Double-exchange(DE) interaction plays an important role in electrocatalytic oxygen evolution reaction(OER).However,precise achievement of DE interaction often requires foreign dopants or vacancy engineering,leading to...Double-exchange(DE) interaction plays an important role in electrocatalytic oxygen evolution reaction(OER).However,precise achievement of DE interaction often requires foreign dopants or vacancy engineering,leading to destabilization of the catalysts and deterioration of performance.By contrast,the utilization of environmentally friendly,contactless,and continuously adjustable magnetic fields to study the OER process is profitable to avoid aforementioned interference factors and further elucidate the direct relationship_(0.5)between DE interaction and OER activity.Here,by using cobalt hydroxide carbonate(Co(OH)(CO_(3))·xH_(2)O,CoHC) nanostructures as a proof-of-concept study,external magnetic fields are carefully implemented to verify the role of DE interaction during water oxidation reaction.Detailed studies reveal that external magnetic fields effectively enhance the reaction rate of the catalyst,the overpotential decreases from 386 to 355 mV(100 mA·cm^(-2)),while Tafel slopes drastically decline from 93 to 67 mV·dec^(-1)(1.0 T).Moreover,magnetic field increment exhibits robust durability.Through in situ Raman and impedance measurements under external field,it can be found that magnetic field promotes the electron migration between Co^(2+) and Co^(3+) in the CoHC catalysts with the assistance of DE interactions,thus boosting the OER efficiency.展开更多
The electrical and magnetic properties of bilayer manganites La1.4Sr1.6Mn1.96TE0.04O7(TE = Mn, Fe, Ti, Nb) were investigated. Doping caused obvious changes in electrical and magnetic behaviors such as decrease of in...The electrical and magnetic properties of bilayer manganites La1.4Sr1.6Mn1.96TE0.04O7(TE = Mn, Fe, Ti, Nb) were investigated. Doping caused obvious changes in electrical and magnetic behaviors such as decrease of insulator-metal transition and magnetic transition temperatures, increase of peak resistivity, and different magnetoresistance effect. These changes had a significant degree of correlation with the valence of doped ions. From Fe, Ti to Nb doping, the effect was doubly stronger. The results could be well understood by considering the different destructions on double-exchange interaction and different influences on lattice distortion caused by Fe, Ti and Nb doping. The temperature dependence of magnetization measured at high field showed that the influence of doping was greatest near three-dimensional magnetic transition temperature of parent phase.展开更多
We extend a previous result of ours [G.S. Tian, Phys. Rev. B63 (2001) 224413] on the antiferromagnetic spin correlations in the half-filled Hubbard model at finite temperature to the double-exchange model. To overcome...We extend a previous result of ours [G.S. Tian, Phys. Rev. B63 (2001) 224413] on the antiferromagnetic spin correlations in the half-filled Hubbard model at finite temperature to the double-exchange model. To overcome the mathematical difficulty caused by the localized spin freedom in this model, we apply both Zener's argument and the finite-temperature spin-reflection-positivity method to show rigorously that, at any temperature , the spin correlations in the half-filled double-exchange model are predominantly antiferromagnetic. This conclusion is completely consistent with the experimental observations and the previous theoretical results by approximate methods.展开更多
High electrochemically active bimessite is always desirable pseudocapacitive material for supercapacitor.Here,two-dimensional(2D)compulsive malposition parallel bimessite standing on β-MnO_(2) interconnected networks...High electrochemically active bimessite is always desirable pseudocapacitive material for supercapacitor.Here,two-dimensional(2D)compulsive malposition parallel bimessite standing on β-MnO_(2) interconnected networks have been designed.Due to the retrition of β-MnO_(2),compulsi ve malposition,slippage of MnO6 slab,occured in bimessite resulting in weaken bi nding force between bimessi te slab and interlayer cations,which enhanced their electrochemical performances.Additionally,the electrical conductivity of the structure was largely promoted by the 2D charge transfer route and double-exchange mechanism in bimessite,also leading to desirable electro-chemical properties.Based on the fraction of as-prepared nanostructure,the par all bimessite exhibited good pseudocapacitance performance(660 F g^(-1))with high rate capability.In addition,the asymmetrice supercapacitor assembled by reduced graphene oxide(RGO)and as-prepared nanostructure,which respectively served as the negative and positive eletrode,delivered an energy density of 33.1 Wh kg^(-1) and a mad mum power density of 64.0 kW kg^(-1) with excellent cyeling stability(95.8% after 10000 cycles).Finally,the study opens new avenwes for synthesizing high eletrochemically actiwe bimessite structure for high-performance energy storage devices.展开更多
基金financially supported by the Program B for Outstanding PhD Candidate of Nanjing University(No.201801B067)。
文摘Double-exchange(DE) interaction plays an important role in electrocatalytic oxygen evolution reaction(OER).However,precise achievement of DE interaction often requires foreign dopants or vacancy engineering,leading to destabilization of the catalysts and deterioration of performance.By contrast,the utilization of environmentally friendly,contactless,and continuously adjustable magnetic fields to study the OER process is profitable to avoid aforementioned interference factors and further elucidate the direct relationship_(0.5)between DE interaction and OER activity.Here,by using cobalt hydroxide carbonate(Co(OH)(CO_(3))·xH_(2)O,CoHC) nanostructures as a proof-of-concept study,external magnetic fields are carefully implemented to verify the role of DE interaction during water oxidation reaction.Detailed studies reveal that external magnetic fields effectively enhance the reaction rate of the catalyst,the overpotential decreases from 386 to 355 mV(100 mA·cm^(-2)),while Tafel slopes drastically decline from 93 to 67 mV·dec^(-1)(1.0 T).Moreover,magnetic field increment exhibits robust durability.Through in situ Raman and impedance measurements under external field,it can be found that magnetic field promotes the electron migration between Co^(2+) and Co^(3+) in the CoHC catalysts with the assistance of DE interactions,thus boosting the OER efficiency.
