Bismuth vanadate(BiVO_(4))is a promising photoanode material for efficient photoelectrochemical(PEC)water splitting,whereas its performance is inhibited by detrimental surface states.To solve the problem,herein,a low-...Bismuth vanadate(BiVO_(4))is a promising photoanode material for efficient photoelectrochemical(PEC)water splitting,whereas its performance is inhibited by detrimental surface states.To solve the problem,herein,a low-cost organic molecule 1,3,5-benzenetricarboxylic acid(BTC)is selected for surface passivation of BiVO_(4) photoanodes(BVOs),which also provides bonding sites for Co^(2+)to anchor,resulting in a Co-BTC-BVO photoanode.Owing to its strong coordination with metal ions,BTC not only passivates surface states of BVO,but also provides bonding between BVO and catalytic active sites(Co^(2+))to form a molecular cocatalyst.Computational study and interfacial charge kinetic investigation reveal that chemical bonding formed at the interface greatly suppresses charge recombination and accelerates charge transfer.The obtained Co-BTC-BVO photoanode exhibits a photocurrent density of 4.82 mA/cm^(2) at 1.23 V vs.reversible hydrogen electrode(RHE)and a low onset potential of 0.22 VRHE under AM 1.5 G illumination,which ranks among the best photoanodes coupled with Co-based cocatalysts.This work presents a novel selection of passivation layers and emphasizes the significance of interfacial chemical bonding for the construction of efficient photoanodes.展开更多
A high-efficiency electro-thermal heater requires simultaneously high electrical and thermal conductivities to generate and dissipate Joule heat efficiently.A low in put voltage is essential to en sure the heaters saf...A high-efficiency electro-thermal heater requires simultaneously high electrical and thermal conductivities to generate and dissipate Joule heat efficiently.A low in put voltage is essential to en sure the heaters safe applications.However,the low voltage gen erally leads to low saturated temperature and heati ng rate and hence a low thermal efficie ncy.How to reduce the in put voltage while maintai ning a high electro-thermal efficiency is still a challenge.Herein,a highly electrical and thermal conductive film was 8nstructed using a graphene-based composite which has an internal three-dimensional(3D)conductive network.In the 3D framework,cellulose nanocrystalline(CNC)phase with chiral liquid crystal manner presents in the form of alig ned helix betwee n the graphe ne oxide(GO)layers.Carbon nano dots(CDs)are assembled泊side the composite as con ductive nano fillers.Subseque nt an neali ng and compressi on results in the formati on of the assembled GO-CNC-CDs film.The carb on ized CNC nano rods(CNR)with the helical alignment act as irrplane and through-pla ne conn ecti ons of n eighbori ng reduced GO(rGO)nano sheets,forming a con ductive network in the composite film.The CDs with ultrafast electr ons tran sfer rates provide additi onal electro ns and phonons tran sport paths for the composite.As a result,the obtai ned graphe ne?based composite film(rGO-CNR-CDs)exhibited a high thermal conductivity of 1,978.6 W m^-1·K^-1 and electrical conductivity of 2,053.4 S·cm^-1,respectively.The composite film showed an outstanding electro-thermal heating efficiency with the saturated temperature of 315℃and maximum heating rate of 44.9℃·s^-1 at a very low in put voltage of 10 V.The freestandi ng graphe ne composite film with the delicate nano structure desig n has a great pote ntial to be integrated into electro-thermal devices.展开更多
Hypoxia is a huge barrier for the development of photodynamic therapy(PDT).Chemodynamic therapy(CDT)could provide a possible solution to this dilemma.In this work,a controlled Schiff-base reaction was conducted betwee...Hypoxia is a huge barrier for the development of photodynamic therapy(PDT).Chemodynamic therapy(CDT)could provide a possible solution to this dilemma.In this work,a controlled Schiff-base reaction was conducted between amido groups on the surface of carbon dots(CDs)and aldehyde groups on aldehyde-modified cellulose nanocrystals(mCNCs)as well as aldehydemCNCs decorated with Fe_(3)O_(4)nanoparticles.In this process,the mCNCs not only prevent the agglomeration of Fe_(3)O_(4)but also form hydrogels with CDs.The CDs act as both photothermal agent and photosensitizer.The hypoxia could be effectively relieved through the Fenton reaction due to the addition of Fe_(3)O_(4),and the·OH produced in the reaction further induces CDT and enhances tumor therapy efficiency.The therapy performance was further verified through in vitro cell experiments and in vivo animal experiments.This convenient method provides inspirations for the design and preparation of advanced biomaterials with multiple functions for cancer therapy.展开更多
基金support from the National Natural Science Foundation of China(No.51672173,U1733130)Shanghai Science and Technology Committee(Nos.21ZR1435700,18520744700, 18JC1410500)Shanghai Jiao Tong University Medical Engineering Cross Research Program(No.YG2023ZD18).
