The self-charging concept has drawn considerable attention due to its excellent ability to achieve environmental energy harvesting,conversion and storage without an external power supply.However,most self-charging des...The self-charging concept has drawn considerable attention due to its excellent ability to achieve environmental energy harvesting,conversion and storage without an external power supply.However,most self-charging designs assembled by multiple energy harvesting,conversion and storage materials increase the energy transfer loss;the environmental energy supply is generally limited by climate and meteorological conditions,hindering the potential application of these selfpowered devices to be available at all times.Based on aerobic autoxidation of catechol,which is similar to the electrochemical oxidation of the catechol groups on the carbon materials under an electrical charge,we proposed an air-breathing chemical self-charge concept based on the aerobic autoxidation of catechol groups on oxygen-enriched carbon materials to ortho-quinone groups.Energy harvesting,conversion and storage functions could be integrated on a single carbon material to avoid the energy transfer loss among the different materials.Moreover,the assembled Cu/oxygen-enriched carbon battery confirmed the feasibility of the air-oxidation self-charging/electrical discharging mechanism for potential applications.This air-breathing chemical self-charge concept could facilitate the exploration of high-efficiency sustainable air self-charging devices.展开更多
Carbon hollow microspheres as microwave absorption materials(MAMs)are of great significance in the research focuses owing to their lightweight,good impedance matching,and modifiable dielectric proper-ties.However,it i...Carbon hollow microspheres as microwave absorption materials(MAMs)are of great significance in the research focuses owing to their lightweight,good impedance matching,and modifiable dielectric proper-ties.However,it is still a huge challenge to distinguish the contribution of dielectric attenuation between carbon intrinsic feature and hollow structure due to the lack of appropriate model materials.Then,the inadequate analysis of effective dielectric attenuation resulted in the construction of carbon hollow mi-crospheres semiempirical and often lacked precise modification of microstructure.Herein,a series of car-bon hollow microspheres with controllable graphitization and thickness of shell derived from phenolic resin coated on polystyrene microspheres that fully decomposed were synthesized,which is free of the impact of template residue.The carbon fragments ground from hollow microspheres exhibit the same broadband response as hollow microspheres,with effective bandwidth(RL<-10 dB)of 7.6 GHz,while their electromagnetic wave loss mechanisms are distinct.The high dielectric loss of carbon fragments with the same intrinsic characteristics as carbon hollow microspheres is mainly caused by dipole po-larization relaxation and enhancement of electrical conductivity ascribed to overlapping between carbon sheets.For the hollow structure,in addition to dipole polarization relaxation attributed to carbon intrin-sic feature,the effective dielectric loss is also comprised of the interfacial polarization in advantage due to the effective heterogeneous interface between air and carbon shell.This work provides a simplified model to clarify the effect of carbon intrinsic feature and microstructure on the dielectric loss of carbon hollow microspheres.展开更多
Porous heteroatom-doped carbon materials exhibit promising electrochemical applications because of tunable porous structure and doping heteroatom-induced charge redistribution.Nevertheless,it is still a great challeng...Porous heteroatom-doped carbon materials exhibit promising electrochemical applications because of tunable porous structure and doping heteroatom-induced charge redistribution.Nevertheless,it is still a great challenge to develop porous heteroatom-doped carbon materials with both high-content active heteroatom species and facilitated diffusion route.Herein,we report a bowl-shaped nitrogen and oxygen dual-doping carbon(N,O-doped carbon)material based on low-temperature defluorination pyrolysis and alkali-etched activation of 3-fluorophenol-3-amino-4-hydroxypyridine-formaldehyde co-condensed resin and its excellent supercapacitance.This low-temperature thermal treatment strategy ensures high-content pyrrolic nitrogen(4.6 at.%)and oxygen species(15.9 at.%)to avoid high-temperature treatment-induced heteroatom loss and undesired configuration conversion.In these processes,the defluorination pyrolysis promotes the transformation from the resin to carbon material to some extent,and KOH activation also promotes the ordered arrangement of 002 planes,which together assure the appropriate conductivity of the final microporous carbon material.More importantly,KOH-etched activation partially removes an un-stable nano/microscale domain of the intermediate carbon microspheres to form a unique bowl-shaped structure extremely facilitating the diffusion of the substitutes and/or electrolyte ions.As expected,N,O-doped carbon material displays a remarkable specific capacitance of 486.4 F g^(−1)at 1 A g^(−1)with nitro-gen/oxygen species-dependant pseudocapacitance and good electrochemical durability.展开更多
基金financially supported by the National Natural Science Foundation of China(51503178,52202048,52027801)National Key R&D Program of China(2017YFA0206301)+1 种基金China-Germany Collaboration Project(M-0199)Natural Science Foundation of Hebei Province(B2021203012,E2022203082)。
文摘The self-charging concept has drawn considerable attention due to its excellent ability to achieve environmental energy harvesting,conversion and storage without an external power supply.However,most self-charging designs assembled by multiple energy harvesting,conversion and storage materials increase the energy transfer loss;the environmental energy supply is generally limited by climate and meteorological conditions,hindering the potential application of these selfpowered devices to be available at all times.Based on aerobic autoxidation of catechol,which is similar to the electrochemical oxidation of the catechol groups on the carbon materials under an electrical charge,we proposed an air-breathing chemical self-charge concept based on the aerobic autoxidation of catechol groups on oxygen-enriched carbon materials to ortho-quinone groups.Energy harvesting,conversion and storage functions could be integrated on a single carbon material to avoid the energy transfer loss among the different materials.Moreover,the assembled Cu/oxygen-enriched carbon battery confirmed the feasibility of the air-oxidation self-charging/electrical discharging mechanism for potential applications.This air-breathing chemical self-charge concept could facilitate the exploration of high-efficiency sustainable air self-charging devices.
