The stability and electrocatalytic efficiency of transition metal oxides for water splitting is determined by geometric and electronic structure,especially under high current densities.Herein,a newly designed lamella-...The stability and electrocatalytic efficiency of transition metal oxides for water splitting is determined by geometric and electronic structure,especially under high current densities.Herein,a newly designed lamella-heterostructured nanoporous CoFe/CoFe_(2)O_(4) and CeO_(2−x),in situ grown on nickel foam(NF),holds great promise as a high-efficient bifunctional electrocatalyst(named R-CoFe/Ce/NF)for water splitting.Experimental characterization verifies surface reconstruction from CoFe alloy/oxide to highly active CoFeOOH during in situ electrochemical polarization.By virtues of three-dimensional nanoporous architecture and abundant electroactive CoFeOOH/CeO_(2−x) heterostructure interfaces,the R-CoFe/Ce/NF electrode achieves low overpotentials for oxygen evolution(η_(10)=227 mV;η_(500)=450 mV)and hydrogen evolution(η_(10)=35 mV;η_(408)=560 mV)reactions with high normalized electrochemical active surface areas,respectively.Additionally,the alkaline full water splitting electrolyzer of R-CoFe/Ce/NF||R-CoFe/Ce/NF achieves a current density of 50 mA·cm^(−2) only at 1.75 V;the decline of activity is satisfactory after 100-h durability test at 300 mA·cm^(−2).Density functional theory also demonstrates that the electron can transfer from CeO_(2−x) by virtue of O atom to CoFeOOH at CoFeOOH/CeO_(2−x) heterointerfaces and enhancing the adsorption of reactant,thus optimizing electronic structure and Gibbs free energies for the improvement of the activity for water splitting.展开更多
DC-inverter split air-conditioner is widely used in Chinese homes as a result of its high-efficiency and energy-saving. Recently, the researches on its outdoor unit have focused on the influence of surrounding structu...DC-inverter split air-conditioner is widely used in Chinese homes as a result of its high-efficiency and energy-saving. Recently, the researches on its outdoor unit have focused on the influence of surrounding structures upon the aerodynamic and acoustic performance, however they are only limited to the influence of a few parameters on the performance, and practical design of the unit requires more detailed parametric analysis. Three-dimensional computational fluid dynamics（CFD） and computational aerodynamic acoustics（CAA） simulation based on FLUENT solver is used to study the influence of surrounding structures upon the aforementioned properties of the unit. The flow rate and sound pressure level are predicted for different rotating speed, and agree well with the experimental results. The parametric influence of three main surrounding structures（i.e. the heat sink, the bell-mouth type shroud and the outlet grille） upon the aerodynamic performance of the unit is analyzed thoroughly. The results demonstrate that the tip vortex plays a major role in the flow fields near the blade tip and has a great effect on the flow field of the unit. The inlet ring＇s size and throat＇s depth of the bell-mouth type shroud, and the through-flow area and configuration of upwind and downwind sections of the outlet grille are the most important factors that affect the aerodynamic performance of the unit. Furthermore, two improved schemes against the existing prototype of the unit are developed, which both can significantly increase the flow rate more than 6 %（i.e. 100 m3·h～（-1）） at given rotating speeds. The inevitable increase of flow noise level when flow rate is increased and the advantage of keeping a lower rotating speed are also discussed. The presented work could be a useful guideline in designing the aerodynamic and acoustic performance of the split air-conditioner in engineering practice.展开更多
Constructing heterointerface engineering has becoming an effective and general strategy for developing highly efficient and durable nonnoble electrocatalysts for catalyzing both hydrogen evolution reaction(HER)and oxy...Constructing heterointerface engineering has becoming an effective and general strategy for developing highly efficient and durable nonnoble electrocatalysts for catalyzing both hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).In this work,we synthesized a self-supporting heterogeneous NiSe@Co_(0.85)Se/NF electrocatalyst using a facile in situ selenization of transition metal precursors that coated on the nickel foam(NF)in polyol solution.The NF was used as both conductive substrate and nickel source,ensuring superior electronic conductivity for catalyzing.The NiSe@-Co_(0.85)Se/NF exhibited remarkable bifunctional electrocatalytic activities with HER overpotential of 168 mV and OER overpotential of 258 mV to achieve 10 mA·cm-2.The water splitting system using NiSe@Co_(0.85)Se/NF as both anode and cathode electrodes achieved a current density of 10 mA·cm^(-2) at 1.61 V with nearly 100% faradaic efficiency and impressively long-term stability.The efficient bifunctional catalytic performance of NiSe@-Co_(0.85)Se/NF should be attributed to the electronic modulation and synergistic effect between NiSe and Co_(0.85)Se,the intrinsic metallic conductivity and the enlarged active sites exposure.This work provides a facile method for developing heterogeneous bifunctional catalysts for advanced electrochemical energy conversion technologies.展开更多
