Lithium-ion batteries(LIBs), as the first choice for green batteries, have been widely used in energy storage, electric vehicles, 3C devices, and other related fields, and will have greater application prospects in th...Lithium-ion batteries(LIBs), as the first choice for green batteries, have been widely used in energy storage, electric vehicles, 3C devices, and other related fields, and will have greater application prospects in the future. However, one of the obstacles hindering the future development of battery technology is how to accurately evaluate and monitor battery health, which affects the entire lifespan of battery use. It is not enough to assess battery health comprehensively through the state of health(SoH) alone, especially when nonlinear aging occurs in onboard applications. Here, for the first time, we propose a brand-new health evaluation indicator—state of nonlinear aging(SoNA) to explain the nonlinear aging phenomenon that occurs during the battery use, and also design a knee-point identification method and two SoNA quantitative methods. We apply our health evaluation indicator to build a complete LIB full-lifespan grading evaluation system and a ground-to-cloud service framework, which integrates multi-scenario data collection, multi-dimensional data-based grading evaluation, and cloud management functions. Our works fill the gap in the LIBs’ health evaluation of nonlinear aging, which is of great significance for the health and safety evaluation of LIBs in the field of echelon utilization such as vehicles and energy storage. In addition, this comprehensive evaluation system and service framework are expected to be extended to other battery material systems other than LIBs, yet guiding the design of new energy ecosystem.展开更多
Superionic and electride behaviors in materials,which induce a variety of exotic physical properties of ions and electrons,are of great importance both in fundamental research and for practical applications.However,th...Superionic and electride behaviors in materials,which induce a variety of exotic physical properties of ions and electrons,are of great importance both in fundamental research and for practical applications.However,their coexistence in hot alkali-metal borides has not been observed.In this work,we apply first-principles structure search calculations to identify eight Na-B compounds with host-vip structures,which exhibit a wide range of building blocks and interesting properties linked to the Na/B composition.Among the known borides,Na-rich Na9B stands out as the composition with the highest alkali-metal content,featuring vertex-and face-sharing BNa16 polyhedra.Notably,it exhibits electride characteristics and transforms into a superionic electride at 200 GPa and 2000 K,displaying unusual Na atomic diffusion behavior attributed to the modulation of the interstitial anion electrons.It demonstrates semiconductor behavior in the solid state,and metallic properties associated with Na 3p/3s states in the superionic and liquid regions.On the other hand,B-rich NaB7,consisting of a unique covalent B framework,is predicted to exhibit low-frequency phonon-mediated superconductivity with a T_(c) of 16.8 K at 55 GPa.Our work advances the understanding of the structures and properties of alkali-metal borides.展开更多
Electrides,materials in which a portion of valence electrons reside as interstitial anionic electrons(IAEs)within lattice cavities-exhibit a wide range of extraordinary physical and chemical properties,making them a c...Electrides,materials in which a portion of valence electrons reside as interstitial anionic electrons(IAEs)within lattice cavities-exhibit a wide range of extraordinary physical and chemical properties,making them a central focus of condensed matter physics.Under high pressure,intermetallic systems provide a unique pathway to novel electrides by enabling unconventional charge-transfer mechanisms.Here,we employ first-principles structure searches to identify two stable Li-Mg electrides,Li_(3)Mg and Li_(4)Mg.At low pressure,Mg atoms act as anionic centers through occupation of their outer-shell 3p orbitals.Upon compression,charge is transferred from Mg to the lattice cavities,enhancing the localization and density of IAEs.This,in turn,strengths electron-phonon coupling and raises the superconducting transition temperature(T_(c))to 13.3 K at 75 GPa for Li_(3)Mg and 19.7 K at 80 GPa for Li_(4)Mg-values that surpass most known electride superconductors below 100 GPa.Selective hydrogen insertion into the lattice cavities in Li_(4)Mg quenches the IAEs and confirms their essential role in superconductivity.Further compression drives a transition to poor or non-superconducting phases,with Mg atoms switching from electron acceptors to donors,contrary to the typical behavior of electropositive metals,which tend to transition from donors into acceptors under pressure.These findings highlight the pivotal role of IAEs in electride superconductivity and pave the way for designing novel intermetallic electrides with tunable properties.展开更多
