To address the challenges of high energy consumption and prominent costs in the traditional three-columns distillation process for cellulosic fuel ethanol,a distillation–molecular sieve coupling separation process is...To address the challenges of high energy consumption and prominent costs in the traditional three-columns distillation process for cellulosic fuel ethanol,a distillation–molecular sieve coupling separation process is proposed.This process integrates a three-column(crude distillation column,first distillation column,second distillation column)system with a 3A molecular sieve adsorption deep dehydration unit.A thermal coupling network is constructed via differential pressure design(steam from medium/high-pressure columns as mutual heat sources,reboiler liquid waste heat for feed preheating),and molecular sieve adsorption conditions are optimized.The study first performs a thermodynamic consistency test on the ethanol–water system,determines optimal non-random two-liquid(NRTL)model binary interaction parameters via experimental data regression for Aspen Plus simulation.Aiming at minimum total annual cost(TAC),Aspen Plus is used to optimize process parameters(theoretical tray number,feed location,reflux ratio,side-draw position,etc.).Economic analysis shows this process reduces CO_(2) emission costs by 27.56%,TAC by 15.58%(to 5.123×10^(6) USD·a^(−1)),and increases ethanol purity to>99.6%,providing an effective solution for green,efficient separation.展开更多
N,N,N',N'-tetraoctyl diglycolamide(TODGA)is a potential extractant for the co-extraction of lanthanides and actinides in high-level liquid waste.In this study,the radiolysis and extraction properties of TODGA ...N,N,N',N'-tetraoctyl diglycolamide(TODGA)is a potential extractant for the co-extraction of lanthanides and actinides in high-level liquid waste.In this study,the radiolysis and extraction properties of TODGA in kerosene solvents contacted with the aqueous phase of varying HNO_(3) concentrations were systematically investigated,and the complexation mechanism was analyzed in conjunction with density functional theory(DFT)calculations.After γ-irradiation,the variation of TODGA concentration was detected,and the variation trends in the relative content of radiolysis products(RPs)with sample type and absorbed dose were demonstrated.Results indicated that the breaking of the amide bond,ether bond,and C_(amide)-C_(ether)bond was the primary radiolysis routes.The aqueous-phase precipitate was studied as a potential new mode of TODGA radiolysis in ultrapure water aqueous phase.Moreover,TODGA/kerosene exhibited excellent extraction capabilities for lanthanides even after absorbing 100 kGy,and HNO_(3) can maintain a portion of TODGA's extraction capacity.The DFT method was applied to calculate and evaluate the complexing ability of TODGA and some of its RPs toward lanthanides.The results revealed that the complexing ability of TODGA for Ce(Ⅲ),Eu(Ⅲ),and Dy(Ⅲ)was enhanced successively,and the complexing ability of the RPs with intact oxygen-containing structures could not be neglected.展开更多
The liquid-only transfer dividing wall column(LDWC)offers a promising path for industrializing dividing wall columns by simplifying vapor split control.However,their energy efficiency is insufficient due to the additi...The liquid-only transfer dividing wall column(LDWC)offers a promising path for industrializing dividing wall columns by simplifying vapor split control.However,their energy efficiency is insufficient due to the addition of heat at the bottom and its removal at the top.Therefore,developing an effective strategy to enhance the energy efficiency of the entire LDWC system is crucial.This work investigates the intensification of LDWC based on the column grand composite curve(CGCC)and thermodynamic analysis,proposing a novel intensification strategy to improve energy efficiency effectively.An optimization model with four blocks is developed to minimize the total annual cost(TAC)of the intensified LDWC.Energy,exergy,economic,and environmental analyses are used to evaluate its performance.Ternary mixtures with different easy separation indexes(ESI)are selected as illustrative examples.For mixtures with ESI≤1,the optimal configuration involves partial feed preheating,compressors and intermediate reboilers on both side sections,along with optimized operating pressure.This setup leads to significant reductions in total energy consumption,TAC,and gas emissions by 43.80%,28.08%,and 42.85%for ESI=1,and by 46.17%,29.06%,and 45.35%for ESI<1,respectively,when compared to conventional distillation sequences(CDS).For mixtures with ESI>1,the best performance is achieved by implementing partial feed preheating and modifications only to the right section.This results in reductions of 21.64%in energy consumption,16.26%in TAC,and 21.51%in gas emissions when compared to CDS.In all cases,the optimal configurations show the lowest lost work and minimum work,indicating an improved thermodynamic performance.展开更多
The volatilization characteristics and kinetic mechanisms of arsenic were investigated in the temperature range of 623−773 K and pressure ranges of 10−10000 Pa.The experimental results reveal that the evaporation rate...The volatilization characteristics and kinetic mechanisms of arsenic were investigated in the temperature range of 623−773 K and pressure ranges of 10−10000 Pa.The experimental results reveal that the evaporation rate increases with increasing temperature and decreasing pressure.Surface reaction control dominates at low pressures(<100 Pa),whereas diffusion control dominates at high pressures(>5000 Pa).The evaporation behavior is successfully described by an Arrhenius-type model for temperature dependence and Logistic model for pressure dependence.Key kinetic parameters,including the critical pressure,maximum evaporation rate and evaporation coefficient,were calculated.The evaporation coefficient varies between 0.010 and 0.223,and the critical pressures vary between 281 and 478 Pa with temperature.展开更多
