The effect of rare earth ion Er 3+ on myoglobin(Mb) was studied by using Resonance Raman spectroscopy. The results show that with the variation of Er 3+ concentrations, both the oxidation state and spin state of Mb ar...The effect of rare earth ion Er 3+ on myoglobin(Mb) was studied by using Resonance Raman spectroscopy. The results show that with the variation of Er 3+ concentrations, both the oxidation state and spin state of Mb are sensitive to the perturbation of Er 3+ . Er 3+ added to Mb affects the oxidation and spin state synchronously. The structure sensitive groups of Mb are more accessible to the Er 3+ than other groups. According to the fluorometry and CD spectra studied and our results as mentioned above, we considered that Er 3+ does not interact with heme directly, and Er 3+ probably leads to the conformational changes of Mb due to the change of oxidation and spin state of Heme. [WT5HZ]展开更多
The effect of Dy doping on magnetism of La 0.7 Sr 0.3 CoO 3 system was studied through the measurements of M-T curves and M-H curves. The results show that with Dy content increasing, T C decreases, M weakens, the coe...The effect of Dy doping on magnetism of La 0.7 Sr 0.3 CoO 3 system was studied through the measurements of M-T curves and M-H curves. The results show that with Dy content increasing, T C decreases, M weakens, the coercive force strengthens, and the samples exhibit the abnormal phenomenon that M increases continuously with T decreasing in low temperature range. Research indicates that the variation of magnetism in the system comes from the changes of lattice parameters and magnetic environment caused by Dy doping and from the spin-state transition of Co ions induced by Dy ions.展开更多
We present a novel class of Rydberg-mediated nuclear-spin entanglement in divalent atoms with global laser pulses.First,we show a fast nuclear-spin controlled phase gate of an arbitrary phase realizable either with tw...We present a novel class of Rydberg-mediated nuclear-spin entanglement in divalent atoms with global laser pulses.First,we show a fast nuclear-spin controlled phase gate of an arbitrary phase realizable either with two laser pulses when assisted by Stark shifts,or with three pulses.Second,we propose to create an electrons−nuclei-entangled state,which is named a super bell state(SBS)for it mimics a large Bell state incorporating three small Bell states.Third,we show a protocol to create a three-atom electrons-nuclei entangled state which contains the three-body W and Greenberger−Horne−Zeilinger(GHZ)states simultaneously.These protocols possess high intrinsic fidelities,do not require single-site Rydberg addressing,and can be executed with large Rydberg Rabi frequencies in a weak,Gauss-scale magnetic field.The latter two protocols can enable measurement-based preparation of Bell,hyperentangled,and GHZ states,and,specifically,SBS can enable quantum dense coding where one can share three classical bits of information by sending one particle.展开更多
The residual of oxidant chemicals in advanced oxidation processes(AOPs)resulted in both economic cost and secondary pollution.Herein,we report a direct oxidation of phenolic pollutants induced by Ca-Mn-O perovskites w...The residual of oxidant chemicals in advanced oxidation processes(AOPs)resulted in both economic cost and secondary pollution.Herein,we report a direct oxidation of phenolic pollutants induced by Ca-Mn-O perovskites without using an oxidant.Governed by one-electron transfer process(ETP)from the phenolics to the Ca-Mn-O perovskites,this direct oxidation proceeds in fast reaction kinetics with activation energy of 51.4 kJ/mol,which was comparable with those AOPs-based catalytic systems.Additionally,mineralization and polymerization reactions occurred on the Ca-Mn-O surface and ensured the complete removal of phenolics.The high spin state Mn(III)within Ca-Mn-O structure was the dominant active site for this ETP.The elongated axial Mn(III)–O bonds within the[MnO_(6)]octahedron facilitated the acceptance of the electrons from the phenolics and thus promoted the initiation of the direct oxidation process.Mn(III)in the high spin state can also activate dissolved O_(2)to produce singlet oxygen(^(1)O_(2))for a fast removal of phenolics.The mixed Mn(III)/Mn(IV)within Ca-Mn-O accelerated the ETP by enhancing the electrical conductivity.This efficient Ca-Mn-O-induced ETP for removal of organic contaminants casts off the dependence on external chemical and energy inputs and provides a sustainable approach for transforming the toxic organic pollutants into value-added polymers.展开更多
