Charging P2-Na_(2/3)Ni_(1/3)Mn_(2/3)O_(2)to 4.5 V for higher capacity is enticing.However,it leads to severe capacity fading,ascribing to the lattice oxygen evolution and the P2-O2 phase transformation.Here,the Mg Fe_...Charging P2-Na_(2/3)Ni_(1/3)Mn_(2/3)O_(2)to 4.5 V for higher capacity is enticing.However,it leads to severe capacity fading,ascribing to the lattice oxygen evolution and the P2-O2 phase transformation.Here,the Mg Fe_(2)O_(4) coating and Mg,Fe co-doping were constructed simultaneously by Mg,Fe surface treatment to suppress lattice oxygen evolution and P2-O2 phase transformation of P2-Na_(2/3)Ni_(1/3)Mn_(2/3)O_(2)at deep charging.Through ex-situ X-ray diffraction(XRD)tests,we found that the Mg,Fe bulk co-doping could reduce the repulsion between transition metals and Na+/vacancies ordering,thus inhibiting the P2-O2 phase transition and significantly reducing the irreversible volume change of the material.Meanwhile,the internal electric field formed by the dielectric polarization of Mg Fe_(2)O_(4) effectively inhibits the outward migration of oxidized O^(a-)(a<2),thereby suppressing the lattice oxygen evolution at deep charging,confirmed by in situ Raman and ex situ XPS techniques.P2-Na NM@MF-3 shows enhanced high-voltage cycling performance with capacity retentions of 84.8% and 81.3%at 0.1 and 1 C after cycles.This work sheds light on regulating the surface chemistry for Na-layered oxide materials to enhance the high-voltage performance of Na-ion batteries.展开更多
Temperature is a fundamental thermodynamic variable for matter.Physical observables are often found to either increase or decrease with it,or show a non-monotonic dependence with peaks signaling underlying phase trans...Temperature is a fundamental thermodynamic variable for matter.Physical observables are often found to either increase or decrease with it,or show a non-monotonic dependence with peaks signaling underlying phase transitions or anomalies.Statistical Held theory has established connection between temperature and time:a quantum ensemble with inverse temperatureβis formally equivalent to a dynamic system evolving along an imaginary time from 0 to iβin the space one dimension higher.Here we report that a gas of hard-core bosons interacting with a thermal bath manifests an unexpected temperature-periodic oscillation of its macroscopic observables,arising from the microscopic origin of space-time locked translational symmetry breaking and crystalline ordering.Such a temperature crystal,supported by quantum Monte Carlo simulation,generalizes the concept of purely spatial density-wave order to the imaginary time axis for Euclidean action.展开更多
基金supported by the Special Project for the Central Government to Guide Local Technological Development (GUIKE ZY20198008)the Guangxi Technology Base and talent Subject (GUIKE AD20238012,AD20297086)+5 种基金the Natural Science Foundation of Guangxi Province (2021GXNSFDA075012)the National Natural Science Foundation of China (51902108,52104298,22169004)the National Natural Science Foundation of China (U20A20249)the Regional Innovation and Development Joint Fundthe Guangxi Innovation Driven Development Subject (GUIKE AA19182020,19254004)the Special Fund for Guangxi Distinguished Expert。
文摘Charging P2-Na_(2/3)Ni_(1/3)Mn_(2/3)O_(2)to 4.5 V for higher capacity is enticing.However,it leads to severe capacity fading,ascribing to the lattice oxygen evolution and the P2-O2 phase transformation.Here,the Mg Fe_(2)O_(4) coating and Mg,Fe co-doping were constructed simultaneously by Mg,Fe surface treatment to suppress lattice oxygen evolution and P2-O2 phase transformation of P2-Na_(2/3)Ni_(1/3)Mn_(2/3)O_(2)at deep charging.Through ex-situ X-ray diffraction(XRD)tests,we found that the Mg,Fe bulk co-doping could reduce the repulsion between transition metals and Na+/vacancies ordering,thus inhibiting the P2-O2 phase transition and significantly reducing the irreversible volume change of the material.Meanwhile,the internal electric field formed by the dielectric polarization of Mg Fe_(2)O_(4) effectively inhibits the outward migration of oxidized O^(a-)(a<2),thereby suppressing the lattice oxygen evolution at deep charging,confirmed by in situ Raman and ex situ XPS techniques.P2-Na NM@MF-3 shows enhanced high-voltage cycling performance with capacity retentions of 84.8% and 81.3%at 0.1 and 1 C after cycles.This work sheds light on regulating the surface chemistry for Na-layered oxide materials to enhance the high-voltage performance of Na-ion batteries.
基金National Key Research and Development Program of China(Grant No.2016YFA0302001)National Natural Science Foundation of China(Grant Nos.11674221 and 11745006)+5 种基金Shanghai Rising-Star ProgramEastern Scholar Professor of Distinguished Appointment Programthe AFOSR(Grant No.FA9550-16-1-0006)MURI-ARO(Grant No.W911NF-17-1-0323)through UC Santa Barbara,the NSF China Overseas Scholar Collaborative Program(Grant No.11429402)Shanghai Municipal Science and Technology Major Project(Grant No.2019SHZDZX01)。
文摘Temperature is a fundamental thermodynamic variable for matter.Physical observables are often found to either increase or decrease with it,or show a non-monotonic dependence with peaks signaling underlying phase transitions or anomalies.Statistical Held theory has established connection between temperature and time:a quantum ensemble with inverse temperatureβis formally equivalent to a dynamic system evolving along an imaginary time from 0 to iβin the space one dimension higher.Here we report that a gas of hard-core bosons interacting with a thermal bath manifests an unexpected temperature-periodic oscillation of its macroscopic observables,arising from the microscopic origin of space-time locked translational symmetry breaking and crystalline ordering.Such a temperature crystal,supported by quantum Monte Carlo simulation,generalizes the concept of purely spatial density-wave order to the imaginary time axis for Euclidean action.
