As a potential adsorption material,it is still a challenge for activated carbon fiber(ACF)in efficient adsorption of ethanol due to its nonpolar surface,which is mainly emitted from the grain drying industry.This stud...As a potential adsorption material,it is still a challenge for activated carbon fiber(ACF)in efficient adsorption of ethanol due to its nonpolar surface,which is mainly emitted from the grain drying industry.This study prepared surface polarity-modified ACF using the heteroatom doping method.The modified ACF possessed a richer array of strongly polar oxygen/nitrogen-containing functional groups(primarily phenolic hydroxyl and lactone groups),a larger specific surface are1,and a more developed micropore structure.The adsorption capacities of ethanol for O-ACF and N-ACF were 4.110 mmol/g and 1.698 mmol/g,respectively,which were 11.3 times and 4.7 times those of unmodified ACF.This was a significant improvement over our previous work(0.363 mmol/g).The improvement of adsorption capacity for the N-ACF was mainly due to the higher specific surface are1,greater number of micropores(more adsorption sites)and abundant existence of defects,whereas,for O-ACF,the improvement mainly relied on the abundant presence of oxygen-containing functional groups on the surface.However,water had a negative effect on the adsorption of ethanol for the modified ACF due to competitive adsorption and the disappearance of capillary condensation.It was further revealed that the adsorption process of ethanol and water was quite different.It obeyed the linear driving force(LDF)model for ethanol adsorption,however,the intraparticle diffusion(IPD)model for water adsorption.展开更多
The oxygen evolution reaction(OER)serves as a fundamental half–reaction in the electrolysis of water for hydrogen production,which is restricted by the sluggish OER reaction kinetics and unable to be practically appl...The oxygen evolution reaction(OER)serves as a fundamental half–reaction in the electrolysis of water for hydrogen production,which is restricted by the sluggish OER reaction kinetics and unable to be practically applied.The traditional lattice oxygen oxidation mechanism(LOM)offers an advantageous route by circumventing the formation of M-OOH^(*)in the adsorption evolution mechanism(AEM),thus enhancing the reaction kinetics of the OER but resulting in possible structural destabilization due to the decreased M–O bond order.Fortunately,the asymmetry of tetrahedral and octahedral sites in transition metal spinel oxides permits the existence of non-bonding oxygen,which could be activated by rational band structure design for direct O-O coupling,where the M–O bond maintains its initial bond order.Here,non-bonding oxygen was introduced into NiFe_(2)O_(4)via annealing in an oxygen-deficient atmosphere.Then,in-situ grown sulfate species on octahedral nickel sites significantly improved the reactivity of the non-bonding oxygen electrons,thereby facilitating the transformation of the redox center from metal to oxygen.LOM based on non-bonding oxygen(LOMNB)was successfully activated within NiFe_(2)O_(4),exhibiting a low overpotential of 206 mV to achieve a current density of 10 mA cm^(-2)and excellent durability of stable operation for over 150 h.Additionally,catalysts featuring varying band structures were synthesized for comparative analysis,and it was found that the reversible redox processes of non-bonding oxygen and the accumulation of non-bonding oxygen species containing 2p holes are critical prerequisites for triggering and sustaining the LOMNB pathway in transition metal spinel oxides.These findings may provide valuable insights for the future development of spinel-oxide-based LOM catalysts.展开更多