Carbon nanofibers(CNFs)with high specific surface area show great potential for sodium storage as a hard carbon material.Herein,CNFs anchored with Ni nanoparticles(CNFs/Ni)were prepared through chemical vapor depositi...Carbon nanofibers(CNFs)with high specific surface area show great potential for sodium storage as a hard carbon material.Herein,CNFs anchored with Ni nanoparticles(CNFs/Ni)were prepared through chemical vapor deposition and impregnation reduction methods,in situ growing on the three-dimensional porous copper current collector(3DP-Cu).The coupling effect of high-spin state Ni nanopar-ticles leads to the increase of defect density and the expansion of lattice spacing of CNFs.Meanwhile,the 3DP-Cu ensures a high loading capacity of CNFs and short ion/electron transport channels.As an integral binder-free anode,the 3DP-Cu/CNFs/Ni exhibits excellent electrochemical performance,which demon-strates a high specific capacity with 298.5 mAh g^(-1)at 1000 mA g^(-1)after 1500 cycles,and a high power density with 200 mAh g^(-1)over 1000 cycles at 5000 mA g^(-1).Density functional theory calculation re-sults show that the high-spin state Ni regulates the electronic structure of CNFs,which significantly reduces the adsorption energy for Na^(+)(-2.7 Ev)and thus enables high-rate capability.The regulation of the electronic structure of carbon materials by high-spin state metal provides a new strategy for developing high-power carbonaceous anode materials for sodium-ion batteries.展开更多
Efficient electrocatalysts are vital to large-current hydrogen production in commercial water splitting for green energy generation.Herein,a novel heterophase engineering strategy is described to produce polymorphic C...Efficient electrocatalysts are vital to large-current hydrogen production in commercial water splitting for green energy generation.Herein,a novel heterophase engineering strategy is described to produce polymorphic CoSe_(2)electrocatalysts.The composition of the electrocatalysts consisting of both cubic CoSe_(2)(c-CoSe_(2))and orthorhombic CoSe_(2)(o-CoSe_(2))phases can be controlled precisely.Our results demonstrate that junction-induced spin-state modulation of Co atoms enhances the adsorption of intermediates and accelerates charge transfer resulting in superior large-current hydrogen evolution reaction(HER)properties.Specifically,the CoSe_(2)based heterophase catalyst with the optimal c-CoSe_(2)content requires an overpotential of merely 240 mV to achieve 1,000 mA·cm^(-2)as well as a Tafel slope of 50.4 mV·dec^(-1).Furthermore,the electrocatalyst can maintain a large current density of 1,500 mA·cm^(-2)for over 320 h without decay.The results reveal the advantages and potential of heterophase junction engineering pertaining to design and fabrication of low-cost transition metal catalysts for large-current water splitting.展开更多
In this paper,an integrated guidance and control method based on an adaptive path-following controller is proposed to control a spin-stabilized projectile with only translational motion information under the constrain...In this paper,an integrated guidance and control method based on an adaptive path-following controller is proposed to control a spin-stabilized projectile with only translational motion information under the constraint of an actuator,uncertainties in aerodynamic parameters and measurements,and control system complexity.Owing to the fairly high rotation speed,the dynamic model of this missile is strongly nonlinear,uncertain and coupled in pitch,yaw and roll channels.A theoretical equivalent resultant force and uncertainty compensation method are comprehensively used to realize decoupling of pitch and yaw.In response to the strong nonlinear and time-varying characteristics of the dynamic system,the quasi-linear model whose parameters are obtained by interpolation of points selected as the segmentation points in the trajectory envelope,is used for calculation in each step.To cope with the system uncertainty caused by model approximation,parameter uncertainty and ballistic interference,an extended state estimator is used to compensate the output feedback according to the test ballistic angle.In order to improve the tracking efficiency and ensure the tracking error convergence with only translational motion information,the virtual guide point,whose derivative is deduced according to the Lyapunov