文摘Bismuth vanadate(BiVO_(4))is a promising photoanode material for efficient photoelectrochemical(PEC)water splitting,whereas its performance is inhibited by detrimental surface states.To solve the problem,herein,a low-cost organic molecule 1,3,5-benzenetricarboxylic acid(BTC)is selected for surface passivation of BiVO_(4) photoanodes(BVOs),which also provides bonding sites for Co^(2+)to anchor,resulting in a Co-BTC-BVO photoanode.Owing to its strong coordination with metal ions,BTC not only passivates surface states of BVO,but also provides bonding between BVO and catalytic active sites(Co^(2+))to form a molecular cocatalyst.Computational study and interfacial charge kinetic investigation reveal that chemical bonding formed at the interface greatly suppresses charge recombination and accelerates charge transfer.The obtained Co-BTC-BVO photoanode exhibits a photocurrent density of 4.82 mA/cm^(2) at 1.23 V vs.reversible hydrogen electrode(RHE)and a low onset potential of 0.22 VRHE under AM 1.5 G illumination,which ranks among the best photoanodes coupled with Co-based cocatalysts.This work presents a novel selection of passivation layers and emphasizes the significance of interfacial chemical bonding for the construction of efficient photoanodes.
基金This work was supported by the National Key R&D Program of China(Nos.2016YFA0202900 and 2016YFC1402400)National Natural Science Foundation of China(No.51672173)+2 种基金Shanghai Science and Technology committee(No.17JC1400700 and 18520744700)Science and Technology Planning Project of Guangdong Province(No.2016A010103018)The authors gratefully acknowledge the Shanghai Synchrotron Radiation Facility(SSRF)and Shanghai LEVSON Group Co.,Ltd.for the measurements.
文摘A high-efficiency electro-thermal heater requires simultaneously high electrical and thermal conductivities to generate and dissipate Joule heat efficiently.A low in put voltage is essential to en sure the heaters safe applications.However,the low voltage gen erally leads to low saturated temperature and heati ng rate and hence a low thermal efficie ncy.How to reduce the in put voltage while maintai ning a high electro-thermal efficiency is still a challenge.Herein,a highly electrical and thermal conductive film was 8nstructed using a graphene-based composite which has an internal three-dimensional(3D)conductive network.In the 3D framework,cellulose nanocrystalline(CNC)phase with chiral liquid crystal manner presents in the form of alig ned helix betwee n the graphe ne oxide(GO)layers.Carbon nano dots(CDs)are assembled泊side the composite as con ductive nano fillers.Subseque nt an neali ng and compressi on results in the formati on of the assembled GO-CNC-CDs film.The carb on ized CNC nano rods(CNR)with the helical alignment act as irrplane and through-pla ne conn ecti ons of n eighbori ng reduced GO(rGO)nano sheets,forming a con ductive network in the composite film.The CDs with ultrafast electr ons tran sfer rates provide additi onal electro ns and phonons tran sport paths for the composite.As a result,the obtai ned graphe ne?based composite film(rGO-CNR-CDs)exhibited a high thermal conductivity of 1,978.6 W m^-1·K^-1 and electrical conductivity of 2,053.4 S·cm^-1,respectively.The composite film showed an outstanding electro-thermal heating efficiency with the saturated temperature of 315℃and maximum heating rate of 44.9℃·s^-1 at a very low in put voltage of 10 V.The freestandi ng graphe ne composite film with the delicate nano structure desig n has a great pote ntial to be integrated into electro-thermal devices.
基金Ministry of Education Joint Foundation(No.6141A02022264)the National Natural Science Foundation of China(Nos.51672173,U1733130,and 81770934)+3 种基金Shanghai Science and Technology Committee(Nos.21ZR1435700,18520744700,and 18JC1410500)Translational Medicine National Key Science and Technology Infrastructure(Shanghai)Open Project(No.TMSK2020128)Shanghai Municipal Education Commission-Gaofeng Clinical Medicine Grant Support(No.20181810)Clinical research MDT project of the Ninth People's Hospital Affiliated to Shanghai Jiaotong University School of Medicine(No.201905).
文摘Hypoxia is a huge barrier for the development of photodynamic therapy(PDT).Chemodynamic therapy(CDT)could provide a possible solution to this dilemma.In this work,a controlled Schiff-base reaction was conducted between amido groups on the surface of carbon dots(CDs)and aldehyde groups on aldehyde-modified cellulose nanocrystals(mCNCs)as well as aldehydemCNCs decorated with Fe_(3)O_(4)nanoparticles.In this process,the mCNCs not only prevent the agglomeration of Fe_(3)O_(4)but also form hydrogels with CDs.The CDs act as both photothermal agent and photosensitizer.The hypoxia could be effectively relieved through the Fenton reaction due to the addition of Fe_(3)O_(4),and the·OH produced in the reaction further induces CDT and enhances tumor therapy efficiency.The therapy performance was further verified through in vitro cell experiments and in vivo animal experiments.This convenient method provides inspirations for the design and preparation of advanced biomaterials with multiple functions for cancer therapy.