Stable non-noble metal bifunctional electrocatalysts are one of the challenges to the fluctuating overall water splitting driven by re-newable energy.Herein,a novel self-supporting hierarchically porous Ni_(x)Fe-S/NiF...Stable non-noble metal bifunctional electrocatalysts are one of the challenges to the fluctuating overall water splitting driven by re-newable energy.Herein,a novel self-supporting hierarchically porous Ni_(x)Fe-S/NiFe_(2)O_(4) heterostructure as bifunctional electrocatalyst was constructed based on porous Ni-Fe electrodeposition on three-dimensional(3D)carbon fiber cloth,in situ oxidation,and chemical sulfuration.Results showed that the Ni_(x)Fe-S/NiFe_(2)O_(4) heterostructure with a large specific surface area exhibits good bifunctional activity and stability for both hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)because of the abundance of active sites,synergistic effect of the heterostructure,superhydrophilic surface,and stable,self-supporting structure.The results further confirmed that the Ni_(x)Fe-S phase in the heterostructure is transformed into metal oxides/hydroxides and Ni_(3)S_(2) during OER.Compared with the commercial 20wt%Pt/C||IrO_(2)-Ta_(2)O_(5) electrolyzer,the self-supporting Ni1/5Fe-S/NiFe_(2)O_(4)||Ni1/2Fe-S/NiFe_(2)O_(4) electrolyzer exhibits better stability and lower cell voltage in the fluctu-ating current density range of 10-500 mA/cm^(2).Particularly,the cell voltage of Ni1/5Fe-S/NiFe_(2)O_(4)||Ni1/2Fe-S/NiFe_(2)O_(4) is only approximately 3.91 V at an industrial current density of 500 mA/cm^(2),which is lower than that of the 20wt%Pt/C||IrO_(2)-Ta_(2)O_(5) electrolyzer(i.e.,approximately 4.79 V).This work provides a promising strategy to develop excellent bifunctional electrocatalysts for fluctuating overall water splitting.展开更多
Transition-metal phosphides(TMPs)with high catalytic activity are widely used in the design of electrodes for water splitting.However,a major challenge is how to achieve the trade-off between activity and stability of...Transition-metal phosphides(TMPs)with high catalytic activity are widely used in the design of electrodes for water splitting.However,a major challenge is how to achieve the trade-off between activity and stability of TMPs.Herein,a novel method for synthesizing CoP nanoparticles encapsu-lated in a rich-defect carbon shell(CoP/DCS)is developed through the self-assembly of modified polycyclic aromatic molecules.The graft and removal of high-activity C-N bonds of aromatic molecules render the controllable design of crystallite defects of carbon shell.The density functional theory calculation indicates that the carbon defects with unpaired electrons could effectively tailor the band structure of CoP.Benefiting from the improved activity and corrosion resistance,the CoP/DCS delivers outstanding difunctional hydrogen evolution reaction(88 mV)and oxygen evolution reaction(251 mV)performances at 10 mA cm^(−2)current density.Furthermore,the coupled water electrolyzer with CoP/DCS as both the cathode and anode presents ultralow cell voltages of 1.49 V to achieve 10 mA cm^(−2)with long-time stability.This strategy to improve TMPs electrocatalyst with rich-DCS and heterogeneous structure will inspire the design of other transition metal compound electrocatalysts for water splitting.展开更多
Photoelectrochemical(PEC) water splitting offers the capability of harvesting, storing, and converting solar energy into clean and sustainable hydrogen energy. Metal oxides are appealing photoelectrode materials becau...Photoelectrochemical(PEC) water splitting offers the capability of harvesting, storing, and converting solar energy into clean and sustainable hydrogen energy. Metal oxides are appealing photoelectrode materials because of their easy manufacturing and relatively high stability. In particular, metal oxides prepared by electrochemical anodization are typical of ordered nanostructures, which are beneficial for light harvesting, charge transfer and transport, and the adsorption and desorption of reactive species due to their high specific surface area and rich channels. However, bare anodic oxides still suffer from low charge separation and sunlight absorption efficiencies. Accordingly, many strategies of modifying anodic oxides have been explored and investigated. In this review, we attempt to summarize the recent advances in the rational design and modifications of these oxides from processes before, during, and after anodization. Rational design strategies are thoroughly addressed for each part with an aim to boost overall PEC performance. The ongoing efforts and challenges for future development of practical PEC electrodes are also presented.展开更多