principle,is calculated in real time according to the projection relationship between the real-time position and the reference trajectory,and a virtual line-of-sight angle and the backstepping method are used for the design of the guidance and control system.In order to avoid the influence of control input saturation on the guidance and control performance due to the actuator limitation and improve the robustness of the system,an anti-saturation compensator is designed according to the two-step method.The feasibility and effectiveness of the path-following controller is verified through closed-loop flight simulations with measurement,control,and condition uncertainties.The results indicate that the designed controller can conv展开更多
The distribution of the nuclear ground-state spin in a two-body random ensemble(TBRE)was studied using a general classification neural network(NN)model with two-body interaction matrix elements as input features and t...The distribution of the nuclear ground-state spin in a two-body random ensemble(TBRE)was studied using a general classification neural network(NN)model with two-body interaction matrix elements as input features and the corresponding ground-state spins as labels or output predictions.The quantum many-body system problem exceeds the capability of our optimized NNs in terms of accurately predicting the ground-state spin of each sample within the TBRE.However,our NN model effectively captured the statistical properties of the ground-state spin because it learned the empirical regularity of the ground-state spin distribution in TBRE,as discovered by physicists.展开更多
Non-Hermitian systems have been discussed mostly in the context of open systems and nonequilibrium.Recent experimental progress is much from optical,cold-atomic,and classical platforms due to the vast tunability and c...Non-Hermitian systems have been discussed mostly in the context of open systems and nonequilibrium.Recent experimental progress is much from optical,cold-atomic,and classical platforms due to the vast tunability and clear identification of observables.However,their counterpart in solid-state electronic systems in equilibrium remains unmasked although highly desired,where a variety of materials are available,calculations are solidly founded,and accurate spectroscopic techniques can be applied.We demonstrate that,in the surface state of a topological insulator with spin-dependent relaxation due to magnetic impurities,highly nontrivial topological soliton spin textures appear in momentum space.Such spin-channel phenomena are delicately related to the type of non-Hermiticity and correctly reveal the most robust non-Hermitian features detectable spectroscopically.Moreover,the distinct topological soliton objects can be deformed to each other,mediated by topological transitions driven by tuning across a critical direction of doped magnetism.These results not only open a solid-state avenue to exotic spin patterns via spin-and angle-resolved photoemission spectroscopy,but also inspire non-Hermitian dissipation engineering of spins in solids.展开更多
Owing to the distinctive structural characteristics,vanadium nitride(VN)is highly regarded as a catalyst for oxygen reduction reaction(ORR)in zinc-air batteries(ZABs).However,VN exhibits limited intrinsic ORR activity...Owing to the distinctive structural characteristics,vanadium nitride(VN)is highly regarded as a catalyst for oxygen reduction reaction(ORR)in zinc-air batteries(ZABs).However,VN exhibits limited intrinsic ORR activity due to the weak adsorption ability to O-containing species.Here,the S-doped VN anchored on N,S-doped multi-dimensional carbon(S-VN/Co/NS-MC)was constructed using the solvothermal and in-situ doping methods.Incorporating sulfur atoms into VN species alters the electron spin state of vanadium in the S-VN/Co/NS-MC for regulating the adsorption energy of vanadium sites to oxygen molecules.The introduced sulfur atoms polarize the V 3d_(z)^(2) electrons,shifting spin-down electrons closer to the Fermi level in the S-VN/Co/NS-MC.Consequently,the introduction of sulfur atoms into VN species enhances the adsorption energy of vanadium sites for oxygen molecules.The*OOH dissociation transitions from being unspontaneous on the VN surface to a spontaneous state on the S-doped VN surface.Then,the ORR barrier on the S-VN/Co/NS-MC surface is reduced.The S-VN/Co/NS-MC demonstrates a higher half-wave potential and limiting current density compared to the VN/Co/N-MC.The S-VN/Co/NS-MC-based liquid ZABs display a power density of 195.7 m W cm^(-2),a specific capacity of 815.7 m A h g^(-1),and a cycling stability exceeding 250 h.The S-VN/Co/NS-MC-based flexible ZABs are successfully employed to charge both a smart watch and a mobile phone.This approach holds promise for advancing the commercial utilization of VN-based catalysts in ZABs.展开更多