Extended hydrogen-rich frameworks stabilized under high pressure are essential for achieving high-temperature superconductivity in metal hydrides,where metal atoms contribute both charge and intrinsic precompression.I...Extended hydrogen-rich frameworks stabilized under high pressure are essential for achieving high-temperature superconductivity in metal hydrides,where metal atoms contribute both charge and intrinsic precompression.In contrast,p-block nonmetal hydrides lack such extended hydrogenic connectivity.Here,using first-principles crystal structure search calculations,we identify three nitrogen-based superhydrides-NH_(10),NH_(11),and NH_(12)-each featuring a unique extended H sublattice:corrugated graphene-like hydrogen layers in NH_(10),planar H_(16)-ring sheets in NH11,and a fully three-dimensional,densely connected H framework in NH12.These structures are stabilized by NH_(4)^(+)units,which donate charge in a manner analogous to metal atoms in conventional metal superhydrides.Remarkably,NH_(10)exhibits a superconducting critical temperature(T_(c))of 190 K at 200 GPa,driven by strong electron-phonon coupling between H-1s states and low-frequency hydrogen-derived phonon modes-a mechanism notably distinct from that of hydrogen cages in LaH_(10)and CaH_(6).The predicted T_(c)values of NH_(11)and NH_(12)also exceeds 130 K.Our work introduces a new paradigm for designing nonmetal superhydrides with structurally engineered hydrogenic frameworks.展开更多
The search of direct-gap Si-based semiconductors is of great interest due to the potential application in many technologically relevant fields.This work examines the incorporation of He as a possible route to form a d...The search of direct-gap Si-based semiconductors is of great interest due to the potential application in many technologically relevant fields.This work examines the incorporation of He as a possible route to form a direct band gap in Si.Structure predictions and first-principles calculations show that He and Si,at high pressure,form four dynamically stable phases of Si_(2)He(oP36-Si_(2)He,tP9-Si_(2)He,mC18-Si_(2)He,and mC12-Si_(2)He).All phases adopt host–vip structures consisting of a channel-like Si host framework filled with He vip atoms.The Si frameworks in oP36-Si2He,tP9-Si2He,and mC12-Si_(2)He could be retained to ambient pressure after removal of He,forming three pure Si allotropes.Among them,oP36-Si_(2)He and mC12-Si_(2)He exhibit direct band gaps of 1.24 and 1.34 eV,respectively,close to the optimal value(~1.3 eV)for solar cell applications.Analysis shows that mC12-Si_(2)He with an electric dipole transition allowed band gap possesses higher absorption capacity than cubic diamond Si,which makes it to be a promising candidate material for thin-film solar cell.展开更多
基金financially supported by the National Natural Science Foundation of China(NSFC,U20A20310,52107230,52176199,52102470)the support of the research project Model2Life(03XP0334),funded by the German Federal Ministry of Education and Research(BMBF)。
文摘Lithium-ion batteries(LIBs), as the first choice for green batteries, have been widely used in energy storage, electric vehicles, 3C devices, and other related fields, and will have greater application prospects in the future. However, one of the obstacles hindering the future development of battery technology is how to accurately evaluate and monitor battery health, which affects the entire lifespan of battery use. It is not enough to assess battery health comprehensively through the state of health(SoH) alone, especially when nonlinear aging occurs in onboard applications. Here, for the first time, we propose a brand-new health evaluation indicator—state of nonlinear aging(SoNA) to explain the nonlinear aging phenomenon that occurs during the battery use, and also design a knee-point identification method and two SoNA quantitative methods. We apply our health evaluation indicator to build a complete LIB full-lifespan grading evaluation system and a ground-to-cloud service framework, which integrates multi-scenario data collection, multi-dimensional data-based grading evaluation, and cloud management functions. Our works fill the gap in the LIBs’ health evaluation of nonlinear aging, which is of great significance for the health and safety evaluation of LIBs in the field of echelon utilization such as vehicles and energy storage. In addition, this comprehensive evaluation system and service framework are expected to be extended to other battery material systems other than LIBs, yet guiding the design of new energy ecosystem.
