Organic electrode materials are promising for lithium-ion batteries(LIBs) because of their environmental friendliness and structural diversity.However,they always suffer from limited capacity,poor cycling stability,an...Organic electrode materials are promising for lithium-ion batteries(LIBs) because of their environmental friendliness and structural diversity.However,they always suffer from limited capacity,poor cycling stability,and rate performance.Herein,hexaazatrinaphthalene-based azo-linked hyperbranched polymer(HAHP) is designed and synthesized as a cathode for LIBs.However,the densely stacked morphology lowers the chance of the active sites participating in the redox reaction.To address this issue,the singlewalled carbon nanotube(SWCNT) template is used to induce the growth of nanosized HAHP on the surface of SWCNTs.The HAHP@SWCNT nanocomposites have porous structures and highly accessible active sites.Moreover,the strong π-π interaction between HAHP and highly conductive SWCNTs effectively endows the HAHP@SWCNT nanocomposites with improved cycling stability and fast charge-discharge rates.As a result,the HAHP@SWCNT nanocomposite cathode shows a high specific capacity(320.4 mA h g^(-1)at 100 mA g^(-1)),excellent cycling stability(800 cycles;290 mA h g^(-1)at 100 mA g^(-1),capacity retained 91%) and outstanding rate performance(235 mA h g^(-1)at 2000 mA g^(-1),76% capacity retention versus 50 mA g^(-1)).This work provides a strategy to combine the macromolecular structural design and micromorphology control of electrode materials for obtaining organic polymer cathodes for high-performance LIBs.展开更多
Carbon dots(CDs),as a new kind of carbon-based luminescent nanomaterials,have drawn widespread attention in the fields of fluorescence sensing,optoelectronic devices,and biological imaging.This work uses citric acid(C...Carbon dots(CDs),as a new kind of carbon-based luminescent nanomaterials,have drawn widespread attention in the fields of fluorescence sensing,optoelectronic devices,and biological imaging.This work uses citric acid(CA)and Nile Blue A(NBA)as precursors.By simply changing the solvent in the reaction,their bandgaps were systematically controlled,thereby successfully obtaining bright blue,yellow and red fluorescence emission CDs(B-,Y-and RCDs).The higher quantum yield(QY)of B-,Y-and RCDs are 64%,57%and 51%,respectively.The selected precursors and different solvents are the key to the formation of three emission CDs.Detailed characterization and density functional theory(DFT)calculations further indicate that the difference in emission color of CDs is due to the size of the sp^(2) conjugate domain.In addition,we used multicolor CDs as fluorescent probes to investigate their performance in detection.Among them,BCDs and YCDs can detect Sudan Red I with high selectivity and sensitivity.In the concentration range of 0 to 80 pM,the detection limits are 56 and 41 nM,respectively.Multicolor emitting phosphors and fluorescent films are also obtained by mixing CDs with other matrices.Using Ultraviolet(UV)chip as the excitation source and combining with multicolor fluorescent film and a certain proportion of B-,Y-,and RCDs/epoxy resin composites,bright monochromatic light-emitting diodes(LEDs)and white LED(WLED)with high color rendering index(CRI)were prepared.The above results indicate that the multicolor CDs prepared by us have great application potential in the fields of food safety control and optical devices.展开更多
With the in-depth research of sodium-ion batteries(SIBs),the development of novel sodium-ion anode material has become a top priority.In this work,tube cluster-shaped SbPS_(4)was synthesized by a high-temperature soli...With the in-depth research of sodium-ion batteries(SIBs),the development of novel sodium-ion anode material has become a top priority.In this work,tube cluster-shaped SbPS_(4)was synthesized by a high-temperature solid phase reaction.Then the typical short tubular ternary thiophosphate SbPS_(4)compounded with graphene oxide(SbPS_(4)/GO)was successfully synthesized after ultrasonication and freeze-drying.SbPS_(4)shows a high theoretical specific capacity(1335 mAh/g)according to the conversion-alloying dual mechanisms.The unique short tube inserted in the spongy graphene structure of SbPS_(4)/GO results in boosting the Na ions transport and alleviating the huge volume change in the charging and discharging processes,improving the sodium storage performance.Consequently,the tubular SbPS_(4)compounded with 10%GO provides an outstanding capacity of 359.58 mAh/g at 500 mA/g.The result indicates that SbPS_(4)/GO anode has a promising application potential for SIBs.展开更多
A knowledge of the adsorption and desorption behavior of sorbates on surface adsorptive site(SAS)is the key to optimizing the chemical reactivity of catalysts.However,direct identification of the chemical reactivity o...A knowledge of the adsorption and desorption behavior of sorbates on surface adsorptive site(SAS)is the key to optimizing the chemical reactivity of catalysts.However,direct identification of the chemical reactivity of SASs is still a challenge due to the limitations of characterization techniques.Here,we present a new pathway to determine the kinetics of adsorption/desorption on SASs of graphene oxide(GO)based on total internal reflectance fluorescence microscopy.The switching on and off of the fluorescent signal of SAS lit by carbon dots(CDs)was used to trace the adsorption process and desorption process.We find that sodium pyrophosphate(PPi)could increase the adsorption equilibrium of CDs thermodynamically and promote the substrate-assisted desorption pathway kinetically.At the single turnover level,it was disclosed that the species that can promote desorption may also be an adsorption promoter.Such discovery provides significant guidance for improving the chemical reactivity of the heterogeneous catalyst.展开更多
基金supported by the National Natural Science Foundation of China(Grant No.51903100)the Science and Technology Development Plan of Jilin Province,China(Grant No.20210402060GH)。
文摘Organic electrode materials are promising for lithium-ion batteries(LIBs) because of their environmental friendliness and structural diversity.However,they always suffer from limited capacity,poor cycling stability,and rate performance.Herein,hexaazatrinaphthalene-based azo-linked hyperbranched polymer(HAHP) is designed and synthesized as a cathode for LIBs.However,the densely stacked morphology lowers the chance of the active sites participating in the redox reaction.To address this issue,the singlewalled carbon nanotube(SWCNT) template is used to induce the growth of nanosized HAHP on the surface of SWCNTs.The HAHP@SWCNT nanocomposites have porous structures and highly accessible active sites.Moreover,the strong π-π interaction between HAHP and highly conductive SWCNTs effectively endows the HAHP@SWCNT nanocomposites with improved cycling stability and fast charge-discharge rates.As a result,the HAHP@SWCNT nanocomposite cathode shows a high specific capacity(320.4 mA h g^(-1)at 100 mA g^(-1)),excellent cycling stability(800 cycles;290 mA h g^(-1)at 100 mA g^(-1),capacity retained 91%) and outstanding rate performance(235 mA h g^(-1)at 2000 mA g^(-1),76% capacity retention versus 50 mA g^(-1)).This work provides a strategy to combine the macromolecular structural design and micromorphology control of electrode materials for obtaining organic polymer cathodes for high-performance LIBs.