Metal-organic frameworks(MOFs)have been developed as an ideal platform for exploration of the relationship between intrinsic structure and catalytic activity,but the limited catalytic activity and stability has hamper...Metal-organic frameworks(MOFs)have been developed as an ideal platform for exploration of the relationship between intrinsic structure and catalytic activity,but the limited catalytic activity and stability has hampered their practical use in water splitting.Herein,we develop a bond length adjustment strategy for optimizing naphthalene-based MOFs that synthesized by acid etching Co-naphthalenedicarboxylic acid-based MOFs(donated as AE-CoNDA)to serve as efficient catalyst for water splitting.AE-CoNDA exhibits a low overpotential of 260 mV to reach 10 mA cm^(−2)and a small Tafel slope of 62 mV dec^(−1)with excellent stability over 100 h.After integrated AE-CoNDA onto BiVO_(4),photocurrent density of 4.3 mA cm^(−2)is achieved at 1.23 V.Experimental investigations demonstrate that the stretched Co-O bond length was found to optimize the orbitals hybridization of Co 3d and O 2p,which accounts for the fast kinetics and high activity.Theoretical calculations reveal that the stretched Co-O bond length strengthens the adsorption of oxygen-contained intermediates at the Co active sites for highly efficient water splitting.展开更多
Open-shell oligomers and polymers have exhibited intriguing electronic and magnetic properties, making them highly desirable for a wide range of applications, including ambipolar organic field-effect transistors (OFET...Open-shell oligomers and polymers have exhibited intriguing electronic and magnetic properties, making them highly desirable for a wide range of applications, including ambipolar organic field-effect transistors (OFETs), photodetectors, organic thermoelectrics, and spintronics. Although open-shell ground states have been observed in certain small molecules and doped organic semiconductors, the exploration of open-shell ground-state conjugated polymers is still limited, and the strategies for designing these polymers remain obscure. This review aims to briefly introduce the theory and characterization methods of open-shell conjugated polymers, along with an overview of recent progress and applications. The objective is to stimulate further advancements and investigations in this promising area by shedding light on the potential of open-shell conjugated polymers and the challenges that lie ahead.展开更多
Carbon nanofibers(CNFs)have received extensive and in-depth studied as anodes for sodium-ion batteries(SIBs),and yet their initial Coulombic efficiency and rate capability remain enormous challenge at practical level....Carbon nanofibers(CNFs)have received extensive and in-depth studied as anodes for sodium-ion batteries(SIBs),and yet their initial Coulombic efficiency and rate capability remain enormous challenge at practical level.Herein,CNFs anchored with cobalt nanocluster(CNFs-Co)were prepared using chemical vapor deposition and thermal reduction methods.The as-prepared CNFs-Co shows a high initial Coulombic efficiency of 91%and a high specific discharge capacity of 246 mAh/g at 0.1 A/g after 200 cycles as anode for SIBs.Meanwhile,the CNFs-Co anode still delivers a high cycling stability with 108 mAh/g after 1000 cycles at 10 A/g.These excellent electrochemical properties could be attributed to the involved spin state Co,which endows CNFs with large interplanar spacing(0.39 nm)and abundant vacancy defects.Importantly,the spin state Co downshifts the p-band center of carbon and strengthens the Na+adsorption energy from-2.33 eV to-2.64 eV based on density functional theory calculation.This novel strategy of modulating the carbon electronic structure by the spin state of magnetic metals provides a reference for the development of high-performance carbon-based anode materials.展开更多