基金This work was supported by the Natural Science Foundation of China under Grant No.21573037the Postdoctoral Science Foundation of China under Grant No.2013M541283+4 种基金the Natural Science Foundation of Hebei Province(Grant No.B2021203030)the Science and Technology Project of Hebei Education Department(Grant Nos.JZX2023020 and QN2023246)A.B.acknowledges financial support from the Spanish Ministry of Science and Innovation(Grant No.PID2019-105488GB-I00)the Department of Education,Universities and Research of the Basque Government and the University of the Basque Country(Grant No.IT1707-22)This work was carried out at the National Supercomputer Center in Tianjin,and the calculations were performed on TianHe-1(A).
文摘Superionic and electride behaviors in materials,which induce a variety of exotic physical properties of ions and electrons,are of great importance both in fundamental research and for practical applications.However,their coexistence in hot alkali-metal borides has not been observed.In this work,we apply first-principles structure search calculations to identify eight Na-B compounds with host-vip structures,which exhibit a wide range of building blocks and interesting properties linked to the Na/B composition.Among the known borides,Na-rich Na9B stands out as the composition with the highest alkali-metal content,featuring vertex-and face-sharing BNa16 polyhedra.Notably,it exhibits electride characteristics and transforms into a superionic electride at 200 GPa and 2000 K,displaying unusual Na atomic diffusion behavior attributed to the modulation of the interstitial anion electrons.It demonstrates semiconductor behavior in the solid state,and metallic properties associated with Na 3p/3s states in the superionic and liquid regions.On the other hand,B-rich NaB7,consisting of a unique covalent B framework,is predicted to exhibit low-frequency phonon-mediated superconductivity with a T_(c) of 16.8 K at 55 GPa.Our work advances the understanding of the structures and properties of alkali-metal borides.
基金supported by the Natural Science Foundation of China under Grants No.22372142,12304028,and 12404027the Foreign Expert Introduction Program(G2023003004L)+6 种基金the Central Guiding Local Science and Technology Development Fund Projects(236Z7605G)the Natural Science Foundation of Hebei Province(Grant No.B2024203051,A2024203023,and A2024203002)the Science and Technology Project of Hebei Education Department(Grants No.JZX2023020)Innovation Capability Improvement Project of Hebei province(22567605H)Hebei Province Yan Zhao Huang Jin Tai Talent Program(Postdoctoral Platform,B2024003003)support from the Spanish Ministry of Science and Innovation(Grant No.PID2022-139230NB-I00)the Department of Education,Universities and Research of the Basque Government and the University of the Basque Country(Grant No.IT1707-22).
文摘Electrides,materials in which a portion of valence electrons reside as interstitial anionic electrons(IAEs)within lattice cavities-exhibit a wide range of extraordinary physical and chemical properties,making them a central focus of condensed matter physics.Under high pressure,intermetallic systems provide a unique pathway to novel electrides by enabling unconventional charge-transfer mechanisms.Here,we employ first-principles structure searches to identify two stable Li-Mg electrides,Li_(3)Mg and Li_(4)Mg.At low pressure,Mg atoms act as anionic centers through occupation of their outer-shell 3p orbitals.Upon compression,charge is transferred from Mg to the lattice cavities,enhancing the localization and density of IAEs.This,in turn,strengths electron-phonon coupling and raises the superconducting transition temperature(T_(c))to 13.3 K at 75 GPa for Li_(3)Mg and 19.7 K at 80 GPa for Li_(4)Mg-values that surpass most known electride superconductors below 100 GPa.Selective hydrogen insertion into the lattice cavities in Li_(4)Mg quenches the IAEs and confirms their essential role in superconductivity.Further compression drives a transition to poor or non-superconducting phases,with Mg atoms switching from electron acceptors to donors,contrary to the typical behavior of electropositive metals,which tend to transition from donors into acceptors under pressure.These findings highlight the pivotal role of IAEs in electride superconductivity and pave the way for designing novel intermetallic electrides with tunable properties.
