Inferior cycling stability, poor safety, and gas generation are long lasting problems of Ni-rich Li Ni0.80 Co0.10 Mn0.10 O2(NCM811) cathode material. Although much effort has been made, mechanisms for the above proble...Inferior cycling stability, poor safety, and gas generation are long lasting problems of Ni-rich Li Ni0.80 Co0.10 Mn0.10 O2(NCM811) cathode material. Although much effort has been made, mechanisms for the above problems are poorly understood. Studying the cycling and float-charging characteristics of Li/NCM811 cells in high voltage conditions(4.5 V and 4.7 V, respectively), in this work we find that nearly all known problems with NCM811 material can be attributed to the oxidation of lattice oxygen occurring in the capacity region corresponding to H2 → H3 phase transition. While contributing to overall capacity,the oxidation of lattice oxygen results in a loss of oxygen through oxygen evolution and relative reactions between active oxygen evolution intermediates and electrolyte solvents. It is the loss of oxygen that results in irreversible layered-spinel-rocksalt phase transition, secondary particle cracking, and performance degradation. The conclusions of this work suggest that the priority for further research on NCM811 material should give to the suppression of oxygen evolution, followed by the use of the anti-oxygen electrolyte being chemically stable against the active oxygen evolution intermediates.展开更多
The 26 plots including natural forestland, secondary forestland, shrub-grassland, sloping cropland, artificial forest and abandoned field, were selected to discuss the impact of land cover on the soil characteristics ...The 26 plots including natural forestland, secondary forestland, shrub-grassland, sloping cropland, artificial forest and abandoned field, were selected to discuss the impact of land cover on the soil characteristics in the three karst districts of Chongqing. The results showed that： （1） After the vegetation turned into secondary vegetation or artificial vegetation, or reclamation, soil physical properties would be degraded. In the surface-layer soil of sloping cropland, the contents of 〉2 mm water-stable aggregates decreased obviously with apparent sandification. （2） The contents of soil organic matter and total nitrogen are controlled completely by vegetation type and land use intensity. The increasing trend is rather slow in the early days when over-reclamation is stopped and the land is converted to forest and pasture. （3） Herbaceous species increase and woody plants species decrease with the increase of land use intensity, therefore, the soil seed banks degrade more seriously. （4） The soil degradation index has been set up to describe the relative soil degradation degree under the conditions of different vegetation types. （5） Land cover has a significant effect on karst soil characteristics, land degradation in the karst ecosystem is essentially characterized by the different degradation of soil functions that serve as water banks, nutrient banks and soil seed banks.展开更多
Porous g-C_3N_4 and supported porous g-C_3N_4 were fabricated for the first time by a simple strategy using pretreated melamine as a raw material and pretreated quartz rod as a substrate.The formation of a richly poro...Porous g-C_3N_4 and supported porous g-C_3N_4 were fabricated for the first time by a simple strategy using pretreated melamine as a raw material and pretreated quartz rod as a substrate.The formation of a richly porous microstructure can be attributed to the co-existence of different pore-fabricating units in the preparation system for porous g-C_3N_4.The richly porous microstructure endowed the as-prepared porous g-C_3N_4 with an excellent photocatalytic activity.The as-prepared supported porous g-C_3N_4 exhibited considerable stability because of the existence of chemical interaction between porous g-C_3N_4 and the quartz rod substrate.The photocatalytic activity of the supported porous g-C_3N_4 was competitive with that of porous g-C_3N_4 in powder form because neither the surface migration of photogenerated electrons nor the diffusion of the target organic pollutant were affected by the construction of the quartz rod reactor.The photocatalytic activity of the as-prepared porous g-C_3N_4 and supported porous g-C_3N_4 was preliminarily evaluated by the treatment of single-component organic wastewater under visible-light irradiation.Subsequently,the as-prepared porous g-C_3N_4 was further applied in conventional hydrogen evolution and a new system for simultaneous hydrogen evolution with organic-pollutant degradation.The hydrogen yield and degradation efficiency both increased with increasing photocatalytic activity of the as-prepared materials in the system for simultaneous hydrogen evolution with organic-pollutant degradation.展开更多