基金supported by the National Natural Science Foundation of China(Nos.51678409,51638011,and 51578375)Tianjin Research Program of Application Foundation and Advanced Technology(Nos.19JCYBJC19800,18JCYBJC87500,and 15ZCZDSF00880)+1 种基金State Key Laboratory of Separation Membranes and Membrane Processes(Z1-201507)the Program for Innovative Research Team in University of Tianjin(TD13-5042).
文摘Carbon dots(CDs),as a new kind of carbon-based luminescent nanomaterials,have drawn widespread attention in the fields of fluorescence sensing,optoelectronic devices,and biological imaging.This work uses citric acid(CA)and Nile Blue A(NBA)as precursors.By simply changing the solvent in the reaction,their bandgaps were systematically controlled,thereby successfully obtaining bright blue,yellow and red fluorescence emission CDs(B-,Y-and RCDs).The higher quantum yield(QY)of B-,Y-and RCDs are 64%,57%and 51%,respectively.The selected precursors and different solvents are the key to the formation of three emission CDs.Detailed characterization and density functional theory(DFT)calculations further indicate that the difference in emission color of CDs is due to the size of the sp^(2) conjugate domain.In addition,we used multicolor CDs as fluorescent probes to investigate their performance in detection.Among them,BCDs and YCDs can detect Sudan Red I with high selectivity and sensitivity.In the concentration range of 0 to 80 pM,the detection limits are 56 and 41 nM,respectively.Multicolor emitting phosphors and fluorescent films are also obtained by mixing CDs with other matrices.Using Ultraviolet(UV)chip as the excitation source and combining with multicolor fluorescent film and a certain proportion of B-,Y-,and RCDs/epoxy resin composites,bright monochromatic light-emitting diodes(LEDs)and white LED(WLED)with high color rendering index(CRI)were prepared.The above results indicate that the multicolor CDs prepared by us have great application potential in the fields of food safety control and optical devices.
基金the financial support from the National Natural Science Foundation of China(Nos.91963118,51801030)supported by the Open Project Program of Key Laboratory of Preparation and Application of Environmental Friendly Materials(Jilin Normal University,No.2020004)。
文摘With the in-depth research of sodium-ion batteries(SIBs),the development of novel sodium-ion anode material has become a top priority.In this work,tube cluster-shaped SbPS_(4)was synthesized by a high-temperature solid phase reaction.Then the typical short tubular ternary thiophosphate SbPS_(4)compounded with graphene oxide(SbPS_(4)/GO)was successfully synthesized after ultrasonication and freeze-drying.SbPS_(4)shows a high theoretical specific capacity(1335 mAh/g)according to the conversion-alloying dual mechanisms.The unique short tube inserted in the spongy graphene structure of SbPS_(4)/GO results in boosting the Na ions transport and alleviating the huge volume change in the charging and discharging processes,improving the sodium storage performance.Consequently,the tubular SbPS_(4)compounded with 10%GO provides an outstanding capacity of 359.58 mAh/g at 500 mA/g.The result indicates that SbPS_(4)/GO anode has a promising application potential for SIBs.
基金This work was funded by the Research&Development Projects in Key Areas of Guangdong Province,China(2019B010933001)the National Natural Science Foundation of China(21974033,21904026)+1 种基金the National Basic Research Program of China(973 Program,2017YFE0197900)the Innovation Training Program for College Students of Guangzhou University(CX2019185).
文摘A knowledge of the adsorption and desorption behavior of sorbates on surface adsorptive site(SAS)is the key to optimizing the chemical reactivity of catalysts.However,direct identification of the chemical reactivity of SASs is still a challenge due to the limitations of characterization techniques.Here,we present a new pathway to determine the kinetics of adsorption/desorption on SASs of graphene oxide(GO)based on total internal reflectance fluorescence microscopy.The switching on and off of the fluorescent signal of SAS lit by carbon dots(CDs)was used to trace the adsorption process and desorption process.We find that sodium pyrophosphate(PPi)could increase the adsorption equilibrium of CDs thermodynamically and promote the substrate-assisted desorption pathway kinetically.At the single turnover level,it was disclosed that the species that can promote desorption may also be an adsorption promoter.Such discovery provides significant guidance for improving the chemical reactivity of the heterogeneous catalyst.