基金supported by the Natural Science Foundation of China(grant nos.22372142,12304028,and 12404027)Foreign Ex-pert Introduction Program,China(G2023003004L)+6 种基金Central Guiding Local Science and Technology Development Fund Projects,China(236Z7605G)Natural Science Foundation of Hebei Province,China(grant nos.B2024203051,A2024203023,and A2024203002)Science and Technology Project of Hebei Education Department,China(grant no.JZX2023020)Innovation Capability Improvement Project of Hebei province,China(22567605H)Hebei Province Yan Zhao Huang Jin Tai Talent Program,China(Postdoctoral Platform,B2024003003)A.B.acknowledges financial support from the Spanish Ministry of Science and Innovation,Spain(Grant No.PID2022-139230NB-I00)the Department of Education,Universities and Research of the Basque Government,Spain and the University of the Basque Country,Spain(Grant No.IT1707-22).
文摘Extended hydrogen-rich frameworks stabilized under high pressure are essential for achieving high-temperature superconductivity in metal hydrides,where metal atoms contribute both charge and intrinsic precompression.In contrast,p-block nonmetal hydrides lack such extended hydrogenic connectivity.Here,using first-principles crystal structure search calculations,we identify three nitrogen-based superhydrides-NH_(10),NH_(11),and NH_(12)-each featuring a unique extended H sublattice:corrugated graphene-like hydrogen layers in NH_(10),planar H_(16)-ring sheets in NH11,and a fully three-dimensional,densely connected H framework in NH12.These structures are stabilized by NH_(4)^(+)units,which donate charge in a manner analogous to metal atoms in conventional metal superhydrides.Remarkably,NH_(10)exhibits a superconducting critical temperature(T_(c))of 190 K at 200 GPa,driven by strong electron-phonon coupling between H-1s states and low-frequency hydrogen-derived phonon modes-a mechanism notably distinct from that of hydrogen cages in LaH_(10)and CaH_(6).The predicted T_(c)values of NH_(11)and NH_(12)also exceeds 130 K.Our work introduces a new paradigm for designing nonmetal superhydrides with structurally engineered hydrogenic frameworks.
基金The authors acknowledge funding from the NSFC under grants Nos.12074154,11804129,11722433,and 11804128the funding from the Science and Technology Project of Xuzhou under grant No.KC19010+1 种基金Y.L.acknowledges the funding from the Six Talent Peaks Project and 333 High-level Talents Project of Jiangsu ProvinceS.D.acknowledges the founding from Postgraduate Research and Practice Innovation Program of Jiangsu Province No.KYCX20_2223.
文摘The search of direct-gap Si-based semiconductors is of great interest due to the potential application in many technologically relevant fields.This work examines the incorporation of He as a possible route to form a direct band gap in Si.Structure predictions and first-principles calculations show that He and Si,at high pressure,form four dynamically stable phases of Si_(2)He(oP36-Si_(2)He,tP9-Si_(2)He,mC18-Si_(2)He,and mC12-Si_(2)He).All phases adopt host–vip structures consisting of a channel-like Si host framework filled with He vip atoms.The Si frameworks in oP36-Si2He,tP9-Si2He,and mC12-Si_(2)He could be retained to ambient pressure after removal of He,forming three pure Si allotropes.Among them,oP36-Si_(2)He and mC12-Si_(2)He exhibit direct band gaps of 1.24 and 1.34 eV,respectively,close to the optimal value(~1.3 eV)for solar cell applications.Analysis shows that mC12-Si_(2)He with an electric dipole transition allowed band gap possesses higher absorption capacity than cubic diamond Si,which makes it to be a promising candidate material for thin-film solar cell.