Transition metal carbides and nitrides(MXenes)nanosheets are attractive two-dimensional(2D)materials,but they suffer from oxidation/degradation issues during storage and/or applications due to their sensitivity to wat...Transition metal carbides and nitrides(MXenes)nanosheets are attractive two-dimensional(2D)materials,but they suffer from oxidation/degradation issues during storage and/or applications due to their sensitivity to water and oxygen.Despite the great research progress,the exact oxidation kinetics of Ti_(3)C_(2)T_(x)(MXene)and their final products after oxidation are not fully understood.Herein,we systematically tracked the oxidation process of few-layer Ti_(3)C_(2)T_(x) nanosheets in an aqueous solution at room temperature over several weeks.We also studied the oxidation effects on the electrocatalytic properties of Ti_(3)C_(2)T_(x) for hydrogen evolution reaction and found that the overpotential to achieve a current density of 10 mA cm^(-2)increases from 0.435 to 0.877 V after three weeks of degradation,followed by improvement to stabilized values of around 0.40 V after eight weeks.These results suggest that severely oxidized MXene could be a promising candidate for designing efficient catalysts.According to our detailed experimental characterization and theoretical calculations,unlike previous studies,black titanium oxide is formed as the final product in addition to white Ti(IV)oxide and disordered carbons after the complete oxidation of Ti_(3)C_(2)T_(x).This work presents significant advancements in better understanding of 2D Ti_(3)C_(2)T_(x)(MXene)oxidation and enhances the prospects of this material for various applications.展开更多
In this paper, we develop dynamic statistical information theory established by the author. Starting from the ideas that the state variable evolution equations of stochastic dynamic systems, classical and quantum none...In this paper, we develop dynamic statistical information theory established by the author. Starting from the ideas that the state variable evolution equations of stochastic dynamic systems, classical and quantum nonequilibrium statistical physical systems and special electromagnetic field systems can be regarded as their information symbol evolution equations and the definitions of dynamic information and dynamic entropy, we derive the evolution equations of dynamic information and dynamic entropy that describe the evolution laws of dynamic information. These four kinds of evolution equations are of the same mathematical type. They show in unison when information transmits in coordinate space outside the systems that the time rate of change of dynamic information densities originates from their drift, diffusion and dissipation in state variable space inside the systems and coordinate space in the transmission processes, and that the time rate of change of dynamic entropy densities is caused by their drift, diffusion and production in state variable space inside the systems and coordinate space in the transmission processes. When space noise can be neglected, an information wave will appear. If we only consider the information change inside the systems, dynamic information evolution equations reduce to information equations corresponding to the dynamic equations which describe evolution laws of the above dynamic systems. This reveals that the evolution laws of respective dynamic systems can be described by information equations in a unified fashion. Hence, the evolution processes of these dynamic systems can be abstracted as the evolution processes of information. Furthermore, we present the formulas for information flow, information dissipation rate, and entropy production rate. We prove that the information production probably emerges in a dynamic system with internal attractive interaction between the elements, and derive a formula for this information production rate. Thereby, we obtain an expression for the 展开更多
Delivering excellent carrier separation through ferroelectric polarization is desirable to achieve effective solar hydrogen conversion.Here,Bi_(0.9)Dy_(0.1)FeO_(3)/g-C_(3)N_(4)(BDFO/GCN)Z-scheme photocatalyst was cons...Delivering excellent carrier separation through ferroelectric polarization is desirable to achieve effective solar hydrogen conversion.Here,Bi_(0.9)Dy_(0.1)FeO_(3)/g-C_(3)N_(4)(BDFO/GCN)Z-scheme photocatalyst was constructed by loading BDFO nanoparticles onto sheet-like GCN,in which BiFeO_(3)(BFO)was doped with the rare-earth element Dy to narrow the optical bandgap and enhance the ferroelectric property.Residual polarization effectively promoted the separation and transport of photo-generated carriers in BFO,and the Z-scheme exhibited stable reaction activity during photocatalytic degradation and photocatalytic hydrogen evolution.Through electric polarization,the heterojunction photocatalyst achieves 100%degradation of Rhodamine B(RhB)under simulated sunlight.The evolution rate of hydrogen was improved from approximately 742.5 to 1084.0μmol·g^(−1)·h^(−1)after polarization.This remarkable activity is attributed to the improved carrier separation facilitated by the internal polarization field.This work offers novel insights into the rational design of efficient ferroelectric photocatalysts.展开更多
文摘Inferior cycling stability, poor safety, and gas generation are long lasting problems of Ni-rich Li Ni0.80 Co0.10 Mn0.10 O2(NCM811) cathode material. Although much effort has been made, mechanisms for the above problems are poorly understood. Studying the cycling and float-charging characteristics of Li/NCM811 cells in high voltage conditions(4.5 V and 4.7 V, respectively), in this work we find that nearly all known problems with NCM811 material can be attributed to the oxidation of lattice oxygen occurring in the capacity region corresponding to H2 → H3 phase transition. While contributing to overall capacity,the oxidation of lattice oxygen results in a loss of oxygen through oxygen evolution and relative reactions between active oxygen evolution intermediates and electrolyte solvents. It is the loss of oxygen that results in irreversible layered-spinel-rocksalt phase transition, secondary particle cracking, and performance degradation. The conclusions of this work suggest that the priority for further research on NCM811 material should give to the suppression of oxygen evolution, followed by the use of the anti-oxygen electrolyte being chemically stable against the active oxygen evolution intermediates.
