P2型层状过渡金属氧化物(P2-Na_(x)TMO_(2))因其优异的循环稳定性和倍率性能,成为钠离子电池正极材料的有力候选者。然而,其在高电压下的不可逆相变和固有低理论容量问题,阻碍了实际应用。本研究工作提出高熵策略与双相结构的协同设计...P2型层状过渡金属氧化物(P2-Na_(x)TMO_(2))因其优异的循环稳定性和倍率性能,成为钠离子电池正极材料的有力候选者。然而,其在高电压下的不可逆相变和固有低理论容量问题,阻碍了实际应用。本研究工作提出高熵策略与双相结构的协同设计来克服这些挑战。通过在P2相高熵基体中引入O3相,构建新型P2/O3双相高熵层状氧化物Na_(0.70)Ni_(0.25)Mn_(0.35)Co_(0.15)Fe_(0.05)Ti_(0.20)O_(2)(简称Na_(0.70)NMCFT)。其中,高熵设计通过构型熵稳定效应有效抑制P2相的不可逆相变,而O3相则通过协同作用弥补容量不足并提升循环稳定性。此外,双相组分之间的相互作用进一步促进P2-O3与P2-P3相变的高度可逆性。Na_(0.70)NMCFT在1C倍率下的初始放电容量为102.08 mAhg^(-1),200次循环后容量保持率达88.15%,表明具有优异的循环稳定性。更重要的是,即使在10C的高倍率下,Na_(0.70)NMCFT仍能提供85.67 mAh g^(-1)的初始放电比容量,并在1000次循环后容量保持率达70%。本工作证实双相高熵设计在提升钠离子电池正极性能中的关键作用,为开发先进钠离子电池正极材料提供了新思路。展开更多
Supercritical fluids play a crucial role in material transport within Earth's deep interior.Investigating the pressure-dependent atomic structures and transport properties of such fluids is essential for understan...Supercritical fluids play a crucial role in material transport within Earth's deep interior.Investigating the pressure-dependent atomic structures and transport properties of such fluids is essential for understanding their petrological,chemical,and geophysical behaviors.In this study,we employed first-principles molecular dynamics simulations to explore the structures,self-diffusion coefficients(D),and viscosities(η)of supercritical NaAlSi_(3)O_(8)-H_(2)O fluids under conditions of 2000 K and 3-10 GPa,with water contents of 30 wt% and 50 wt%.Our calculations indicate that at a water content of 30 wt%,Q^(2) and Q^(3) exhibit a certain degree of positive and negative pressure dependence,respectively,while other Q^(n) species(n represents the number of bridging oxygens connected to Si/Al)show minimal changes.At a water content of 50 wt%,Q^(2) and Q^(0) exhibit a certain degree of positive and negative pressure dependence,respectively,while other Q^(n) species show minimal changes.At both water contents,Si-O-H and molecular water in the system exhibit negative pressure dependence,suggesting that the migration of supercritical fluids from deep to shallow regions is accompanied by the release of water.The self-diffusion coefficients in the supercritical NaAlSi_(3)O_(8)-H_(2)O fluid follow the order D_(Na)≈D_(H)>D_(O)>D_(Al)≈D_(Si),with an overall weak negative pressure dependence.By comparing the viscosities of anhydrous and hydrous silicate melts from previous studies,we found that the addition of water caused a transition from negative to positive pressure dependence of viscosity,corresponding to a structural change from polymerization to depolymerization.Additionally,we calculated the fluid mobility Δp/η of supercritical NaAlSi_(3)O_(8)-H_(2)O fluids and found that their mobility is several orders of magnitude higher than that of basalt melt and is also significantly greater than that of carbonate melt.As supercritical fluids ascend from deeper to shallower regions,their mobility is further enhanced,significantly contributing to the transport of elements from subducting slabs to the overlying mantle wedge.展开更多
Through measuring the coefficient of linear expansion, the structure and properties of the Li2O-Al2O3-SiO2 low expansion glass ceramics containing B2O3 are studied by JR and XRD. It is shoutn that the IR method is eff...Through measuring the coefficient of linear expansion, the structure and properties of the Li2O-Al2O3-SiO2 low expansion glass ceramics containing B2O3 are studied by JR and XRD. It is shoutn that the IR method is efficient in the study of the glass-ceramics structure. There is a " Boron abnormality" in the system which has an important influence on the properties of the glass-ceramics.展开更多
The commonly-employed material for thermal barrier coatings(TBCs)is 7 wt.%Y2O3 ZrO2(7YSZ),generally deposited by electron beam-physical vapor deposition(EB-PVD).Due to the increasing demand for higher operating temper...The commonly-employed material for thermal barrier coatings(TBCs)is 7 wt.%Y2O3 ZrO2(7YSZ),generally deposited by electron beam-physical vapor deposition(EB-PVD).Due to the increasing demand for higher operating temperature in aero-derivative gas turbines,a lot of effort has been made to prevent the premature failure of columnar 7YSZ TBCs,which is induced by the microstructure degradation,sintering and spallation after the deposition of infiltrated siliceous mineral(consisting of calcium magnesium aluminum silicate(CaO MgO Al2O3 SiO2,i.e.,CMAS)).A new method called Al-modification for columnar 7YSZ TBCs against CMAS corrosion was present.The Al film was magnetron-sputtered on the surface of the columnar 7YSZ TBCs,followed by performing vacuum heat treatment of the Al-deposited TBCs.During the heat treatment,the molten Al reacted with ZrO2 to formα-Al2O3 overlay that effectively hindered CMAS infiltration.Moreover,the Al film could evaporate and re-nucleate,leading to the generation of Al2O3 nanowires,which further restrained the moving of molten CMAS.展开更多
