Here,an agricultural waste(the stem pith of helianthus annuus,SPHA)is firstly used as the precursor for preparing three-dimensional(3D)porous carbon sponge(PCS).The as-prepared 3D PCS(SPHA-700)possesses unique sponge-...Here,an agricultural waste(the stem pith of helianthus annuus,SPHA)is firstly used as the precursor for preparing three-dimensional(3D)porous carbon sponge(PCS).The as-prepared 3D PCS(SPHA-700)possesses unique sponge-like structure,large specific surface area(SSA)and high nitrogen doping level(4.52 at.%),which benefit the enhancement of conductivity(5.8 S cm;)and wettability.As a binder-free electrode for solid-state symmetric supercapacitor,SPHA-700 delivers a relatively high specific capacitance of137.1 F g^(-1)at 0.5 Ag^(-1).Moreover,activated SPHA-700(SPHA-ac-700–2)displays an even higher specific capacitance(403.6 F g^(-1)at 0.5 Ag^(-1))in 6.0 M KOH electrolyte.The SPHA-ac-700–2-based symmetrical supercapacitor can offer high specific capacitance(271 F g^(-1)at 1 Ag^(-1))and good rate capability(82.1%of capacitance retention at 1–80 Ag^(-1))in 6.0 M KOH electrolyte,together with high energy density(23.3 Wh kg^(-1)at 450 W kg^(-1))in 1.0 M Na_(2)SO_(4)electrolyte.Such excellent performance of SPHA-ac-700–2 is believed to have originated from the crushed sponge-like structure,O/N-co-doping(10.6 at.%O and3.3 at.%N),high SSA,large total pore volume,and hierarchical pore structure.展开更多
It is a big challenge to well control the porous structure of carbon materials for supercapacitor application.Herein,a simple in-situ self-templating strategy is developed to prepare three-dimensional(3D)hierarchical ...It is a big challenge to well control the porous structure of carbon materials for supercapacitor application.Herein,a simple in-situ self-templating strategy is developed to prepare three-dimensional(3D)hierarchical porous carbons with good combination of micro and meso-porous architecture derived from a new oxygen-bridged porous organic polymer(OPOP).The OPOP is produced by the condensation polymerization of cyanuric chloride and hydroquinone in NaOH ethanol solution and NaCl is in-situ formed as by-product that will serve as template to construct an interconnected 3D hierarchical porous architecture upon carbonization.The large interface pore architecture,and rich doping of N and O heteroatoms effectively promote the electrolyte accessibility and electronic conductivity,and provide abundant active sites for energy storage.Consequently,the supercapacitors based on the optimized OPOP-800 sample display an energy density of 8.44 and 27.28 Wh·kg^(−1)in 6.0 M KOH and 1.0 M Na2SO4 electrolytes,respectively.The capacitance retention is more than 94%after 10,000 cycles.Furthermore,density functional theory(DFT)calculations have been employed to unveil the charge storage mechanism in the OPOP-800.The results presented in this job are inspiring in finely tuning the porous structure to optimize the supercapacitive performance of carbon materials.展开更多
The exploration of high-efficiency,long-durability,and cost-effectiveness transition metal doped carbon materials to replace the commercial Pt/C in oxygen reduction reaction(ORR)is greatly desirable for promoting the ...The exploration of high-efficiency,long-durability,and cost-effectiveness transition metal doped carbon materials to replace the commercial Pt/C in oxygen reduction reaction(ORR)is greatly desirable for promoting the advancement of sustainable energy devices.Herein,the Fe_(3)N and FeCo alloy decorated N-doped carbon hybrid material(denoted Fe_(3)N-FeCo@NC)is prepared and applied as the ORR catalyst,which is derived from the two-step pyrolysis of an intriguing complex consisted of metal-coordinated porous polydopamine(PDA)nanospheres(i.e.,Fe-PDA@Co)and melamine.The resulting Fe_(3)N-FeCo@NC delivers outstanding ORR activity with an onset potential(E_(on))of 1.05 V,a half-wave potential(E_(1/2))of 0.89 V,as well as excellent long-term stability and methanol resistance over Pt/C.Interestingly,the home-made Zn-air battery with Fe_(3)N-FeCo@NC as the air-cathode demonstrates much higher open-circuit voltage(1.50 vs.1.48 V),power density(141 vs.113 mW·cm^(−2))and specific capacity(806.6 vs.660.6 mAh·g^(−1)_(Zn))than those of Pt/C counterpart.Such a remarkable ORR activity of Fe_(3)N-FeCo@NC may stem from the synergistic effect of Fe_(3)N and FeCo active species,the large surface area,the hierarchical porous structure and the exceptional sphere/sheet hybridized architecture.展开更多
基金financially supported by the National Nature Science Foundation of China(No.21805235)the China Postdoctoral Science Foundation(No.2017M610502)+2 种基金the Hunan Provincial Natural Science Foundation of China(No.2019JJ50614)the Opening Foundation of Creative Platform of the Key Laboratory of the Education Department of Hunan Province(No.20K131)the Construct Program of the Key Discipline in Hunan Province。
