Adsorption and photocatalysis are regarded as two desirable technologies for wastewater remediation,but are still unsatisfactory in removal effect,eco-friendly regeneration and facile reusability.In this study,we deve...Adsorption and photocatalysis are regarded as two desirable technologies for wastewater remediation,but are still unsatisfactory in removal effect,eco-friendly regeneration and facile reusability.In this study,we developed a composite nanofibrous membrane material with excellent removal performance for organic pollutants based on synergistic adsorption and photocatalysis.A novel boron-doped,nitrogen-deficient graphitic carbon nitride(B-C3N4)photocatalyst as well as an amphiphilic copolymer of methyl methacrylate and acrylic acid(p(MMA-AA))were synthesized respectively,and then used to modify polyethersulfone for the fabrication of composite nanofibrous membrane with improved hydrophilicity,negativelycharge property and enhanced visible light response simultaneously.Subsequently,the synergistic effect of adsorption and photocatalytic degradation for organic pollutants were identified especially and resulted in an excellent removal efficiency even superior to the combination of adsorption and photocatalytic degradation,which could be called a“1+1>2”effect.In addition,the regeneration and reusability,the purification ability for multicomponent wastewater,and the photocatalytic mechanism,were investigated and discussed systematically.In this work,we not only prepared the nanofibrous membrane with synergistic effect of adsorption and photocatalysis,but also provided a versatile approach to design dualfunctional support material to ensure the practical applications of powdery photocatalyst in wastewater treatment.展开更多
The protein-bound uremic toxins,represented by indoxyl sulfate(IS),have been associated with the progression of chronic kidney disease and the development of cardiovascular disease in the presence of impaired renal fu...The protein-bound uremic toxins,represented by indoxyl sulfate(IS),have been associated with the progression of chronic kidney disease and the development of cardiovascular disease in the presence of impaired renal function.Herein,we proposed a novel strategy of thin-film nanofibrous composite(TNFC)dialysis membrane combined with reduced graphene oxide(rGO)aerogel adsorbents for clinical removal of IS as well as high retention of proteins.The TFNC membrane was prepared by electrospinning in conjunction with coating-reaction method and proved to have good selectivity and permeability.To further improve the removal rate of toxins,we used a medium hydrothermal method following by freeze-drying treatment to obtain the r GO aerogel adsorbents.It exhibited excellent adsorption for IS with a maximum adsorption capacity of 69.40 mg·g^(-1)throughπ-πinteraction and hydrogen bonding interaction based on Langmuir isotherm models.Time-dependent absorption experiments showed that it reached adsorption equilibrium within 4 h,which was matched with the hemodialysis time.The coordination was significantly exhibited by introducing r GO aerogel blocks into the dialysate for absorbing the diffused free IS during hemodialysis.Taking the advantages of the TFNC dialysis membrane and the rGO aerogel,the volume of dialysate for hemodialysis was only one-tenth of that without adsorbent blocks but with very comparable dialysis performance(the clearance of IS at 51.8%and the retention of HSA over 98%),which could lighten conventional hemodialysis effectively and be benefit to realize the miniaturization of the hemodialysis equipment.Therefore,the coordination of the TFNC dialysis membrane and rGO aerogel adsorbents would open a new path for the development of portable artificial kidney.展开更多
A novel three-tier composite membrane based on highly porous nanofibrous substrate was demonstrated for efficient iso-propanol dehydration by pervaporation.Here,polyethyleneimine(PEI)modified graphene oxide(GO)sheets ...A novel three-tier composite membrane based on highly porous nanofibrous substrate was demonstrated for efficient iso-propanol dehydration by pervaporation.Here,polyethyleneimine(PEI)modified graphene oxide(GO)sheets were vacuum-assistant assembled onto porous electrospun polyacrylonitrile(PAN)nanofibrous substrate to achieve a smooth,hydrophilic and compact PEI-GO intermediate layer.The introduction of PEI chains endowed GO interlayer with sufficient interaction for bonding adjacent GO nanosheets to enhance stability in water/isopropanol mixture and also with the ascended inter-lamellar space to improve the water-sorption ability due to the abundant active amino groups.Benefiting from PEI-GO layer,a defect-free sodium alginate(SA)skin layer could be facilely manufactured with elaborately controlled thickness as thin as possible in order to reduce mass transfer resistant and enhance permeability maximally.Meanwhile,the interlayer would also contribute to enhance interfacial adhesion to promote the structure integrity of three-tier thin-film nanofibrous composite(TFNC)membrane in pervaporation dehydration process.After fine-tuning of membrane preparation process,the SA/PEI(75)-GO-60/PAN TFNC membrane exhibited competitive pervaporation performance with the permeate flux of 2009 g/m2 h and the separation factor of 1276 operated at 70°C for dehydration of 90 wt%isopropanol solution.The unique three-tier composite membrane structure suggested an effective and facile approach to design novel membrane structure for further improvement of pervaporation performance.展开更多
