Optimizing the interfacial environments of electrodes has emerged as an effective strategy to improve their electrochemical properties.Amorphous/crystalline interfacial coupling can effectively utilize the advantages ...Optimizing the interfacial environments of electrodes has emerged as an effective strategy to improve their electrochemical properties.Amorphous/crystalline interfacial coupling can effectively utilize the advantages of amorphous materials to optimize the interfacial structure for efficient Na^(+)storage.Herein,the dense homologous amorphous/crystalline heterointerfaces are in situ achieved in N-doped carbon nanobundles via self-polymerization and precise nitriding(Mo–N/Mo_(2)N@C).The amorphous Mo–N rich in unsaturated vacancy defects provides abundant active sites with isotropic ion-transport channels,and can effectively alleviate structural stress from crystalline Mo_(2)N.Meanwhile,the conductive Mo_(2)N can facilitate effective electron transfer,augmented further by the carbon encapsulation.Theoretical calculations reveal that the dense heterointerfaces can optimize the electronic structure and shift the d-p orbital centers of Mo and N upward,thereby enhancing the adsorption and mobility of Na^(+),and ultimately improving the charge transport and storage efficiency of the electrode.The Mo–N/Mo_(2)N@C as an anode delivers a 46.9%increase in reversible capacity over Mo_(2)N@C,reaching 461.1 m Ah.g^(–1)at 0.1 A.g^(–1),along with improved rate capability and cycling stability,underlining its practical utility.These results suggest that the homologous interfacial coupling can boost the storage properties of nitrides,providing a valuable reference for improving the properties of electrodes with low theoretical capacities.展开更多
Carbon-based materials have become a research hotspot in the field of energy storage devices in recent years due to their abundant resources,low cost,and environmental friendliness.However,the low capacity and poor hi...Carbon-based materials have become a research hotspot in the field of energy storage devices in recent years due to their abundant resources,low cost,and environmental friendliness.However,the low capacity and poor high rate performance still constitute great challenges.Metal organic framework-derived carbon has been widely researched because of its high porosity,tunable structure,and good conductivity.In this work,N/S codoped hierarchical porous carbon microspheres were prepared by a high-temperature heat treatment and atomic doping process using a zinc-based organic framework as the precursor.When used as a potassium-ion battery anode,it has a high reversible specific capacity(435.7 mAh g^(-1)),good rate performance(133.5 mAh g^(-1)at 10,000 m A g^(-1)),and long-term cycling stability(73.2%capacity retention after the 2500th cycle).The potassium storage mechanism of the derived carbon was explained by various electrochemical analysis methods and microstructure characterization techniques,and the relationship between the structural characteristics and electrochemical properties was researched.In a supercapacitor,the porous carbon material exhibits a specific capacitance of 307.2 F g^(-1)at a current density of 0.2 A g^(-1)in a KOH aqueous solution and achieves a retention rate of 99.88%after 10,000 cycles.The assembled symmetric supercapacitor device delivers a high energy density of 6.69 Wh kg^(-1),with a corresponding power density of 2500 W kg^(-1).In addition,density functional theory calculations further confirmed that N/S codoping can improve the adsorption capacities of potassium and hydroxyl ions in the derived carbon.展开更多
Mo-C codoped TiO2 films were prepared by RF magnetron cosputtering. Ultraviolet-visible spectroscopy, atomic force microscopy, X-ray photoelectron spectroscopy, energy dispersive X-ray Analysis and X-Ray Diffraction w...Mo-C codoped TiO2 films were prepared by RF magnetron cosputtering. Ultraviolet-visible spectroscopy, atomic force microscopy, X-ray photoelectron spectroscopy, energy dispersive X-ray Analysis and X-Ray Diffraction were used to study the influences of codoping on energy gap, surface morphology, valence states of elements, ions content and crystal structure, respectively. The concentration of photogenerated carriers was measured by studying photocurrent density, while catalytic property was evaluated by observing degradation rate of methylene blue under visible light. A Mo-doped TiO2 film, whose content of Mo had been optimized in advance, was prepared and later used for subsequent comparisons with codoped samples. The result indicates that Mo-C codoping could curtail the energy gap and shift the absorption edge toward visible range. Under the illumination of visible light, codoped TiO2 films give rise to stronger photocurrent due to smaller band gaps. It is also found that Mo, C codoping results in a porous surface, whose area declines gradually with increasing carbon content. Carbon and Molybdenum doses were delicately optimized. Under the illumination of visible light, sample doped with 9.78at% carbon and 0.36at% Mo presents the strongest photocurrent which is about 8 times larger than undoped TiO2 films, and about 6 times larger than samples doped with Mo only.展开更多
