV（oil）, reaction temperature and reaction time on the fractional conversion of benzothiophene （BT） and dibenzothiophene （DBT） were investigated. GC-MS and micra-coulometric methods were employed to investigate the reaction. The catalyst has high desulfurization activity in the removal of BT and DBT under mild conditions. The recycling experiments indicated that DBT and BT removal could still reach 95.2% and 95.7% after 10 cycles.
基金supported by the National Natural Science Foundation of China(2137303821403026+2 种基金and 21476232)the China Postdoctoral Science Foundation(2015T80255 and 2014M551068)the China-Egypt Scientific-Technologic Exchange Project(21311140474)~~
文摘Sulfur in transportation fuels is a major source of air pollution. New strategies for the desulfurization of fuels have been explored to meet the urgent need to produce cleaner gasoline. Adsorptive desulfurization（ADS） is one of the most promising complementary and alternative methods. Herein,nanocrystalline ferrite adsorbents were synthesized from metal nitrates and urea using a microwave assisted combustion method. A series of ADS experiments were performed using a fixed‐bed reactor to evaluate the ADS reactivity over the ferrites, which was found to have the order MgFe2O4〉NiFe2O4〉CuZnFe2O4〉ZnFe2O4〉CoFe2O4. This effect is explained by the fact that the low degree of alloying of Mg‐Fe and the doped Mg increased the interaction between Fe and S compounds,leading to a significant improvement in the desulfurization capability of the adsorbent.Additionally, Mg can dramatically promote the decomposition of thiophene. X‐ray diffraction and Mosbauer spectroscopy were used to characterize the fresh, regenerated, and sulfided adsorbents.Although the ferrite adsorbents were partially sulfided to bimetallic sulfides during the adsorption process, they were successfully regenerated after calcining at 500 °C in air.
基金The Special Funds for State Key Projects for Fun- damental Research (G1999022201-04).
文摘Application of particle image velocity (PIV) techniques for measuringparticle size distribution and total number in an activation chamber of desulfurization system isintroduced. Watersheld algorithm is used to choose the suitable initial gray level threshold whichis used to change the gray level images taken by PIV to black and white ones, then every particle inan image is isolated totally. For every isolating particle, its contour is tracked by the edgeenhancement filter function and kept by Freeman s chain code. Based on a set of particle s chincode, its size and size distribution are calculated and sorted. Finally, the experimental data ofcalcium particles and water drops, separately injected into the activation chamber, and the erroranalysis of data are given out.
基金supported by the National Basic Research Program of China (2012CB723105)the National Natural Science Foundation of China(20976117)+1 种基金Shanxi Province Natural Science Foundation (2010011014-3)Shanxi Province Basic Conditions Platform for Science and Technology Project(2010091015)
文摘Zn-based sorbent （Z20SC） prepared through semi-coke support in 20 wt% zinc nitrate solution by high-pressure impregnation presents an excellent desulfurization capacity in hot coal gas,in which H2 S can not be nearly detected in the outlet gas before 20 h breakthrough time.The effects of the main operational conditions and the particle size of Z20SC sorbent on its desulfurization performances sorbent were investigated in a fixed-bed reactor and the desulfurization kinetics of Z20SC sorbent removing H2 S from hot coal gas was calculated based on experimental data.Results showed that the conversion of Z20SC sorbent desulfurization reaction increased with the decrease of the particle size of the sorbent and the increases of gas volumetric flow rate,reaction temperature and H 2 S content in inlet gas.Z20SC sorbent obtained from hydrothermal synthesis by high-pressure impregnation possessed much larger surface area and pore volume than semi-coke support,and they were significantly reduced after the desulfurization reaction.The equivalent grain model was reasonably used to analyze experimental data,in which k s=4.382×10-3 exp（-8.270×103/RgT） and Dep=1.262×10-4exp（1.522×104/RgT）.It suggests that the desulfurization reaction of the Z20SC sorbent is mainly controlled by the chemical reaction in the initial stage and later by the diffusion through the reacted sorbent layer.
基金supported by the National Natural Science Foundation of China(Grant No.51704004).
文摘Calcium-based desulfurization ash(CDA)is mainly produced in dry and semi-dry flue gas desulfurization processes.The property of CDA is extremely unstable because its main component,calcium sulfite,makes it difficult to be directly applied to the field of building materials.The modification of desulfurization ash can be realized by high-temperature oxidation and wet oxidation.After modification,CDA can be widely used in building materials.Hydrothermal oxidation has broad development prospects because it can complete the oxidation of CDA and the removal of impurity elements at the same time.CDA can be used to prepare high value-added products of calcium sulfate whiskers and ecological rubber fillers.
文摘Vortexing limestone injection into furnace combined with calcium lime hydration in the downstream is the most promising technology for controlling SO 2 emission. Particle imaging velocimetry (PIV) is used to measure the gas liquid solid three phase flow field in a reactor. By image processing based on newly developed software, the number concentrations of sorbent particles and water droplets are presented. The measuring results are very helpful for better understanding the desulfurization mechanism and optimizing configurational and operational parameters in the hydration reactor.