基金Project supported by the National "973" Project (2006CB921606 )National Natural Science Foundation of China(10574049)Foundation from the Ministry of the National Education (20060487011)
文摘The electrical and magnetic properties of bilayer manganites La1.4Sr1.6Mn1.96TE0.04O7(TE = Mn, Fe, Ti, Nb) were investigated. Doping caused obvious changes in electrical and magnetic behaviors such as decrease of insulator-metal transition and magnetic transition temperatures, increase of peak resistivity, and different magnetoresistance effect. These changes had a significant degree of correlation with the valence of doped ions. From Fe, Ti to Nb doping, the effect was doubly stronger. The results could be well understood by considering the different destructions on double-exchange interaction and different influences on lattice distortion caused by Fe, Ti and Nb doping. The temperature dependence of magnetization measured at high field showed that the influence of doping was greatest near three-dimensional magnetic transition temperature of parent phase.
文摘We extend a previous result of ours [G.S. Tian, Phys. Rev. B63 (2001) 224413] on the antiferromagnetic spin correlations in the half-filled Hubbard model at finite temperature to the double-exchange model. To overcome the mathematical difficulty caused by the localized spin freedom in this model, we apply both Zener's argument and the finite-temperature spin-reflection-positivity method to show rigorously that, at any temperature , the spin correlations in the half-filled double-exchange model are predominantly antiferromagnetic. This conclusion is completely consistent with the experimental observations and the previous theoretical results by approximate methods.
基金the National Natural Science Foundation of China(Grant No.51908092)Projects(No.2020CDJXZ001,2020CDCGJ006 and 2020CDCGCL004)supported by the Fundamental Research Funds for the Central Universities,the Joint Funds of the National Natural Science Foundation of China-Guangdong(Grant No.U1801254)+5 种基金the project funded by Chongqing Special Postdoctoral Science Foundation(XmT2018043)the Chongqing Research Program of Basic Research and Frontier Technology(cstc2017jcyjBX0080)Natural Science Foundation Project of Chongqing for Post-doctor(cstc2019jcyjbsh0079,cstc2019jcyjbshX0085)Technological projects of Chongqing Municipal Education Commission(KJZDK201800801)the Innovative Research Team of Chongqing(CXTDG201602014)the Innovative technology of New materials and metallurgy(2019CDXYCL0031).
文摘High electrochemically active bimessite is always desirable pseudocapacitive material for supercapacitor.Here,two-dimensional(2D)compulsive malposition parallel bimessite standing on β-MnO_(2) interconnected networks have been designed.Due to the retrition of β-MnO_(2),compulsi ve malposition,slippage of MnO6 slab,occured in bimessite resulting in weaken bi nding force between bimessi te slab and interlayer cations,which enhanced their electrochemical performances.Additionally,the electrical conductivity of the structure was largely promoted by the 2D charge transfer route and double-exchange mechanism in bimessite,also leading to desirable electro-chemical properties.Based on the fraction of as-prepared nanostructure,the par all bimessite exhibited good pseudocapacitance performance(660 F g^(-1))with high rate capability.In addition,the asymmetrice supercapacitor assembled by reduced graphene oxide(RGO)and as-prepared nanostructure,which respectively served as the negative and positive eletrode,delivered an energy density of 33.1 Wh kg^(-1) and a mad mum power density of 64.0 kW kg^(-1) with excellent cyeling stability(95.8% after 10000 cycles).Finally,the study opens new avenwes for synthesizing high eletrochemically actiwe bimessite structure for high-performance energy storage devices.