Highly active Fe-N_x sites that effectively improve the performance of non-precious metal electrocatalysts for oxygen reduction reactions(ORRs) are desirable. Herein, we propose a strategy for introducing a carbon t...Highly active Fe-N_x sites that effectively improve the performance of non-precious metal electrocatalysts for oxygen reduction reactions(ORRs) are desirable. Herein, we propose a strategy for introducing a carbon template into a melamine/Fe-salt mixture to inductively generate highly active Fe-N_x sites for ORR. Using 57 Fe M?sbauer spectroscopy, X-ray photoelectron spectroscopy, and X-ray diffraction, we studied the structural composition of the Fe and N co-doped carbon catalysts.Interestingly, the results showed that this system not only converted inactive Fe and Fe-carbides into active Fe-N_4 and other Fe-nitrides, but also improved their intrinsic activities.展开更多
Studies on three-dimensional structured carbon templates have focused on how to guide homogeneous lithium metal nucleation and growth for lithium metal anodes(LMAs).However,there is still insufficient evidence for a k...Studies on three-dimensional structured carbon templates have focused on how to guide homogeneous lithium metal nucleation and growth for lithium metal anodes(LMAs).However,there is still insufficient evidence for a key factor to achieve their high electrochemical performance.Here,the effects of nanopores and sulfur doping on carbon-based nanoporous host(CNH)electrode materials for LMAs were investigated using natural polymer-derived CNHs.Homogeneous pore-filling behaviors of lithium metal in the nanopores of the CNH electrode materials were first observed by ex situ scanning electron microscopy analysis,where the protective lithium metal nucleation and growth process led to significantly high Coulombic efficiency(CE)of~99.4%and stable 600 cycles.In addition,a comparison study of CNH and sulfurdoped CNH(S-CNH)electrodes,which differ only in the presence or absence of sulfur,revealed that sulfur doping can cause lower electrochemical series resistance,higher CE value,and better cycling stability in a wide range of current densities and number of cycles.Moreover,S-CNH-based LMAs showed high electrochemical performance in full-cell Li-S battery tests using a sulfur copolymer cathode,where a high energy density of 1370Wh kgelectrode−1 and an excellent power density of 4120Wkgelectrode−1 were obtained.展开更多
In this work, the morphologies and pore structures of a series of corncob-derived activated carbons and zeolite templated carbon with ultrahigh surface area were carefully investigated by SEM, HRTEM and N2-sorption ch...In this work, the morphologies and pore structures of a series of corncob-derived activated carbons and zeolite templated carbon with ultrahigh surface area were carefully investigated by SEM, HRTEM and N2-sorption characterization technologies. The high-pressure hydrogen uptake performance was analyzed using standard Pressure-Composition-Temperature apparatus in order to study the pore size effects on hydrogen uptake. These as-obtained porous carbons showed different characteristics of pore size distribution as well as specific surface area. The results indicate that the most effective pores for adsorbing hydrogen depended on the storage pressure. These ultramicropores (0.65-0.85 nm) could be the most effective pores on excess H2 uptake at 1 bar, however, micropores (0.85-2 nm) would play a more important role in excess H2 uptake at higher pressure at 77 K. At room temperature, pore size effects on H2 uptake capacity were very weak. Both specific surface area and total pore volume play more important roles than pore size for H2 uptake at room temperature, which was clearly different from that at 77 K. For applications in future, the corncob-derived activated carbons can be more available than zeolite templated carbons at 77 K. Element doping enhanced hydrogen uptake could be main research direction for improving H2 uptake capacity at room temperature.展开更多
NS codoped carbon nanorods(NS-CNRs) were prepared using crab shell as template and polyphenylene sulfide(PPS) as both the C and S precursor, followed by carbonization in NH_3. The as-obtained NS-CNRs had a diamete...NS codoped carbon nanorods(NS-CNRs) were prepared using crab shell as template and polyphenylene sulfide(PPS) as both the C and S precursor, followed by carbonization in NH_3. The as-obtained NS-CNRs had a diameter of ~50 nm, length of several micrometers, and N and S contents of 12.5 at.% and 3.7 at.%,respectively, which can serve as anodes for both lithium-ion batteries(LIBs) and sodium ion batteries(SIBs). When serving as an anode of LIB, the NS-CNRs delivered gravimetric capacities of 2154 mAh g^(-1)at current densities of 0.1 A g^(-1)and 625 mAh g^(-1)at current densities of 5.0 A g^(-1)for 1000 cycles.When serving as an anode of SIB, the NS-CNRs delivered gravimetric capacities of 303 mAh g^(-1)at current densities of 0.1 A g^(-1)and 230 mAh g^(-1)at current densities of 1.0 A g^(-1)for 3000 cycles. The excellent electrochemical performance of NS-CNRs could be ascribed to the one-dimensional nanometer structure and high level of heteroatom doping. We expect that the obtained NS-CNRs would benefit for the future development of the doped carbon materials for lithium ion batteries and other extended applications such as supercapacitor, catalyst and hydrogen storage.展开更多