文摘The effect of rare earth ion Er 3+ on myoglobin(Mb) was studied by using Resonance Raman spectroscopy. The results show that with the variation of Er 3+ concentrations, both the oxidation state and spin state of Mb are sensitive to the perturbation of Er 3+ . Er 3+ added to Mb affects the oxidation and spin state synchronously. The structure sensitive groups of Mb are more accessible to the Er 3+ than other groups. According to the fluorometry and CD spectra studied and our results as mentioned above, we considered that Er 3+ does not interact with heme directly, and Er 3+ probably leads to the conformational changes of Mb due to the change of oxidation and spin state of Heme. [WT5HZ]
基金the Deutsche Forschungsgemeinschaft (grant SFB 410)the German-Israeli Foundation for Scientific Research and Development (grant 881/05)+4 种基金the NSF(grant DMR-0342832)the U.S.Department of EnergyOffice of Basic Energy Sciencesunder contract DE-AC03-76SF00515Focus Center Research Program (FCRP) Center on Functional Engineered Nanoarchitectonics (FENA)
基金supported by the Key Programme of Grand Basic Research Programme of China (No.2007CB925001)the National Key Basic Research Programme of China (No. 001CB610604)the Grand Natural Science Research Programme of Anhui Education Department (Nos. ZD2007003-1 and KJ2010A074)
文摘The effect of Dy doping on magnetism of La 0.7 Sr 0.3 CoO 3 system was studied through the measurements of M-T curves and M-H curves. The results show that with Dy content increasing, T C decreases, M weakens, the coercive force strengthens, and the samples exhibit the abnormal phenomenon that M increases continuously with T decreasing in low temperature range. Research indicates that the variation of magnetism in the system comes from the changes of lattice parameters and magnetic environment caused by Dy doping and from the spin-state transition of Co ions induced by Dy ions.
基金supported by the National Natural Science Foundation of China under Grant Nos.12074300 and 11805146the Innovation Program for Quantum Science and Technology 2021ZD0302100the Fundamental Research Funds for the Central Universities.
文摘We present a novel class of Rydberg-mediated nuclear-spin entanglement in divalent atoms with global laser pulses.First,we show a fast nuclear-spin controlled phase gate of an arbitrary phase realizable either with two laser pulses when assisted by Stark shifts,or with three pulses.Second,we propose to create an electrons−nuclei-entangled state,which is named a super bell state(SBS)for it mimics a large Bell state incorporating three small Bell states.Third,we show a protocol to create a three-atom electrons-nuclei entangled state which contains the three-body W and Greenberger−Horne−Zeilinger(GHZ)states simultaneously.These protocols possess high intrinsic fidelities,do not require single-site Rydberg addressing,and can be executed with large Rydberg Rabi frequencies in a weak,Gauss-scale magnetic field.The latter two protocols can enable measurement-based preparation of Bell,hyperentangled,and GHZ states,and,specifically,SBS can enable quantum dense coding where one can share three classical bits of information by sending one particle.
基金the National Natural Science Foundation of China(Nos.21978324 and 22278436)the Science Foundation of China University of Petroleum,Beijing(No.2462021QNXZ009).
文摘The residual of oxidant chemicals in advanced oxidation processes(AOPs)resulted in both economic cost and secondary pollution.Herein,we report a direct oxidation of phenolic pollutants induced by Ca-Mn-O perovskites without using an oxidant.Governed by one-electron transfer process(ETP)from the phenolics to the Ca-Mn-O perovskites,this direct oxidation proceeds in fast reaction kinetics with activation energy of 51.4 kJ/mol,which was comparable with those AOPs-based catalytic systems.Additionally,mineralization and polymerization reactions occurred on the Ca-Mn-O surface and ensured the complete removal of phenolics.The high spin state Mn(III)within Ca-Mn-O structure was the dominant active site for this ETP.The elongated axial Mn(III)–O bonds within the[MnO_(6)]octahedron facilitated the acceptance of the electrons from the phenolics and thus promoted the initiation of the direct oxidation process.Mn(III)in the high spin state can also activate dissolved O_(2)to produce singlet oxygen(^(1)O_(2))for a fast removal of phenolics.The mixed Mn(III)/Mn(IV)within Ca-Mn-O accelerated the ETP by enhancing the electrical conductivity.This efficient Ca-Mn-O-induced ETP for removal of organic contaminants casts off the dependence on external chemical and energy inputs and provides a sustainable approach for transforming the toxic organic pollutants into value-added polymers.