文摘Here,an agricultural waste(the stem pith of helianthus annuus,SPHA)is firstly used as the precursor for preparing three-dimensional(3D)porous carbon sponge(PCS).The as-prepared 3D PCS(SPHA-700)possesses unique sponge-like structure,large specific surface area(SSA)and high nitrogen doping level(4.52 at.%),which benefit the enhancement of conductivity(5.8 S cm;)and wettability.As a binder-free electrode for solid-state symmetric supercapacitor,SPHA-700 delivers a relatively high specific capacitance of137.1 F g^(-1)at 0.5 Ag^(-1).Moreover,activated SPHA-700(SPHA-ac-700–2)displays an even higher specific capacitance(403.6 F g^(-1)at 0.5 Ag^(-1))in 6.0 M KOH electrolyte.The SPHA-ac-700–2-based symmetrical supercapacitor can offer high specific capacitance(271 F g^(-1)at 1 Ag^(-1))and good rate capability(82.1%of capacitance retention at 1–80 Ag^(-1))in 6.0 M KOH electrolyte,together with high energy density(23.3 Wh kg^(-1)at 450 W kg^(-1))in 1.0 M Na_(2)SO_(4)electrolyte.Such excellent performance of SPHA-ac-700–2 is believed to have originated from the crushed sponge-like structure,O/N-co-doping(10.6 at.%O and3.3 at.%N),high SSA,large total pore volume,and hierarchical pore structure.
基金the National Natural Science Foundation of China(No.21805235)China Postdoctoral Science Foundation(No.2017M610502)+2 种基金the Opening Foundation of Creative Platform of the Key Laboratory of the Education Department of Hunan Province(No.20K131)the Construct Program of the Key Discipline in Hunan Province is greatly acknowledged.H.C.and Z.G.L.thank the support from the Basic Research Project of the Science and Technology Innovation Commission of Shenzhen(No.JCYJ20170817110251498)Shenzhen Key Laboratory of Interfacial Science and Engineering of Materials(No.ZDSYS20200421111401738).
文摘It is a big challenge to well control the porous structure of carbon materials for supercapacitor application.Herein,a simple in-situ self-templating strategy is developed to prepare three-dimensional(3D)hierarchical porous carbons with good combination of micro and meso-porous architecture derived from a new oxygen-bridged porous organic polymer(OPOP).The OPOP is produced by the condensation polymerization of cyanuric chloride and hydroquinone in NaOH ethanol solution and NaCl is in-situ formed as by-product that will serve as template to construct an interconnected 3D hierarchical porous architecture upon carbonization.The large interface pore architecture,and rich doping of N and O heteroatoms effectively promote the electrolyte accessibility and electronic conductivity,and provide abundant active sites for energy storage.Consequently,the supercapacitors based on the optimized OPOP-800 sample display an energy density of 8.44 and 27.28 Wh·kg^(−1)in 6.0 M KOH and 1.0 M Na2SO4 electrolytes,respectively.The capacitance retention is more than 94%after 10,000 cycles.Furthermore,density functional theory(DFT)calculations have been employed to unveil the charge storage mechanism in the OPOP-800.The results presented in this job are inspiring in finely tuning the porous structure to optimize the supercapacitive performance of carbon materials.
基金upported by the National Natural Science Foundation of China(No.52173207)the Natural Science Foundation of Hunan Province(Nos.2022JJ30563,2020JJ5542)the Outstanding Youth Fund Project of Hunan Provincial Department of Education(No.21B0119).
文摘The exploration of high-efficiency,long-durability,and cost-effectiveness transition metal doped carbon materials to replace the commercial Pt/C in oxygen reduction reaction(ORR)is greatly desirable for promoting the advancement of sustainable energy devices.Herein,the Fe_(3)N and FeCo alloy decorated N-doped carbon hybrid material(denoted Fe_(3)N-FeCo@NC)is prepared and applied as the ORR catalyst,which is derived from the two-step pyrolysis of an intriguing complex consisted of metal-coordinated porous polydopamine(PDA)nanospheres(i.e.,Fe-PDA@Co)and melamine.The resulting Fe_(3)N-FeCo@NC delivers outstanding ORR activity with an onset potential(E_(on))of 1.05 V,a half-wave potential(E_(1/2))of 0.89 V,as well as excellent long-term stability and methanol resistance over Pt/C.Interestingly,the home-made Zn-air battery with Fe_(3)N-FeCo@NC as the air-cathode demonstrates much higher open-circuit voltage(1.50 vs.1.48 V),power density(141 vs.113 mW·cm^(−2))and specific capacity(806.6 vs.660.6 mAh·g^(−1)_(Zn))than those of Pt/C counterpart.Such a remarkable ORR activity of Fe_(3)N-FeCo@NC may stem from the synergistic effect of Fe_(3)N and FeCo active species,the large surface area,the hierarchical porous structure and the exceptional sphere/sheet hybridized architecture.