文摘P2型层状过渡金属氧化物(P2-Na_(x)TMO_(2))因其优异的循环稳定性和倍率性能,成为钠离子电池正极材料的有力候选者。然而,其在高电压下的不可逆相变和固有低理论容量问题,阻碍了实际应用。本研究工作提出高熵策略与双相结构的协同设计来克服这些挑战。通过在P2相高熵基体中引入O3相,构建新型P2/O3双相高熵层状氧化物Na_(0.70)Ni_(0.25)Mn_(0.35)Co_(0.15)Fe_(0.05)Ti_(0.20)O_(2)(简称Na_(0.70)NMCFT)。其中,高熵设计通过构型熵稳定效应有效抑制P2相的不可逆相变,而O3相则通过协同作用弥补容量不足并提升循环稳定性。此外,双相组分之间的相互作用进一步促进P2-O3与P2-P3相变的高度可逆性。Na_(0.70)NMCFT在1C倍率下的初始放电容量为102.08 mAhg^(-1),200次循环后容量保持率达88.15%,表明具有优异的循环稳定性。更重要的是,即使在10C的高倍率下,Na_(0.70)NMCFT仍能提供85.67 mAh g^(-1)的初始放电比容量,并在1000次循环后容量保持率达70%。本工作证实双相高熵设计在提升钠离子电池正极性能中的关键作用,为开发先进钠离子电池正极材料提供了新思路。
基金funded by National Natural Science Foundation of China(42373033,Yicheng Sun)Fundamental Research Funds for the Central Universities(B240201111,Yicheng Sun)。
文摘Supercritical fluids play a crucial role in material transport within Earth's deep interior.Investigating the pressure-dependent atomic structures and transport properties of such fluids is essential for understanding their petrological,chemical,and geophysical behaviors.In this study,we employed first-principles molecular dynamics simulations to explore the structures,self-diffusion coefficients(D),and viscosities(η)of supercritical NaAlSi_(3)O_(8)-H_(2)O fluids under conditions of 2000 K and 3-10 GPa,with water contents of 30 wt% and 50 wt%.Our calculations indicate that at a water content of 30 wt%,Q^(2) and Q^(3) exhibit a certain degree of positive and negative pressure dependence,respectively,while other Q^(n) species(n represents the number of bridging oxygens connected to Si/Al)show minimal changes.At a water content of 50 wt%,Q^(2) and Q^(0) exhibit a certain degree of positive and negative pressure dependence,respectively,while other Q^(n) species show minimal changes.At both water contents,Si-O-H and molecular water in the system exhibit negative pressure dependence,suggesting that the migration of supercritical fluids from deep to shallow regions is accompanied by the release of water.The self-diffusion coefficients in the supercritical NaAlSi_(3)O_(8)-H_(2)O fluid follow the order D_(Na)≈D_(H)>D_(O)>D_(Al)≈D_(Si),with an overall weak negative pressure dependence.By comparing the viscosities of anhydrous and hydrous silicate melts from previous studies,we found that the addition of water caused a transition from negative to positive pressure dependence of viscosity,corresponding to a structural change from polymerization to depolymerization.Additionally,we calculated the fluid mobility Δp/η of supercritical NaAlSi_(3)O_(8)-H_(2)O fluids and found that their mobility is several orders of magnitude higher than that of basalt melt and is also significantly greater than that of carbonate melt.As supercritical fluids ascend from deeper to shallower regions,their mobility is further enhanced,significantly contributing to the transport of elements from subducting slabs to the overlying mantle wedge.
文摘Through measuring the coefficient of linear expansion, the structure and properties of the Li2O-Al2O3-SiO2 low expansion glass ceramics containing B2O3 are studied by JR and XRD. It is shoutn that the IR method is efficient in the study of the glass-ceramics structure. There is a " Boron abnormality" in the system which has an important influence on the properties of the glass-ceramics.
基金Project(2017YFB0306100) supported by the National Key Research&Development Plan of ChinaProjects(51801034,51771059) supported by the National Natural Science Foundation of China+3 种基金Projects(2018GDASCX-0949,2018GDASCX-0950,2017GDASCX-0111) supported by the Guangdong Academy of Sciences,ChinaProjects(2017B090916002,2017A070701027) supported by the Guangdong Technical Research Program,ChinaProjects(2016A030312015,2017A030310315) supported by the Natural Science Foundation of Guangdong Province,ChinaProjects(201605131008557,201707010385) supported by the Technical Research Program of Guangzhou City,China
文摘The commonly-employed material for thermal barrier coatings(TBCs)is 7 wt.%Y2O3 ZrO2(7YSZ),generally deposited by electron beam-physical vapor deposition(EB-PVD).Due to the increasing demand for higher operating temperature in aero-derivative gas turbines,a lot of effort has been made to prevent the premature failure of columnar 7YSZ TBCs,which is induced by the microstructure degradation,sintering and spallation after the deposition of infiltrated siliceous mineral(consisting of calcium magnesium aluminum silicate(CaO MgO Al2O3 SiO2,i.e.,CMAS)).A new method called Al-modification for columnar 7YSZ TBCs against CMAS corrosion was present.The Al film was magnetron-sputtered on the surface of the columnar 7YSZ TBCs,followed by performing vacuum heat treatment of the Al-deposited TBCs.During the heat treatment,the molten Al reacted with ZrO2 to formα-Al2O3 overlay that effectively hindered CMAS infiltration.Moreover,the Al film could evaporate and re-nucleate,leading to the generation of Al2O3 nanowires,which further restrained the moving of molten CMAS.