Poly(vinylidene fluoride-co-hexafluoropropylene)(PVDF-HFP)receives increasing attention in membrane separation field based on its advantages such as high mechanical strength,thermal and chemical stability.However,cont...Poly(vinylidene fluoride-co-hexafluoropropylene)(PVDF-HFP)receives increasing attention in membrane separation field based on its advantages such as high mechanical strength,thermal and chemical stability.However,controlling the microporous structure is still challenging.In this work,we attempted to tailor the morphology of PVDF-HFP membrane via a one-step reactive vapor induced phase separation method.Namely,PVDF-HFP was dissolved in a volatile solvent and then was cast in an ammonia water vapor atmosphere.After complete evaporation of solvent,membranes with adjustable porous structure were prepared,and the microstructures of the membranes were analyzed by scanning electron microscopy,Fourier transform infrared spectroscopy,X-ray photoelectron spectroscopy and X-ray diffraction characterizations.Based on the results,a mechanism of dehydrofluorination induced cross-linking of PVDF-HFP has been suggested to understand the morphology tailoring.To our knowledge,this is the first report of one-step reactive vapor induced phase separation strategy to tailor morphology of PVDF-HFP membrane.In addition,the membranes prepared in the ammonia water vapor exhibited enhanced mechanical strength and achieved satisfactory separation efficiency for water-in-oil emulsions,suggesting promising potential.展开更多
Ambient particulate matter(PM)can cause adverse health effects via their ability to produce Reactive Oxygen Species(ROS).Water-Soluble Organic Compounds(WSOCs),a complex mixture of organic compounds which usually coex...Ambient particulate matter(PM)can cause adverse health effects via their ability to produce Reactive Oxygen Species(ROS).Water-Soluble Organic Compounds(WSOCs),a complex mixture of organic compounds which usually coexist with Transition Metals(TMs)in PM,have been found to contribute to ROS formation.However,the interaction between WSOCs and TMs and its effect on ROS generation are still unknown.In this study,we examined the ROS concentrations of V,Zn,Suwannee River Fulvic Acid(SRFA),Suwannee River Humic Acid(SRHA)and the mixtures of V/Zn and SRFA/SRHA by using a cell-free 2’,7’-Dichlorodihydrofluorescein(DCFH)assay.The results showed that V or Zn synergistically promoted ROS generated by SRFA,but had an antagonistic effect on ROS generated by SRHA.Fluorescence quenching experiments indicated that V and Zn were more prone to form stable complexes with aromatic humic acid-like component(C1)and fulvic acidlike component(C3)in SRFA and SRHA.Results suggested that the underlying mechanism involving the fulvic acid-like component in SRFA more tending to complex with TMs to facilitate ROS generation throughπelectron transfer.Our work showed that the complexing ability and complexing stability of atmospheric PM organics with metals could significantly affect ROS generation.It is recommended that the research deploying multiple analytical methods to quantify the impact of PM components on public health and environment is needed in the future.展开更多
基金supported by the National Key R&D Program of China(Nos.2022YFB4101500 and 2022YFE0209500)the National Natural Science Foundation of China(Nos.22276191 and 21976177)the Qinghai Province Air Pollution Assessment and Fine Management Support Project,and the University of Chinese Academy of Science.
文摘As a potential adsorption material,it is still a challenge for activated carbon fiber(ACF)in efficient adsorption of ethanol due to its nonpolar surface,which is mainly emitted from the grain drying industry.This study prepared surface polarity-modified ACF using the heteroatom doping method.The modified ACF possessed a richer array of strongly polar oxygen/nitrogen-containing functional groups(primarily phenolic hydroxyl and lactone groups),a larger specific surface are1,and a more developed micropore structure.The adsorption capacities of ethanol for O-ACF and N-ACF were 4.110 mmol/g and 1.698 mmol/g,respectively,which were 11.3 times and 4.7 times those of unmodified ACF.This was a significant improvement over our previous work(0.363 mmol/g).The improvement of adsorption capacity for the N-ACF was mainly due to the higher specific surface are1,greater number of micropores(more adsorption sites)and abundant existence of defects,whereas,for O-ACF,the improvement mainly relied on the abundant presence of oxygen-containing functional groups on the surface.However,water had a negative effect on the adsorption of ethanol for the modified ACF due to competitive adsorption and the disappearance of capillary condensation.It was further revealed that the adsorption process of ethanol and water was quite different.It obeyed the linear driving force(LDF)model for ethanol adsorption,however,the intraparticle diffusion(IPD)model for water adsorption.