Tuning porous structure of carbon nanomaterials has been found to be important for their performance enhancement in electrochemical energy storage applications. In this work we employed a natural nanomaterial kaolinit...Tuning porous structure of carbon nanomaterials has been found to be important for their performance enhancement in electrochemical energy storage applications. In this work we employed a natural nanomaterial kaolinite, which is abundant and cheap, as hard template to synthesis porous carbon nanomaterial. By tuning the structure of hard template kaolinite, we have achieved a template directed formation of holey carbon nanosheet/nanotube materials. This carbon nanomaterials with hierarchical in-plane and out-of-plane pores have shown electrochemical energy storage capacity of 286 F/g(equal to 314 F/cm^3) at 0.1 A/g and 85 F/g(equal to 93 F/cm^3) at 100 A/g, which is comparable to variety of reported carbon based electrochemical energy storage electrode materials.展开更多
Hybrid ion capacitors have been considered as a very attractive energy source with high energy density and power density since it combines both merits of lithium ion batteries and supercapacitors. However,their commer...Hybrid ion capacitors have been considered as a very attractive energy source with high energy density and power density since it combines both merits of lithium ion batteries and supercapacitors. However,their commercial application has been limited by the mismatch of charge-storage capacity and electrode kinetics between the capacitor-type cathode and battery-type anode. Herein, B and N dual-doped 3D superstructure carbon cathode is prepared through a facile template method. It delivers a high specific capacity, excellent rate capability and good cycling stability due to the B, N dual-doping, which has a profound effect in control the porosity, functional groups, and electronic conductivity for the carbon cathode. The hybrid ion capacitors using B, N dual-doping carbon cathode and prelithiated graphite anode show a high energy density of 115.5 Wh/kg at 250 W/kg and remain about 53.6 Wh/kg even at a high power density of 10 kW/kg. Additionally, the novel hybrid device achieves 76.3% capacity retention after 2000 cycles tested at 1250 W/kg power density. Significantly, the simultaneous manipulation of heteroatoms in carbon materials provides new opportunities to boost the energy and power density for hybrid ion capacitors.展开更多
文摘Highly active Fe-N_x sites that effectively improve the performance of non-precious metal electrocatalysts for oxygen reduction reactions(ORRs) are desirable. Herein, we propose a strategy for introducing a carbon template into a melamine/Fe-salt mixture to inductively generate highly active Fe-N_x sites for ORR. Using 57 Fe M?sbauer spectroscopy, X-ray photoelectron spectroscopy, and X-ray diffraction, we studied the structural composition of the Fe and N co-doped carbon catalysts.Interestingly, the results showed that this system not only converted inactive Fe and Fe-carbides into active Fe-N_4 and other Fe-nitrides, but also improved their intrinsic activities.
基金National Research Foundation of Korea,Grant/Award Numbers:2019R1A2C1084836,2021R1A4A2001403。
文摘Studies on three-dimensional structured carbon templates have focused on how to guide homogeneous lithium metal nucleation and growth for lithium metal anodes(LMAs).However,there is still insufficient evidence for a key factor to achieve their high electrochemical performance.Here,the effects of nanopores and sulfur doping on carbon-based nanoporous host(CNH)electrode materials for LMAs were investigated using natural polymer-derived CNHs.Homogeneous pore-filling behaviors of lithium metal in the nanopores of the CNH electrode materials were first observed by ex situ scanning electron microscopy analysis,where the protective lithium metal nucleation and growth process led to significantly high Coulombic efficiency(CE)of~99.4%and stable 600 cycles.In addition,a comparison study of CNH and sulfurdoped CNH(S-CNH)electrodes,which differ only in the presence or absence of sulfur,revealed that sulfur doping can cause lower electrochemical series resistance,higher CE value,and better cycling stability in a wide range of current densities and number of cycles.Moreover,S-CNH-based LMAs showed high electrochemical performance in full-cell Li-S battery tests using a sulfur copolymer cathode,where a high energy density of 1370Wh kgelectrode−1 and an excellent power density of 4120Wkgelectrode−1 were obtained.
