As the primary suppliers of cyclable sodium ions,O3-type layer-structured manganese-based oxides are recognized as highly competitive cathode candidates for sodium-ion batteries.To advance the development of high-ener...As the primary suppliers of cyclable sodium ions,O3-type layer-structured manganese-based oxides are recognized as highly competitive cathode candidates for sodium-ion batteries.To advance the development of high-energy sodium-ion batteries,it is crucial to explore cathode materials operating at high voltages while maintaining a stable cycling behavior.The orbital and electronic structure of the octahedral center metal element plays a crucial role in maintaining the octahedra structural integrity and improving Na^(+)ion diffusion by introducing heterogeneous chemical bonding.Inspired by the abundant configuration of extra nuclear electrons and large ion radius,we employed trace amounts of tungsten in this study.The obtained cathode material can promote the reversibility of oxygen redox reactions in the high-voltage region and inhibit the loss of lattice oxygen.Additionally,the formation of a Na_(2)WO_(4) coating on the material surface can improve the interfacial stability and interface ions diffusion.It demonstrates an initial Coulombic efficiency(ICE)of 94.6%along with 168.5 mA h g^(-1 )discharge capacity within the voltage range of 1.9-4.35 V.These findings contribute to the advancement of high-energy sodium-ion batteries by providing insights into the benefits of tungsten doping and Na_(2)WO_(4) coating on cathode materials.展开更多
Owing to the environmental and inherent advantages,nitrogen reduction reaction(NRR)by electrocatalysts attracts global attention.The surface engineering is widely employed to enhance the electrocatalytic activity by a...Owing to the environmental and inherent advantages,nitrogen reduction reaction(NRR)by electrocatalysts attracts global attention.The surface engineering is widely employed to enhance the electrocatalytic activity by atomic defects and heterostructure effects.A three-dimensional(3D)free-standing integrated electrode was fabricated by numerous nearly-single-crystal TiO_(2-δ)N_δnanowire arrays.Based on the high electronic conductivity network,it exposes numerous active sites as well to facilitate the selective nitrogen adsorption and*H adsorption suppression.The synergistic effects between Ti^(3+)and oxygen vacancy(O_v)boost the intrinsic catalytic activity,in which Ti^(3+)acquired electrons via Ovcan effectively activate the N≡N bond and make it easy to bind with protons.The energy barrier of primary protonation process(*N_(2)+H^(+)+e^(-)→*NNH)can be dramatically decreased.The highest ammonia yield rate(14.33μg h^(-1)mgcat^(-1))emerges at-0.2 V,while the optimal ammonia Faradaic efficiency(9.17%)is acquired at-0.1 V.Density functional theory(DFT)calculation reveals that the Ti^(3+)can be served as the active sites for nitrogen adsorption and activation,while ammonia synthesis is accomplished by the distal pathway.The high electronic conductivity integrated network and synergistic effects can significantly facilitate nitrogen absorption and accelerate electrocatalytic reaction kinetic,which are responsible for the excellent NRR performance at room temperature.展开更多
Rechargeable sodium–oxygen(Na-O_(2))and sodium–carbon dioxide(Na-CO_(2))batteries have attracted intensive research attention in recent years owing to their advantages of high theoretical energy density,modest cost,...Rechargeable sodium–oxygen(Na-O_(2))and sodium–carbon dioxide(Na-CO_(2))batteries have attracted intensive research attention in recent years owing to their advantages of high theoretical energy density,modest cost,abundance of sodium resources,and promising potential for achieving real sodium–air batteries in large-scale energy storage systems.Nevertheless,current research on Na-O_(2)and Na-CO_(2)batteries is facing enormous challenges,such as low energy efficiency and limited cycle life,which are restricting their progress at the initial stage.Therefore,understanding their working principles,and the chemical and electrochemical reactions of the electrodes is indispensable to achieve their practical application and even the goal of true sodium–air batteries.This review aims to provide an overview of the research developments and future perspectives on Na-O_(2)and Na-CO_(2)batteries,which include the major aspects,such as working mechanisms,air cathode materials design strategies,sodium anode protection,and electrolyte stability.Moreover,the remaining issues and future research directions are also thoroughly discussed and presented.展开更多