文摘The oxygen evolution reaction(OER)serves as a fundamental half–reaction in the electrolysis of water for hydrogen production,which is restricted by the sluggish OER reaction kinetics and unable to be practically applied.The traditional lattice oxygen oxidation mechanism(LOM)offers an advantageous route by circumventing the formation of M-OOH^(*)in the adsorption evolution mechanism(AEM),thus enhancing the reaction kinetics of the OER but resulting in possible structural destabilization due to the decreased M–O bond order.Fortunately,the asymmetry of tetrahedral and octahedral sites in transition metal spinel oxides permits the existence of non-bonding oxygen,which could be activated by rational band structure design for direct O-O coupling,where the M–O bond maintains its initial bond order.Here,non-bonding oxygen was introduced into NiFe_(2)O_(4)via annealing in an oxygen-deficient atmosphere.Then,in-situ grown sulfate species on octahedral nickel sites significantly improved the reactivity of the non-bonding oxygen electrons,thereby facilitating the transformation of the redox center from metal to oxygen.LOM based on non-bonding oxygen(LOMNB)was successfully activated within NiFe_(2)O_(4),exhibiting a low overpotential of 206 mV to achieve a current density of 10 mA cm^(-2)and excellent durability of stable operation for over 150 h.Additionally,catalysts featuring varying band structures were synthesized for comparative analysis,and it was found that the reversible redox processes of non-bonding oxygen and the accumulation of non-bonding oxygen species containing 2p holes are critical prerequisites for triggering and sustaining the LOMNB pathway in transition metal spinel oxides.These findings may provide valuable insights for the future development of spinel-oxide-based LOM catalysts.
基金supported by the Fundamental Research Funds for the Central Universities of China(No.20720200040)the National Natural Science Foundation of China(No.51273166).
文摘Poly(vinylidene fluoride-co-hexafluoropropylene)(PVDF-HFP)receives increasing attention in membrane separation field based on its advantages such as high mechanical strength,thermal and chemical stability.However,controlling the microporous structure is still challenging.In this work,we attempted to tailor the morphology of PVDF-HFP membrane via a one-step reactive vapor induced phase separation method.Namely,PVDF-HFP was dissolved in a volatile solvent and then was cast in an ammonia water vapor atmosphere.After complete evaporation of solvent,membranes with adjustable porous structure were prepared,and the microstructures of the membranes were analyzed by scanning electron microscopy,Fourier transform infrared spectroscopy,X-ray photoelectron spectroscopy and X-ray diffraction characterizations.Based on the results,a mechanism of dehydrofluorination induced cross-linking of PVDF-HFP has been suggested to understand the morphology tailoring.To our knowledge,this is the first report of one-step reactive vapor induced phase separation strategy to tailor morphology of PVDF-HFP membrane.In addition,the membranes prepared in the ammonia water vapor exhibited enhanced mechanical strength and achieved satisfactory separation efficiency for water-in-oil emulsions,suggesting promising potential.
基金supported by the Fundamental Research Funds for the Central Universities (No. E0E48927X2)the National Natural Science Foundation of China (No. 21677145)
文摘Ambient particulate matter(PM)can cause adverse health effects via their ability to produce Reactive Oxygen Species(ROS).Water-Soluble Organic Compounds(WSOCs),a complex mixture of organic compounds which usually coexist with Transition Metals(TMs)in PM,have been found to contribute to ROS formation.However,the interaction between WSOCs and TMs and its effect on ROS generation are still unknown.In this study,we examined the ROS concentrations of V,Zn,Suwannee River Fulvic Acid(SRFA),Suwannee River Humic Acid(SRHA)and the mixtures of V/Zn and SRFA/SRHA by using a cell-free 2’,7’-Dichlorodihydrofluorescein(DCFH)assay.The results showed that V or Zn synergistically promoted ROS generated by SRFA,but had an antagonistic effect on ROS generated by SRHA.Fluorescence quenching experiments indicated that V and Zn were more prone to form stable complexes with aromatic humic acid-like component(C1)and fulvic acidlike component(C3)in SRFA and SRHA.Results suggested that the underlying mechanism involving the fulvic acid-like component in SRFA more tending to complex with TMs to facilitate ROS generation throughπelectron transfer.Our work showed that the complexing ability and complexing stability of atmospheric PM organics with metals could significantly affect ROS generation.It is recommended that the research deploying multiple analytical methods to quantify the impact of PM components on public health and environment is needed in the future.
