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
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.