An effective regulation of the magnetism and interface of ferromagnetic materials is not only of great scientific significance,but also has an urgent need in modern industry.In this work,by using the first-principles ...An effective regulation of the magnetism and interface of ferromagnetic materials is not only of great scientific significance,but also has an urgent need in modern industry.In this work,by using the first-principles calculations,we demonstrate an effective approach to achieve non-volatile electrical control of ferromagnets,which proves this idea in multiferroic heterostructures of ferromagnetic La TiO_(3)and ferroelectric Bi FeO_(3).The results show that the magnetic properties and two-dimensional electron gas concentrations of La TiO_(3)films can be controlled by changing the polarization directions of Bi FeO_(3).The destroyed symmetry being introduced by ferroelectric polarization of the system leads to the transfer and reconstruction of the Ti-3 d electrons,which is the fundamental reason for the changing of magnetic properties.This multiferroic heterostructures will pave the way for non-volatile electrical control of ferromagnets and have potential applications.展开更多
Nitrogen-doped carbon catalysts with hierarchical porous structure are promising oxygen evolution reaction(OER)catalysts due to the faster mass transfer and better charge carrying ability.Herein,an exquisite high nitr...Nitrogen-doped carbon catalysts with hierarchical porous structure are promising oxygen evolution reaction(OER)catalysts due to the faster mass transfer and better charge carrying ability.Herein,an exquisite high nitrogen-containing ligand was designed and readily synthesized from the low-cost biomolecule adenine.Accordingly,three new MOFs(TJU-103,TJU-104 and TJU-105)were prepared using the Co(II)or Mn(II)ions as metal nodes.Through rationally controlling pyrolysis condition,in virtue of the high nitrogen content in well-defined periodic structure of the pristine MOFs,TJU-104–900 among the derived MOFs with hierarchical porous structure,i.e.,N-doped graphitic carbon encapsulating homogeneously distributed cobalt nanoparticles,could be conveniently obtained.Thanks to the synergistic effect of the hierarchical structure and well dispersed active components(i.e.,C=O,Co–Nx,graphitic C and N,pyridinic N),it could exhibit an overpotential of 280 mV@10mA/cm^(2)on carbon cloth for OER activity.This work provides the inspiration for fabrication of nitrogen-doped carbon/metal electrocatalysts from cost-effective and abundant biomolecules,which is promising for practical OER application.展开更多
基金supported by the National Natural Science Foundation of China(Grant No.52272194)LiaoNing Revitalization Talents Program(Grant No.XLYC2007155)。
文摘As the primary suppliers of cyclable sodium ions,O3-type layer-structured manganese-based oxides are recognized as highly competitive cathode candidates for sodium-ion batteries.To advance the development of high-energy sodium-ion batteries,it is crucial to explore cathode materials operating at high voltages while maintaining a stable cycling behavior.The orbital and electronic structure of the octahedral center metal element plays a crucial role in maintaining the octahedra structural integrity and improving Na^(+)ion diffusion by introducing heterogeneous chemical bonding.Inspired by the abundant configuration of extra nuclear electrons and large ion radius,we employed trace amounts of tungsten in this study.The obtained cathode material can promote the reversibility of oxygen redox reactions in the high-voltage region and inhibit the loss of lattice oxygen.Additionally,the formation of a Na_(2)WO_(4) coating on the material surface can improve the interfacial stability and interface ions diffusion.It demonstrates an initial Coulombic efficiency(ICE)of 94.6%along with 168.5 mA h g^(-1 )discharge capacity within the voltage range of 1.9-4.35 V.These findings contribute to the advancement of high-energy sodium-ion batteries by providing insights into the benefits of tungsten doping and Na_(2)WO_(4) coating on cathode materials.
基金financially supported by the Liao Ning Revitalization Talents Program(XLYC2007155)the Fundamental Research Funds for the Central Universities(N2025018,N2025009)。
文摘Owing to the environmental and inherent advantages,nitrogen reduction reaction(NRR)by electrocatalysts attracts global attention.The surface engineering is widely employed to enhance the electrocatalytic activity by atomic defects and heterostructure effects.A three-dimensional(3D)free-standing integrated electrode was fabricated by numerous nearly-single-crystal TiO_(2-δ)N_δnanowire arrays.Based on the high electronic conductivity network,it exposes numerous active sites as well to facilitate the selective nitrogen adsorption and*H adsorption suppression.The synergistic effects between Ti^(3+)and oxygen vacancy(O_v)boost the intrinsic catalytic activity,in which Ti^(3+)acquired electrons via Ovcan effectively activate the N≡N bond and make it easy to bind with protons.The energy barrier of primary protonation process(*N_(2)+H^(+)+e^(-)→*NNH)can be dramatically decreased.The highest ammonia yield rate(14.33μg h^(-1)mgcat^(-1))emerges at-0.2 V,while the optimal ammonia Faradaic efficiency(9.17%)is acquired at-0.1 V.Density functional theory(DFT)calculation reveals that the Ti^(3+)can be served as the active sites for nitrogen adsorption and activation,while ammonia synthesis is accomplished by the distal pathway.The high electronic conductivity integrated network and synergistic effects can significantly facilitate nitrogen absorption and accelerate electrocatalytic reaction kinetic,which are responsible for the excellent NRR performance at room temperature.