基金National Natural Science Foundation of China(grant No.51802278)Natural Science Foundation of Hebei Province(grant Nos.B2021203012,E2022203082)Department of Education of Hebei Province(grant No.QN2021140).
文摘Carbon hollow microspheres as microwave absorption materials(MAMs)are of great significance in the research focuses owing to their lightweight,good impedance matching,and modifiable dielectric proper-ties.However,it is still a huge challenge to distinguish the contribution of dielectric attenuation between carbon intrinsic feature and hollow structure due to the lack of appropriate model materials.Then,the inadequate analysis of effective dielectric attenuation resulted in the construction of carbon hollow mi-crospheres semiempirical and often lacked precise modification of microstructure.Herein,a series of car-bon hollow microspheres with controllable graphitization and thickness of shell derived from phenolic resin coated on polystyrene microspheres that fully decomposed were synthesized,which is free of the impact of template residue.The carbon fragments ground from hollow microspheres exhibit the same broadband response as hollow microspheres,with effective bandwidth(RL<-10 dB)of 7.6 GHz,while their electromagnetic wave loss mechanisms are distinct.The high dielectric loss of carbon fragments with the same intrinsic characteristics as carbon hollow microspheres is mainly caused by dipole po-larization relaxation and enhancement of electrical conductivity ascribed to overlapping between carbon sheets.For the hollow structure,in addition to dipole polarization relaxation attributed to carbon intrin-sic feature,the effective dielectric loss is also comprised of the interfacial polarization in advantage due to the effective heterogeneous interface between air and carbon shell.This work provides a simplified model to clarify the effect of carbon intrinsic feature and microstructure on the dielectric loss of carbon hollow microspheres.
基金the National Natural Science Foundation of China(No.52202048)the Hebei Natural Science Foundation(Nos.E2022203082 and B2021203012)the Department of Education of Hebei Province(No.QN2021140).
文摘Porous heteroatom-doped carbon materials exhibit promising electrochemical applications because of tunable porous structure and doping heteroatom-induced charge redistribution.Nevertheless,it is still a great challenge to develop porous heteroatom-doped carbon materials with both high-content active heteroatom species and facilitated diffusion route.Herein,we report a bowl-shaped nitrogen and oxygen dual-doping carbon(N,O-doped carbon)material based on low-temperature defluorination pyrolysis and alkali-etched activation of 3-fluorophenol-3-amino-4-hydroxypyridine-formaldehyde co-condensed resin and its excellent supercapacitance.This low-temperature thermal treatment strategy ensures high-content pyrrolic nitrogen(4.6 at.%)and oxygen species(15.9 at.%)to avoid high-temperature treatment-induced heteroatom loss and undesired configuration conversion.In these processes,the defluorination pyrolysis promotes the transformation from the resin to carbon material to some extent,and KOH activation also promotes the ordered arrangement of 002 planes,which together assure the appropriate conductivity of the final microporous carbon material.More importantly,KOH-etched activation partially removes an un-stable nano/microscale domain of the intermediate carbon microspheres to form a unique bowl-shaped structure extremely facilitating the diffusion of the substitutes and/or electrolyte ions.As expected,N,O-doped carbon material displays a remarkable specific capacitance of 486.4 F g^(−1)at 1 A g^(−1)with nitro-gen/oxygen species-dependant pseudocapacitance and good electrochemical durability.