Metal-organic framework(MOF)/polymer composites have attracted extensive attention in the recent years.However,it still remains challenging to efficiently and effectively fabricate these composite materials.In this st...Metal-organic framework(MOF)/polymer composites have attracted extensive attention in the recent years.However,it still remains challenging to efficiently and effectively fabricate these composite materials.In this study,we propose a facile one-pot electrospinning strategy for preparation of HKUST-1/polyacrylonitrile(PAN)nanofibrous membranes from a homogeneous stock solution containing HKUST-1 precursors and PAN.MOF crystallization and polymer solidification occur simultaneously during the electrospinning process,thus avoiding the issues of aggregation and troublesome multistep fabrication of the conventional approach.The obtained HKUST-1/PAN electrospun membranes show uniform MOF distribution throughout the nanofibers and yield good mechanical properties.The membranes are used as separators in Li-metal full batteries under harsh testing conditions,using an ultrathin Li-metal anode,a high mass loading cathode,and the HKUST-1/PAN nanofibrous separator.The results demonstrate significantly improved cycling performance(capacity retention of 83.1%after 200 cycles)under a low negative to positive capacity ratio(N/P ratio of 1.86).The improvement can be attributed to an enhanced wettability of the separator towards electrolyte stemmed from the nanofibrous structure,and a uniform lithium ion flux stabilized by the open metal sites of uniformly distributed HKUST-1 particles in the membrane during cycling.展开更多
基金the National Natural Science Foundation of China(Nos.52003179 and 52073190)。
文摘Adsorption and photocatalysis are regarded as two desirable technologies for wastewater remediation,but are still unsatisfactory in removal effect,eco-friendly regeneration and facile reusability.In this study,we developed a composite nanofibrous membrane material with excellent removal performance for organic pollutants based on synergistic adsorption and photocatalysis.A novel boron-doped,nitrogen-deficient graphitic carbon nitride(B-C3N4)photocatalyst as well as an amphiphilic copolymer of methyl methacrylate and acrylic acid(p(MMA-AA))were synthesized respectively,and then used to modify polyethersulfone for the fabrication of composite nanofibrous membrane with improved hydrophilicity,negativelycharge property and enhanced visible light response simultaneously.Subsequently,the synergistic effect of adsorption and photocatalytic degradation for organic pollutants were identified especially and resulted in an excellent removal efficiency even superior to the combination of adsorption and photocatalytic degradation,which could be called a“1+1>2”effect.In addition,the regeneration and reusability,the purification ability for multicomponent wastewater,and the photocatalytic mechanism,were investigated and discussed systematically.In this work,we not only prepared the nanofibrous membrane with synergistic effect of adsorption and photocatalysis,but also provided a versatile approach to design dualfunctional support material to ensure the practical applications of powdery photocatalyst in wastewater treatment.
基金supported by the Fundamental Research Funds for the Central Universities(2232020A-04)Natural Science Foundation of Shanghai City(19ZR1401300)。
文摘The protein-bound uremic toxins,represented by indoxyl sulfate(IS),have been associated with the progression of chronic kidney disease and the development of cardiovascular disease in the presence of impaired renal function.Herein,we proposed a novel strategy of thin-film nanofibrous composite(TNFC)dialysis membrane combined with reduced graphene oxide(rGO)aerogel adsorbents for clinical removal of IS as well as high retention of proteins.The TFNC membrane was prepared by electrospinning in conjunction with coating-reaction method and proved to have good selectivity and permeability.To further improve the removal rate of toxins,we used a medium hydrothermal method following by freeze-drying treatment to obtain the r GO aerogel adsorbents.It exhibited excellent adsorption for IS with a maximum adsorption capacity of 69.40 mg·g^(-1)throughπ-πinteraction and hydrogen bonding interaction based on Langmuir isotherm models.Time-dependent absorption experiments showed that it reached adsorption equilibrium within 4 h,which was matched with the hemodialysis time.The coordination was significantly exhibited by introducing r GO aerogel blocks into the dialysate for absorbing the diffused free IS during hemodialysis.Taking the advantages of the TFNC dialysis membrane and the rGO aerogel,the volume of dialysate for hemodialysis was only one-tenth of that without adsorbent blocks but with very comparable dialysis performance(the clearance of IS at 51.8%and the retention of HSA over 98%),which could lighten conventional hemodialysis effectively and be benefit to realize the miniaturization of the hemodialysis equipment.Therefore,the coordination of the TFNC dialysis membrane and rGO aerogel adsorbents would open a new path for the development of portable artificial kidney.