基金Supported by the key plan of Chongqing Science and Technology Committee (6759, 7355)
文摘The 26 plots including natural forestland, secondary forestland, shrub-grassland, sloping cropland, artificial forest and abandoned field, were selected to discuss the impact of land cover on the soil characteristics in the three karst districts of Chongqing. The results showed that： （1） After the vegetation turned into secondary vegetation or artificial vegetation, or reclamation, soil physical properties would be degraded. In the surface-layer soil of sloping cropland, the contents of 〉2 mm water-stable aggregates decreased obviously with apparent sandification. （2） The contents of soil organic matter and total nitrogen are controlled completely by vegetation type and land use intensity. The increasing trend is rather slow in the early days when over-reclamation is stopped and the land is converted to forest and pasture. （3） Herbaceous species increase and woody plants species decrease with the increase of land use intensity, therefore, the soil seed banks degrade more seriously. （4） The soil degradation index has been set up to describe the relative soil degradation degree under the conditions of different vegetation types. （5） Land cover has a significant effect on karst soil characteristics, land degradation in the karst ecosystem is essentially characterized by the different degradation of soil functions that serve as water banks, nutrient banks and soil seed banks.
基金supported by the National Natural Science Foundation of China(51568049,51208248,51468043,21366024)the National Science Fund for Excellent Young Scholars(51422807)+1 种基金the Natural Science Foundation of Jiangxi Province,China(20161BAB206118,20114BAB213015)the Natural Science Foundation of Jiangxi Provincial Department of Education,China(GJJ14515,GJJ12456)~~
文摘Porous g-C_3N_4 and supported porous g-C_3N_4 were fabricated for the first time by a simple strategy using pretreated melamine as a raw material and pretreated quartz rod as a substrate.The formation of a richly porous microstructure can be attributed to the co-existence of different pore-fabricating units in the preparation system for porous g-C_3N_4.The richly porous microstructure endowed the as-prepared porous g-C_3N_4 with an excellent photocatalytic activity.The as-prepared supported porous g-C_3N_4 exhibited considerable stability because of the existence of chemical interaction between porous g-C_3N_4 and the quartz rod substrate.The photocatalytic activity of the supported porous g-C_3N_4 was competitive with that of porous g-C_3N_4 in powder form because neither the surface migration of photogenerated electrons nor the diffusion of the target organic pollutant were affected by the construction of the quartz rod reactor.The photocatalytic activity of the as-prepared porous g-C_3N_4 and supported porous g-C_3N_4 was preliminarily evaluated by the treatment of single-component organic wastewater under visible-light irradiation.Subsequently,the as-prepared porous g-C_3N_4 was further applied in conventional hydrogen evolution and a new system for simultaneous hydrogen evolution with organic-pollutant degradation.The hydrogen yield and degradation efficiency both increased with increasing photocatalytic activity of the as-prepared materials in the system for simultaneous hydrogen evolution with organic-pollutant degradation.