基金supported by the National Natural Science Foundation of China(Nos.52271011,52102291).
文摘Carbon nanofibers(CNFs)with high specific surface area show great potential for sodium storage as a hard carbon material.Herein,CNFs anchored with Ni nanoparticles(CNFs/Ni)were prepared through chemical vapor deposition and impregnation reduction methods,in situ growing on the three-dimensional porous copper current collector(3DP-Cu).The coupling effect of high-spin state Ni nanopar-ticles leads to the increase of defect density and the expansion of lattice spacing of CNFs.Meanwhile,the 3DP-Cu ensures a high loading capacity of CNFs and short ion/electron transport channels.As an integral binder-free anode,the 3DP-Cu/CNFs/Ni exhibits excellent electrochemical performance,which demon-strates a high specific capacity with 298.5 mAh g^(-1)at 1000 mA g^(-1)after 1500 cycles,and a high power density with 200 mAh g^(-1)over 1000 cycles at 5000 mA g^(-1).Density functional theory calculation re-sults show that the high-spin state Ni regulates the electronic structure of CNFs,which significantly reduces the adsorption energy for Na^(+)(-2.7 Ev)and thus enables high-rate capability.The regulation of the electronic structure of carbon materials by high-spin state metal provides a new strategy for developing high-power carbonaceous anode materials for sodium-ion batteries.
基金financially supported by the National Natural Science Foundation of China(Nos.52002294 and 52202111)the Key Research and Development Program of Hubei Province(No.2021BAA208)+3 种基金the Knowledge Innovation Program of Wuhan-Shuguang Project(No.2022010801020364)City University of Hong Kong Donation Research Grant(No.DON-RMG 9229021)City University of Hong Kong Donation Grant(No.9220061)City University of Hong Kong Strategic Research Grant(SRG)(No.7005505)。
文摘Efficient electrocatalysts are vital to large-current hydrogen production in commercial water splitting for green energy generation.Herein,a novel heterophase engineering strategy is described to produce polymorphic CoSe_(2)electrocatalysts.The composition of the electrocatalysts consisting of both cubic CoSe_(2)(c-CoSe_(2))and orthorhombic CoSe_(2)(o-CoSe_(2))phases can be controlled precisely.Our results demonstrate that junction-induced spin-state modulation of Co atoms enhances the adsorption of intermediates and accelerates charge transfer resulting in superior large-current hydrogen evolution reaction(HER)properties.Specifically,the CoSe_(2)based heterophase catalyst with the optimal c-CoSe_(2)content requires an overpotential of merely 240 mV to achieve 1,000 mA·cm^(-2)as well as a Tafel slope of 50.4 mV·dec^(-1).Furthermore,the electrocatalyst can maintain a large current density of 1,500 mA·cm^(-2)for over 320 h without decay.The results reveal the advantages and potential of heterophase junction engineering pertaining to design and fabrication of low-cost transition metal catalysts for large-current water splitting.