Understanding the underlying mechanism that enhances the separation of specific target ions from complex background aqueous solutions is crucial for achieving controllable chemical reactions and industrial purificatio...Understanding the underlying mechanism that enhances the separation of specific target ions from complex background aqueous solutions is crucial for achieving controllable chemical reactions and industrial purification processes in modern industries.This study investigated the enhanced kinetic separatio n of target metal ions from complex aqueous solutio ns at a liquid-liquid interface,focusing on the presence of coexisting salt cations.Employing a typical thin-layer organic oil film(TOOF)extraction as a model system,the research examines how background Al^(3+)ions influence the mass transfer and separation of ions.Notably,the co ncentration of Al^(3+)ions affects both the distribution of Er^(3+)ions at the oil-water interface and the arrangement and orientation of P507 extractant molecules through the formation of unique hydrogen-bonding interactions.These interactions influence the selectivity of mass transfer,facilitating the separation of Er^(3+)from Al^(3+)ions.Specifically,the hydration shell of Er^(3+)ions is disrupted due to the strong hydration capability of coexisting Al^(3+)ions,leading to a higher interfacial concentration of Er^(3+)ions and a more ordered interfacial orientation of P507 molecules.At lower concentrations of Al^(3+)ions,the diffusion rate of Er^(3+)ions near the interface is high,enhancing the sepa ration perfo rmance of these ions.In contrast,at higher concentrations of Al^(3+)ions,the competitive hydration by Al^(3+)ions increases,and the interfacial concentration of Er^(3+)ions decreases due to enhanced diffusion resistance,resulting in poorer separation performance.Furthermore,a thinner membrane is more effective than a thicker one in enriching target Er^(3+)ions at the interface and achieving an ordered interfacial orientation of P507 molecules,thereby enhancing the separation coefficient(β_(Er/Al)).This work provides novel insights into the behaviors of ions and extractants at oil-wate r interface and the kinetic separation selectivity under varying concentrations of coexisting salt cations.展开更多
基金support from the National Key Research and Development Program of China(2022YFC2106300)the National Natural Science Foundation of China(42177400).
文摘To address the challenges of high energy consumption and prominent costs in the traditional three-columns distillation process for cellulosic fuel ethanol,a distillation–molecular sieve coupling separation process is proposed.This process integrates a three-column(crude distillation column,first distillation column,second distillation column)system with a 3A molecular sieve adsorption deep dehydration unit.A thermal coupling network is constructed via differential pressure design(steam from medium/high-pressure columns as mutual heat sources,reboiler liquid waste heat for feed preheating),and molecular sieve adsorption conditions are optimized.The study first performs a thermodynamic consistency test on the ethanol–water system,determines optimal non-random two-liquid(NRTL)model binary interaction parameters via experimental data regression for Aspen Plus simulation.Aiming at minimum total annual cost(TAC),Aspen Plus is used to optimize process parameters(theoretical tray number,feed location,reflux ratio,side-draw position,etc.).Economic analysis shows this process reduces CO_(2) emission costs by 27.56%,TAC by 15.58%(to 5.123×10^(6) USD·a^(−1)),and increases ethanol purity to>99.6%,providing an effective solution for green,efficient separation.
文摘N,N,N',N'-tetraoctyl diglycolamide(TODGA)is a potential extractant for the co-extraction of lanthanides and actinides in high-level liquid waste.In this study,the radiolysis and extraction properties of TODGA in kerosene solvents contacted with the aqueous phase of varying HNO_(3) concentrations were systematically investigated,and the complexation mechanism was analyzed in conjunction with density functional theory(DFT)calculations.After γ-irradiation,the variation of TODGA concentration was detected,and the variation trends in the relative content of radiolysis products(RPs)with sample type and absorbed dose were demonstrated.Results indicated that the breaking of the amide bond,ether bond,and C_(amide)-C_(ether)bond was the primary radiolysis routes.The aqueous-phase precipitate was studied as a potential new mode of TODGA radiolysis in ultrapure water aqueous phase.Moreover,TODGA/kerosene exhibited excellent extraction capabilities for lanthanides even after absorbing 100 kGy,and HNO_(3) can maintain a portion of TODGA's extraction capacity.The DFT method was applied to calculate and evaluate the complexing ability of TODGA and some of its RPs toward lanthanides.The results revealed that the complexing ability of TODGA for Ce(Ⅲ),Eu(Ⅲ),and Dy(Ⅲ)was enhanced successively,and the complexing ability of the RPs with intact oxygen-containing structures could not be neglected.