基金supported by the Australian Research Council (DE220100521 and DP200101217)supported by Fellow research grant of National University of Mongolia (No.P2021-4197)+2 种基金the support of Griffith University internal grantssupport from King Abdullah University of Science and Technology (KAUST)through the Ibn Rushd Postdoctoral Fellowship Awardsupport from the US Office of Naval Research (ONR),Office of Naval Research Global (ONRG)under the grant N62909-23-1-2035。
文摘Transition metal carbides and nitrides(MXenes)nanosheets are attractive two-dimensional(2D)materials,but they suffer from oxidation/degradation issues during storage and/or applications due to their sensitivity to water and oxygen.Despite the great research progress,the exact oxidation kinetics of Ti_(3)C_(2)T_(x)(MXene)and their final products after oxidation are not fully understood.Herein,we systematically tracked the oxidation process of few-layer Ti_(3)C_(2)T_(x) nanosheets in an aqueous solution at room temperature over several weeks.We also studied the oxidation effects on the electrocatalytic properties of Ti_(3)C_(2)T_(x) for hydrogen evolution reaction and found that the overpotential to achieve a current density of 10 mA cm^(-2)increases from 0.435 to 0.877 V after three weeks of degradation,followed by improvement to stabilized values of around 0.40 V after eight weeks.These results suggest that severely oxidized MXene could be a promising candidate for designing efficient catalysts.According to our detailed experimental characterization and theoretical calculations,unlike previous studies,black titanium oxide is formed as the final product in addition to white Ti(IV)oxide and disordered carbons after the complete oxidation of Ti_(3)C_(2)T_(x).This work presents significant advancements in better understanding of 2D Ti_(3)C_(2)T_(x)(MXene)oxidation and enhances the prospects of this material for various applications.
文摘In this paper, we develop dynamic statistical information theory established by the author. Starting from the ideas that the state variable evolution equations of stochastic dynamic systems, classical and quantum nonequilibrium statistical physical systems and special electromagnetic field systems can be regarded as their information symbol evolution equations and the definitions of dynamic information and dynamic entropy, we derive the evolution equations of dynamic information and dynamic entropy that describe the evolution laws of dynamic information. These four kinds of evolution equations are of the same mathematical type. They show in unison when information transmits in coordinate space outside the systems that the time rate of change of dynamic information densities originates from their drift, diffusion and dissipation in state variable space inside the systems and coordinate space in the transmission processes, and that the time rate of change of dynamic entropy densities is caused by their drift, diffusion and production in state variable space inside the systems and coordinate space in the transmission processes. When space noise can be neglected, an information wave will appear. If we only consider the information change inside the systems, dynamic information evolution equations reduce to information equations corresponding to the dynamic equations which describe evolution laws of the above dynamic systems. This reveals that the evolution laws of respective dynamic systems can be described by information equations in a unified fashion. Hence, the evolution processes of these dynamic systems can be abstracted as the evolution processes of information. Furthermore, we present the formulas for information flow, information dissipation rate, and entropy production rate. We prove that the information production probably emerges in a dynamic system with internal attractive interaction between the elements, and derive a formula for this information production rate. Thereby, we obtain an expression for the
基金supported by the National Natural Science Foundation of China(52172205,51872145).
文摘Delivering excellent carrier separation through ferroelectric polarization is desirable to achieve effective solar hydrogen conversion.Here,Bi_(0.9)Dy_(0.1)FeO_(3)/g-C_(3)N_(4)(BDFO/GCN)Z-scheme photocatalyst was constructed by loading BDFO nanoparticles onto sheet-like GCN,in which BiFeO_(3)(BFO)was doped with the rare-earth element Dy to narrow the optical bandgap and enhance the ferroelectric property.Residual polarization effectively promoted the separation and transport of photo-generated carriers in BFO,and the Z-scheme exhibited stable reaction activity during photocatalytic degradation and photocatalytic hydrogen evolution.Through electric polarization,the heterojunction photocatalyst achieves 100%degradation of Rhodamine B(RhB)under simulated sunlight.The evolution rate of hydrogen was improved from approximately 742.5 to 1084.0μmol·g^(−1)·h^(−1)after polarization.This remarkable activity is attributed to the improved carrier separation facilitated by the internal polarization field.This work offers novel insights into the rational design of efficient ferroelectric photocatalysts.