To effectively address energy challenges,it is crucial to explore efficient and stable bifunctional nonprecious metal catalysts.In this study,a Mo-doped nickeliron layered double hydroxide with flower-cluster architec...To effectively address energy challenges,it is crucial to explore efficient and stable bifunctional nonprecious metal catalysts.In this study,a Mo-doped nickeliron layered double hydroxide with flower-cluster architecture was successfully prepared by a one-step hydrothermal method,which demonstrated a good water splitting performance.After an appropriate amount of Mo doping,some lattice distortions in the material provided reactive sites for the adsorption and conversion of intermediates,thus optimising the charge distribution of the material.Moreover,the multidimensional void structures formed after doping had a larger specific surface area and accelerated the penetration of the electrolyte,which significantly improved the activity of the catalyst in alkaline media.At 10 mA·cm^(-2),the hydrogen and oxygen evolution overpotentials of Mo-doped nickel-iron double hydroxides(Mo-NiFe LDH/NF-0.2)were 167 and 220 mV,respectively,with an excellent durability up to 24 h.When the Mo-NiFe LDH/NF-0,2 catalyst was used as the cathode and anode of an electrolytic cell,the catalyst achieved a current density of 10 mA·cm^(-2)at an applied voltage of 1.643 V.This study provides a novel approach for designing excellent bifunctional electrocatalysts containing nonprecious metals.展开更多
Photoelectrocatalytic(PEC)seawater splitting as a green and sustainable route to harvest hydrogen is attractive yet hampered by low activity of photoanodes and unexpected high selectivity to the corrosive and toxic ch...Photoelectrocatalytic(PEC)seawater splitting as a green and sustainable route to harvest hydrogen is attractive yet hampered by low activity of photoanodes and unexpected high selectivity to the corrosive and toxic chlorine.Especially,it is full of challenges to unveil the key factors influencing the selectivity of such complex PEC processes.Herein,by regulating the energy band and surface structure of the anatase TiO_(2) nanotube array photoanode via nitrogen-doping,the seawater PEC oxidation shifts from Cl^(-)oxidation reaction(ClOR)dominant on the TiO_(2) photoanode(61.6%)to oxygen evolution reaction(OER)dominant on the N-TiO_(2) photoanode(62.9%).Comprehensive investigations including operando photoelectrochemical FTIR and DFT calculations unveil that the asymmetric hydrogen-bonding water at the N-TiO_(2) electrode/electrolyte interface enriches under illumination,facilitating proton transfer and moderate adsorption strength of oxygen-intermediates,which lowers the energy barrier for the OER yet elevates the energy barrier for the ClOR,resulting to a promoted selectivity towards the OER.The work sheds light on the underlying mechanism of the PEC water oxidation processes,and highlights the crucial role of interfacial water on the PEC selectivity,which could be regulated by controlling the energy band and the surface structure of semiconductors.展开更多
This study investigates the dynamic compressive behavior of three periodic lattice structures fabricated from Ti-6Al-4V titanium alloy,each with distinct topologies:simple cubic(SC),body-centered cubic(BCC),and face-c...This study investigates the dynamic compressive behavior of three periodic lattice structures fabricated from Ti-6Al-4V titanium alloy,each with distinct topologies:simple cubic(SC),body-centered cubic(BCC),and face-centered cubic(FCC).Dynamic compression experiments were conducted using a Split Hopkinson Pressure Bar(SHPB)system,complemented by high-speed imaging to capture real-time deformation and failure mechanisms under impact loading.The influence of cell topology,relative density,and strain rate on dynamic mechanical properties,failure behavior,and stress wave propagation was systematically examined.Finite element modeling was performed,and the simulated results showed good agreement with experimental data.The findings reveal that the dynamic mechanical properties of the lattice structures are generally insensitive to strain rate variations,while failure behavior is predominantly governed by structural configuration.The SC structure exhibited strut buckling and instability-induced fracture,whereas the BCC and FCC structures displayed layer-by-layer crushing with lower strain rate sensitivity.Regarding stress wave propagation,all structures demonstrated significant attenuation capabilities,with the BCC structure achieving the greatest reduction in transmitted wave amplitude and energy.Across all configurations,wave reflection was identified as the primary energy dissipation mechanism.These results provide critical insights into the design of lattice structures for impact mitigation and energy absorption applications.展开更多