基金from Natural Science Foundation of Shanghai with Grand No.19ZR1401300Program for Innovative Research Team in University of Ministry of Education of China with Grand No.IRT_16R13.
文摘A novel three-tier composite membrane based on highly porous nanofibrous substrate was demonstrated for efficient iso-propanol dehydration by pervaporation.Here,polyethyleneimine(PEI)modified graphene oxide(GO)sheets were vacuum-assistant assembled onto porous electrospun polyacrylonitrile(PAN)nanofibrous substrate to achieve a smooth,hydrophilic and compact PEI-GO intermediate layer.The introduction of PEI chains endowed GO interlayer with sufficient interaction for bonding adjacent GO nanosheets to enhance stability in water/isopropanol mixture and also with the ascended inter-lamellar space to improve the water-sorption ability due to the abundant active amino groups.Benefiting from PEI-GO layer,a defect-free sodium alginate(SA)skin layer could be facilely manufactured with elaborately controlled thickness as thin as possible in order to reduce mass transfer resistant and enhance permeability maximally.Meanwhile,the interlayer would also contribute to enhance interfacial adhesion to promote the structure integrity of three-tier thin-film nanofibrous composite(TFNC)membrane in pervaporation dehydration process.After fine-tuning of membrane preparation process,the SA/PEI(75)-GO-60/PAN TFNC membrane exhibited competitive pervaporation performance with the permeate flux of 2009 g/m2 h and the separation factor of 1276 operated at 70°C for dehydration of 90 wt%isopropanol solution.The unique three-tier composite membrane structure suggested an effective and facile approach to design novel membrane structure for further improvement of pervaporation performance.
基金We sincerely thank the State Key Laboratory of Chemical Engineering at Zhejiang University(No.SKL-ChE-20D01)the Program for Guangdong Introducing Innovative and Entrepreneurial Teams(No.2017ZT07C291)+1 种基金Shenzhen Science and Technology Program(No.KQTD20170810141424366)2019 Special Program for Central Government Guiding Local Science and Technology Development:Environmental Purification Functional Materials Research Platform,and Shenzhen Key Laboratory of Advanced Materials Product Engineering(No.ZDSYS20190911164401990)for supporting this research work。
文摘Metal-organic framework(MOF)/polymer composites have attracted extensive attention in the recent years.However,it still remains challenging to efficiently and effectively fabricate these composite materials.In this study,we propose a facile one-pot electrospinning strategy for preparation of HKUST-1/polyacrylonitrile(PAN)nanofibrous membranes from a homogeneous stock solution containing HKUST-1 precursors and PAN.MOF crystallization and polymer solidification occur simultaneously during the electrospinning process,thus avoiding the issues of aggregation and troublesome multistep fabrication of the conventional approach.The obtained HKUST-1/PAN electrospun membranes show uniform MOF distribution throughout the nanofibers and yield good mechanical properties.The membranes are used as separators in Li-metal full batteries under harsh testing conditions,using an ultrathin Li-metal anode,a high mass loading cathode,and the HKUST-1/PAN nanofibrous separator.The results demonstrate significantly improved cycling performance(capacity retention of 83.1%after 200 cycles)under a low negative to positive capacity ratio(N/P ratio of 1.86).The improvement can be attributed to an enhanced wettability of the separator towards electrolyte stemmed from the nanofibrous structure,and a uniform lithium ion flux stabilized by the open metal sites of uniformly distributed HKUST-1 particles in the membrane during cycling.