文摘In this paper,an integrated guidance and control method based on an adaptive path-following controller is proposed to control a spin-stabilized projectile with only translational motion information under the constraint of an actuator,uncertainties in aerodynamic parameters and measurements,and control system complexity.Owing to the fairly high rotation speed,the dynamic model of this missile is strongly nonlinear,uncertain and coupled in pitch,yaw and roll channels.A theoretical equivalent resultant force and uncertainty compensation method are comprehensively used to realize decoupling of pitch and yaw.In response to the strong nonlinear and time-varying characteristics of the dynamic system,the quasi-linear model whose parameters are obtained by interpolation of points selected as the segmentation points in the trajectory envelope,is used for calculation in each step.To cope with the system uncertainty caused by model approximation,parameter uncertainty and ballistic interference,an extended state estimator is used to compensate the output feedback according to the test ballistic angle.In order to improve the tracking efficiency and ensure the tracking error convergence with only translational motion information,the virtual guide point,whose derivative is deduced according to the Lyapunov principle,is calculated in real time according to the projection relationship between the real-time position and the reference trajectory,and a virtual line-of-sight angle and the backstepping method are used for the design of the guidance and control system.In order to avoid the influence of control input saturation on the guidance and control performance due to the actuator limitation and improve the robustness of the system,an anti-saturation compensator is designed according to the two-step method.The feasibility and effectiveness of the path-following controller is verified through closed-loop flight simulations with measurement,control,and condition uncertainties.The results indicate that the designed controller can conv
基金supported by the National Natural Science Foundation of China Youth Fund(12105234)。
文摘The distribution of the nuclear ground-state spin in a two-body random ensemble(TBRE)was studied using a general classification neural network(NN)model with two-body interaction matrix elements as input features and the corresponding ground-state spins as labels or output predictions.The quantum many-body system problem exceeds the capability of our optimized NNs in terms of accurately predicting the ground-state spin of each sample within the TBRE.However,our NN model effectively captured the statistical properties of the ground-state spin because it learned the empirical regularity of the ground-state spin distribution in TBRE,as discovered by physicists.
基金supported by JSPS KAKENHI(18H03676)JST CREST(JPMJCR1874)supported by RIKEN Special Postdoctoral Researcher Program。
文摘Non-Hermitian systems have been discussed mostly in the context of open systems and nonequilibrium.Recent experimental progress is much from optical,cold-atomic,and classical platforms due to the vast tunability and clear identification of observables.However,their counterpart in solid-state electronic systems in equilibrium remains unmasked although highly desired,where a variety of materials are available,calculations are solidly founded,and accurate spectroscopic techniques can be applied.We demonstrate that,in the surface state of a topological insulator with spin-dependent relaxation due to magnetic impurities,highly nontrivial topological soliton spin textures appear in momentum space.Such spin-channel phenomena are delicately related to the type of non-Hermiticity and correctly reveal the most robust non-Hermitian features detectable spectroscopically.Moreover,the distinct topological soliton objects can be deformed to each other,mediated by topological transitions driven by tuning across a critical direction of doped magnetism.These results not only open a solid-state avenue to exotic spin patterns via spin-and angle-resolved photoemission spectroscopy,but also inspire non-Hermitian dissipation engineering of spins in solids.
基金financially supported by the National Natural Science Foundation of China(Grant Nos.22178148,22278193,22075113)the Jiangsu Province and Education Ministry Co-Sponsored Synergistic Innovation Center of Modern Agricultural Equipment(Grant No.XTCX2029)+1 种基金a Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutionsthe Postgraduate Research&Practice Innovation Program of Jiangsu Province(Grant No.KYCX22_3691)。
文摘Owing to the distinctive structural characteristics,vanadium nitride(VN)is highly regarded as a catalyst for oxygen reduction reaction(ORR)in zinc-air batteries(ZABs).However,VN exhibits limited intrinsic ORR activity due to the weak adsorption ability to O-containing species.Here,the S-doped VN anchored on N,S-doped multi-dimensional carbon(S-VN/Co/NS-MC)was constructed using the solvothermal and in-situ doping methods.Incorporating sulfur atoms into VN species alters the electron spin state of vanadium in the S-VN/Co/NS-MC for regulating the adsorption energy of vanadium sites to oxygen molecules.The introduced sulfur atoms polarize the V 3d_(z)^(2) electrons,shifting spin-down electrons closer to the Fermi level in the S-VN/Co/NS-MC.Consequently,the introduction of sulfur atoms into VN species enhances the adsorption energy of vanadium sites for oxygen molecules.The*OOH dissociation transitions from being unspontaneous on the VN surface to a spontaneous state on the S-doped VN surface.Then,the ORR barrier on the S-VN/Co/NS-MC surface is reduced.The S-VN/Co/NS-MC demonstrates a higher half-wave potential and limiting current density compared to the VN/Co/N-MC.The S-VN/Co/NS-MC-based liquid ZABs display a power density of 195.7 m W cm^(-2),a specific capacity of 815.7 m A h g^(-1),and a cycling stability exceeding 250 h.The S-VN/Co/NS-MC-based flexible ZABs are successfully employed to charge both a smart watch and a mobile phone.This approach holds promise for advancing the commercial utilization of VN-based catalysts in ZABs.