基金support provided by the National Natural Science Foundation of China(U24B6016)the Higher Education Institution Academic Discipline Innovation and Talent Introduction Plan(“111 Plan”)(No.B23025)are gratefully acknowledged.
文摘The liquid-only transfer dividing wall column(LDWC)offers a promising path for industrializing dividing wall columns by simplifying vapor split control.However,their energy efficiency is insufficient due to the addition of heat at the bottom and its removal at the top.Therefore,developing an effective strategy to enhance the energy efficiency of the entire LDWC system is crucial.This work investigates the intensification of LDWC based on the column grand composite curve(CGCC)and thermodynamic analysis,proposing a novel intensification strategy to improve energy efficiency effectively.An optimization model with four blocks is developed to minimize the total annual cost(TAC)of the intensified LDWC.Energy,exergy,economic,and environmental analyses are used to evaluate its performance.Ternary mixtures with different easy separation indexes(ESI)are selected as illustrative examples.For mixtures with ESI≤1,the optimal configuration involves partial feed preheating,compressors and intermediate reboilers on both side sections,along with optimized operating pressure.This setup leads to significant reductions in total energy consumption,TAC,and gas emissions by 43.80%,28.08%,and 42.85%for ESI=1,and by 46.17%,29.06%,and 45.35%for ESI<1,respectively,when compared to conventional distillation sequences(CDS).For mixtures with ESI>1,the best performance is achieved by implementing partial feed preheating and modifications only to the right section.This results in reductions of 21.64%in energy consumption,16.26%in TAC,and 21.51%in gas emissions when compared to CDS.In all cases,the optimal configurations show the lowest lost work and minimum work,indicating an improved thermodynamic performance.
基金Yunnan Fundamental Research Project,China(No.202201BE070001-056)。
文摘The volatilization characteristics and kinetic mechanisms of arsenic were investigated in the temperature range of 623−773 K and pressure ranges of 10−10000 Pa.The experimental results reveal that the evaporation rate increases with increasing temperature and decreasing pressure.Surface reaction control dominates at low pressures(<100 Pa),whereas diffusion control dominates at high pressures(>5000 Pa).The evaporation behavior is successfully described by an Arrhenius-type model for temperature dependence and Logistic model for pressure dependence.Key kinetic parameters,including the critical pressure,maximum evaporation rate and evaporation coefficient,were calculated.The evaporation coefficient varies between 0.010 and 0.223,and the critical pressures vary between 281 and 478 Pa with temperature.
基金Project supported by the National Natural Science Foundation of China(52074031,51574213,51904027)the Fundamental Research Funds for the Central Universities of China(06500104)。
文摘Understanding the underlying mechanism that enhances the separation of specific target ions from complex background aqueous solutions is crucial for achieving controllable chemical reactions and industrial purification processes in modern industries.This study investigated the enhanced kinetic separatio n of target metal ions from complex aqueous solutio ns at a liquid-liquid interface,focusing on the presence of coexisting salt cations.Employing a typical thin-layer organic oil film(TOOF)extraction as a model system,the research examines how background Al^(3+)ions influence the mass transfer and separation of ions.Notably,the co ncentration of Al^(3+)ions affects both the distribution of Er^(3+)ions at the oil-water interface and the arrangement and orientation of P507 extractant molecules through the formation of unique hydrogen-bonding interactions.These interactions influence the selectivity of mass transfer,facilitating the separation of Er^(3+)from Al^(3+)ions.Specifically,the hydration shell of Er^(3+)ions is disrupted due to the strong hydration capability of coexisting Al^(3+)ions,leading to a higher interfacial concentration of Er^(3+)ions and a more ordered interfacial orientation of P507 molecules.At lower concentrations of Al^(3+)ions,the diffusion rate of Er^(3+)ions near the interface is high,enhancing the sepa ration perfo rmance of these ions.In contrast,at higher concentrations of Al^(3+)ions,the competitive hydration by Al^(3+)ions increases,and the interfacial concentration of Er^(3+)ions decreases due to enhanced diffusion resistance,resulting in poorer separation performance.Furthermore,a thinner membrane is more effective than a thicker one in enriching target Er^(3+)ions at the interface and achieving an ordered interfacial orientation of P507 molecules,thereby enhancing the separation coefficient(β_(Er/Al)).This work provides novel insights into the behaviors of ions and extractants at oil-wate r interface and the kinetic separation selectivity under varying concentrations of coexisting salt cations.