基金supported by the National High Technology Research and Development Program of China(863 Program)(2012AA053305)the International Cooperation Project from Ministry of Science and Technology of China(2010DFA64080)
文摘In this work, the morphologies and pore structures of a series of corncob-derived activated carbons and zeolite templated carbon with ultrahigh surface area were carefully investigated by SEM, HRTEM and N2-sorption characterization technologies. The high-pressure hydrogen uptake performance was analyzed using standard Pressure-Composition-Temperature apparatus in order to study the pore size effects on hydrogen uptake. These as-obtained porous carbons showed different characteristics of pore size distribution as well as specific surface area. The results indicate that the most effective pores for adsorbing hydrogen depended on the storage pressure. These ultramicropores (0.65-0.85 nm) could be the most effective pores on excess H2 uptake at 1 bar, however, micropores (0.85-2 nm) would play a more important role in excess H2 uptake at higher pressure at 77 K. At room temperature, pore size effects on H2 uptake capacity were very weak. Both specific surface area and total pore volume play more important roles than pore size for H2 uptake at room temperature, which was clearly different from that at 77 K. For applications in future, the corncob-derived activated carbons can be more available than zeolite templated carbons at 77 K. Element doping enhanced hydrogen uptake could be main research direction for improving H2 uptake capacity at room temperature.
基金the National Key Basic Research Program of China (2015CB351903)the National Natural Science Foundation of China (51402282, 51373160,21474095, 21476104, 21373197)+1 种基金the Fundamental Research Funds for the Central Universities (WK3430000003)the 100 Talents Program of the Chinese Academy of Sciences
文摘NS codoped carbon nanorods(NS-CNRs) were prepared using crab shell as template and polyphenylene sulfide(PPS) as both the C and S precursor, followed by carbonization in NH_3. The as-obtained NS-CNRs had a diameter of ~50 nm, length of several micrometers, and N and S contents of 12.5 at.% and 3.7 at.%,respectively, which can serve as anodes for both lithium-ion batteries(LIBs) and sodium ion batteries(SIBs). When serving as an anode of LIB, the NS-CNRs delivered gravimetric capacities of 2154 mAh g^(-1)at current densities of 0.1 A g^(-1)and 625 mAh g^(-1)at current densities of 5.0 A g^(-1)for 1000 cycles.When serving as an anode of SIB, the NS-CNRs delivered gravimetric capacities of 303 mAh g^(-1)at current densities of 0.1 A g^(-1)and 230 mAh g^(-1)at current densities of 1.0 A g^(-1)for 3000 cycles. The excellent electrochemical performance of NS-CNRs could be ascribed to the one-dimensional nanometer structure and high level of heteroatom doping. We expect that the obtained NS-CNRs would benefit for the future development of the doped carbon materials for lithium ion batteries and other extended applications such as supercapacitor, catalyst and hydrogen storage.
基金supported by the National Natural Science Foundation of China(Nos.21303129,5110218,51572103,51502272,21303080,41502030)the Fundamental Research Funds(Nos.CUG140620,CUGL150413,G1323511668,G1323511543)for the Central Universities,China University of Geosciences(Wuhan)+1 种基金Zhejiang Provincial Natural Science Foundation of China(Nos.LZ16E020001 and LQY18D020001)Open Project from Inner Mongolia Key Lab of Carbon Nanomaterials(No.MDK2017022)
文摘Tuning porous structure of carbon nanomaterials has been found to be important for their performance enhancement in electrochemical energy storage applications. In this work we employed a natural nanomaterial kaolinite, which is abundant and cheap, as hard template to synthesis porous carbon nanomaterial. By tuning the structure of hard template kaolinite, we have achieved a template directed formation of holey carbon nanosheet/nanotube materials. This carbon nanomaterials with hierarchical in-plane and out-of-plane pores have shown electrochemical energy storage capacity of 286 F/g(equal to 314 F/cm^3) at 0.1 A/g and 85 F/g(equal to 93 F/cm^3) at 100 A/g, which is comparable to variety of reported carbon based electrochemical energy storage electrode materials.
基金financial support from the National Program on Key Basic Research Project of China (No. 2014CB239701)the National Natural Science Foundation of China (Nos. 51372116, 51672128, 21773118)+1 种基金Prospective Joint Research Project of Cooperative Innovation Fund of Jiangsu Province (No. BY2015003-7)Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)
文摘Hybrid ion capacitors have been considered as a very attractive energy source with high energy density and power density since it combines both merits of lithium ion batteries and supercapacitors. However,their commercial application has been limited by the mismatch of charge-storage capacity and electrode kinetics between the capacitor-type cathode and battery-type anode. Herein, B and N dual-doped 3D superstructure carbon cathode is prepared through a facile template method. It delivers a high specific capacity, excellent rate capability and good cycling stability due to the B, N dual-doping, which has a profound effect in control the porosity, functional groups, and electronic conductivity for the carbon cathode. The hybrid ion capacitors using B, N dual-doping carbon cathode and prelithiated graphite anode show a high energy density of 115.5 Wh/kg at 250 W/kg and remain about 53.6 Wh/kg even at a high power density of 10 kW/kg. Additionally, the novel hybrid device achieves 76.3% capacity retention after 2000 cycles tested at 1250 W/kg power density. Significantly, the simultaneous manipulation of heteroatoms in carbon materials provides new opportunities to boost the energy and power density for hybrid ion capacitors.