基金financially supported by an Australian Research Council(ARC)Discovery Project(DP180101453)
文摘Rechargeable sodium–oxygen(Na-O_(2))and sodium–carbon dioxide(Na-CO_(2))batteries have attracted intensive research attention in recent years owing to their advantages of high theoretical energy density,modest cost,abundance of sodium resources,and promising potential for achieving real sodium–air batteries in large-scale energy storage systems.Nevertheless,current research on Na-O_(2)and Na-CO_(2)batteries is facing enormous challenges,such as low energy efficiency and limited cycle life,which are restricting their progress at the initial stage.Therefore,understanding their working principles,and the chemical and electrochemical reactions of the electrodes is indispensable to achieve their practical application and even the goal of true sodium–air batteries.This review aims to provide an overview of the research developments and future perspectives on Na-O_(2)and Na-CO_(2)batteries,which include the major aspects,such as working mechanisms,air cathode materials design strategies,sodium anode protection,and electrolyte stability.Moreover,the remaining issues and future research directions are also thoroughly discussed and presented.
基金the National Natural Science Foundation of China(Grant No.12047517)the International Cooperation Project of Science and Technology of Henan Province,China(Grant No.182102410096)+1 种基金the Natural Science Foundation of Henan Province,China(Grant No.202300410069)the China Postdoctoral Science Foundation(Grant Nos.2020M682274 and 2020TQ0089)。
文摘An effective regulation of the magnetism and interface of ferromagnetic materials is not only of great scientific significance,but also has an urgent need in modern industry.In this work,by using the first-principles calculations,we demonstrate an effective approach to achieve non-volatile electrical control of ferromagnets,which proves this idea in multiferroic heterostructures of ferromagnetic La TiO_(3)and ferroelectric Bi FeO_(3).The results show that the magnetic properties and two-dimensional electron gas concentrations of La TiO_(3)films can be controlled by changing the polarization directions of Bi FeO_(3).The destroyed symmetry being introduced by ferroelectric polarization of the system leads to the transfer and reconstruction of the Ti-3 d electrons,which is the fundamental reason for the changing of magnetic properties.This multiferroic heterostructures will pave the way for non-volatile electrical control of ferromagnets and have potential applications.
基金This work was financially supported by the National Natural Science Foundation of China(Nos.21875165,22272118)the Fundamental Research Funds for the Central Universities(No.22120210529)+1 种基金the Science and Technology Commission of Shanghai Municipality,China(Nos.22ZR1464100,19DZ2271500)the Recruitment Program of Global Experts of China,and Research Grants from the City University of Hong Kong(Nos.CityU 11308420,6000716,9667217).
文摘Nitrogen-doped carbon catalysts with hierarchical porous structure are promising oxygen evolution reaction(OER)catalysts due to the faster mass transfer and better charge carrying ability.Herein,an exquisite high nitrogen-containing ligand was designed and readily synthesized from the low-cost biomolecule adenine.Accordingly,three new MOFs(TJU-103,TJU-104 and TJU-105)were prepared using the Co(II)or Mn(II)ions as metal nodes.Through rationally controlling pyrolysis condition,in virtue of the high nitrogen content in well-defined periodic structure of the pristine MOFs,TJU-104–900 among the derived MOFs with hierarchical porous structure,i.e.,N-doped graphitic carbon encapsulating homogeneously distributed cobalt nanoparticles,could be conveniently obtained.Thanks to the synergistic effect of the hierarchical structure and well dispersed active components(i.e.,C=O,Co–Nx,graphitic C and N,pyridinic N),it could exhibit an overpotential of 280 mV@10mA/cm^(2)on carbon cloth for OER activity.This work provides the inspiration for fabrication of nitrogen-doped carbon/metal electrocatalysts from cost-effective and abundant biomolecules,which is promising for practical OER application.
基金financially supported by the National Key Research and Development Program of China(2017YFA0206600)the National Natural Science Foundation of China(21761132001,91633301,51573057,and 51903095)+1 种基金the Fundamental Research Funds for the Central Universities(D2192160)performed in part on the SAXS/WAXS beamline at the Australian Synchrotron,which is part of the ANSTO.