基金supported by the National Key Research and Development Program of China (2022YFB4002100)the development project of Zhejiang Province's "Jianbing" and "Lingyan" (2023C01226)+4 种基金the National Natural Science Foundation of China (22278364, U22A20432, 22238008, 22211530045, and 22178308)the Fundamental Research Funds for the Central Universities (226-2022-00044 and 226-2022-00055)the Science Foundation of Donghai Laboratory (DH-2022ZY0009)the Startup Foundation for Hundred-Talent Program of Zhejiang UniversityScientific Research Fund of Zhejiang Provincial Education Department.
文摘Metal-organic frameworks(MOFs)have been developed as an ideal platform for exploration of the relationship between intrinsic structure and catalytic activity,but the limited catalytic activity and stability has hampered their practical use in water splitting.Herein,we develop a bond length adjustment strategy for optimizing naphthalene-based MOFs that synthesized by acid etching Co-naphthalenedicarboxylic acid-based MOFs(donated as AE-CoNDA)to serve as efficient catalyst for water splitting.AE-CoNDA exhibits a low overpotential of 260 mV to reach 10 mA cm^(−2)and a small Tafel slope of 62 mV dec^(−1)with excellent stability over 100 h.After integrated AE-CoNDA onto BiVO_(4),photocurrent density of 4.3 mA cm^(−2)is achieved at 1.23 V.Experimental investigations demonstrate that the stretched Co-O bond length was found to optimize the orbitals hybridization of Co 3d and O 2p,which accounts for the fast kinetics and high activity.Theoretical calculations reveal that the stretched Co-O bond length strengthens the adsorption of oxygen-contained intermediates at the Co active sites for highly efficient water splitting.
基金supported by Beijing Natural Science Foundation(No.JQ22006)King Abdullah University of Science and Technology Research Funding(KRF)under Award(No.ORA-2021-CRG10-4668.4).
文摘Open-shell oligomers and polymers have exhibited intriguing electronic and magnetic properties, making them highly desirable for a wide range of applications, including ambipolar organic field-effect transistors (OFETs), photodetectors, organic thermoelectrics, and spintronics. Although open-shell ground states have been observed in certain small molecules and doped organic semiconductors, the exploration of open-shell ground-state conjugated polymers is still limited, and the strategies for designing these polymers remain obscure. This review aims to briefly introduce the theory and characterization methods of open-shell conjugated polymers, along with an overview of recent progress and applications. The objective is to stimulate further advancements and investigations in this promising area by shedding light on the potential of open-shell conjugated polymers and the challenges that lie ahead.
基金the National Natural Science Foundation of China(Nos.52271011,52102291).
文摘Carbon nanofibers(CNFs)have received extensive and in-depth studied as anodes for sodium-ion batteries(SIBs),and yet their initial Coulombic efficiency and rate capability remain enormous challenge at practical level.Herein,CNFs anchored with cobalt nanocluster(CNFs-Co)were prepared using chemical vapor deposition and thermal reduction methods.The as-prepared CNFs-Co shows a high initial Coulombic efficiency of 91%and a high specific discharge capacity of 246 mAh/g at 0.1 A/g after 200 cycles as anode for SIBs.Meanwhile,the CNFs-Co anode still delivers a high cycling stability with 108 mAh/g after 1000 cycles at 10 A/g.These excellent electrochemical properties could be attributed to the involved spin state Co,which endows CNFs with large interplanar spacing(0.39 nm)and abundant vacancy defects.Importantly,the spin state Co downshifts the p-band center of carbon and strengthens the Na+adsorption energy from-2.33 eV to-2.64 eV based on density functional theory calculation.This novel strategy of modulating the carbon electronic structure by the spin state of magnetic metals provides a reference for the development of high-performance carbon-based anode materials.