基金financially supported by the National Natural Science Foundation of China(No.51762021)the Natural Science Foundation of Jiangxi province(Nos.20224ACB204008,20242BAB25223,and 20242BAB25248)the Special Funding Program for Graduate Student Innovation of Jiangxi Province(No.YC2024-S594)。
文摘Optimizing the interfacial environments of electrodes has emerged as an effective strategy to improve their electrochemical properties.Amorphous/crystalline interfacial coupling can effectively utilize the advantages of amorphous materials to optimize the interfacial structure for efficient Na^(+)storage.Herein,the dense homologous amorphous/crystalline heterointerfaces are in situ achieved in N-doped carbon nanobundles via self-polymerization and precise nitriding(Mo–N/Mo_(2)N@C).The amorphous Mo–N rich in unsaturated vacancy defects provides abundant active sites with isotropic ion-transport channels,and can effectively alleviate structural stress from crystalline Mo_(2)N.Meanwhile,the conductive Mo_(2)N can facilitate effective electron transfer,augmented further by the carbon encapsulation.Theoretical calculations reveal that the dense heterointerfaces can optimize the electronic structure and shift the d-p orbital centers of Mo and N upward,thereby enhancing the adsorption and mobility of Na^(+),and ultimately improving the charge transport and storage efficiency of the electrode.The Mo–N/Mo_(2)N@C as an anode delivers a 46.9%increase in reversible capacity over Mo_(2)N@C,reaching 461.1 m Ah.g^(–1)at 0.1 A.g^(–1),along with improved rate capability and cycling stability,underlining its practical utility.These results suggest that the homologous interfacial coupling can boost the storage properties of nitrides,providing a valuable reference for improving the properties of electrodes with low theoretical capacities.
基金supported by the National Natural Science Foundation of China (51764029, 52004116)the National Key Research and Development Program of China (2019YFC1803501)+1 种基金the Applied Basic Research Plan of Yunnan Province(202001AU070039, 2018FB087)the Science Research Foundation of Yunnan Provincial Department of Education (2020J0070)
文摘Carbon-based materials have become a research hotspot in the field of energy storage devices in recent years due to their abundant resources,low cost,and environmental friendliness.However,the low capacity and poor high rate performance still constitute great challenges.Metal organic framework-derived carbon has been widely researched because of its high porosity,tunable structure,and good conductivity.In this work,N/S codoped hierarchical porous carbon microspheres were prepared by a high-temperature heat treatment and atomic doping process using a zinc-based organic framework as the precursor.When used as a potassium-ion battery anode,it has a high reversible specific capacity(435.7 mAh g^(-1)),good rate performance(133.5 mAh g^(-1)at 10,000 m A g^(-1)),and long-term cycling stability(73.2%capacity retention after the 2500th cycle).The potassium storage mechanism of the derived carbon was explained by various electrochemical analysis methods and microstructure characterization techniques,and the relationship between the structural characteristics and electrochemical properties was researched.In a supercapacitor,the porous carbon material exhibits a specific capacitance of 307.2 F g^(-1)at a current density of 0.2 A g^(-1)in a KOH aqueous solution and achieves a retention rate of 99.88%after 10,000 cycles.The assembled symmetric supercapacitor device delivers a high energy density of 6.69 Wh kg^(-1),with a corresponding power density of 2500 W kg^(-1).In addition,density functional theory calculations further confirmed that N/S codoping can improve the adsorption capacities of potassium and hydroxyl ions in the derived carbon.
基金Funded by Chinese National Key Scientific Projects(No.2012CB934303)the Guizhou Education Foundation(KY[2015]332)
文摘Mo-C codoped TiO2 films were prepared by RF magnetron cosputtering. Ultraviolet-visible spectroscopy, atomic force microscopy, X-ray photoelectron spectroscopy, energy dispersive X-ray Analysis and X-Ray Diffraction were used to study the influences of codoping on energy gap, surface morphology, valence states of elements, ions content and crystal structure, respectively. The concentration of photogenerated carriers was measured by studying photocurrent density, while catalytic property was evaluated by observing degradation rate of methylene blue under visible light. A Mo-doped TiO2 film, whose content of Mo had been optimized in advance, was prepared and later used for subsequent comparisons with codoped samples. The result indicates that Mo-C codoping could curtail the energy gap and shift the absorption edge toward visible range. Under the illumination of visible light, codoped TiO2 films give rise to stronger photocurrent due to smaller band gaps. It is also found that Mo, C codoping results in a porous surface, whose area declines gradually with increasing carbon content. Carbon and Molybdenum doses were delicately optimized. Under the illumination of visible light, sample doped with 9.78at% carbon and 0.36at% Mo presents the strongest photocurrent which is about 8 times larger than undoped TiO2 films, and about 6 times larger than samples doped with Mo only.