A comprehensive theoretical study of correlation effects on the fine-structure splitting within the ground configuration 3d9 of the Co-like HI45＋, Ta46＋, W47＋, and Au52＋ ions is performed by employing the multi-co...A comprehensive theoretical study of correlation effects on the fine-structure splitting within the ground configuration 3d9 of the Co-like HI45＋, Ta46＋, W47＋, and Au52＋ ions is performed by employing the multi-configuration Dirac-Hartree- Fock method in the active space approximation. It shows that the core-valence correlation with the inner-core 2p electron is more significant than with the outer 3p and 3s electrons, and the correlation with the 2s electron is also noticeable. The core-core correlation seems to be small and can be ignored. The calculated 2D3/2,5/2 splitting energies agree with the recent electron-beam ion-trap measurements [Phys. Rev. A 83 032517 （2011）, Eur. Phys. J. D 66 286 （2012）] to within the experimental uncertainties.展开更多
The inter-relation between zero-field splitting （ZFS） parameters and local lattice structures of the （CrSe4）6 clusters in ZnSe semiconductors has been established by using the complete diagonalization （of the ene...The inter-relation between zero-field splitting （ZFS） parameters and local lattice structures of the （CrSe4）6 clusters in ZnSe semiconductors has been established by using the complete diagonalization （of the energy matrix） method. On the basis of this, the local lattice distortions, the ZFS parameters D, a, F and the optical spectrum for Cr2＋ ions doped into ZnSe are theoretically investigated, and the contributions of the spin singlets have been taken into account. The calculated ZFS parameters are in good agreement with the experimental values. From our calculations, the tetragonal distortion parameters AR = 0.091A and Aθ = 4.28° of Cr2＋ in ZnSe are acquired, and the results suggest that there exists a tetragonal expansion distortion for the local lattice structure of （CrSe4）6- clusters in ZnSe crystals. The influence of the spin singlets on ZFS parameters is also discussed, indicating that the contributions to ZFS parameters a and F cannot be ignored.展开更多
In order to find the main factors that influence the urban traffic structure,a relational model between the travelers＇ characteristics and the trip mode choice is built.The data of urban residents＇ characteristics a...In order to find the main factors that influence the urban traffic structure,a relational model between the travelers＇ characteristics and the trip mode choice is built.The data of urban residents＇ characteristics are obtained from statistical data,while the trip mode split data is collected through a trip survey in Bengbu.In addition,the discrete choice model is adopted to build the functional relationship between the mode choice and the travelers＇ personal characteristics,as well as family characteristics and trip characteristics.The model shows that the relationship between the mode split and the personal,as well as family and trip characteristics is stable and changes little as the time changes.Deduced by the discrete model,the mode split result is relatively accurate and can be feasibly used for trip mode structure forecasts.Furthermore,the proposed model can also contribute to find the key influencing factors on trip mode choice,and restructure or optimize the urban trip mode structure.展开更多
The high order compact d if ference method is developed for solving the perturbation equations based on Navi er Stokes equations, and is used in studying complex evolution processes from w all negative pulse to the ...The high order compact d if ference method is developed for solving the perturbation equations based on Navi er Stokes equations, and is used in studying complex evolution processes from w all negative pulse to the turbulent coherent structure in the channel flow. Th is method contains three dimensional coupling difference scheme with high accur acy and high resolution, and the high order time splitting methods. Compared with the general spectral method, the method can be used to research turbule nt coherent structure under more general boundary conditions and in flow domains . In this paper, the generation and evolution of the turbulent coherent structur es ind uced by wall pulse in the channel flow are simulated, and the basic characterist ics and rules of the turbulent coherent structure are shown. Computational r esults indicate that a wall negative pulse is more convenient than the resonant three wave model.展开更多
The green hydrogen generation powered by renewable electricity promises the potential decarbonization of the hard-to-abate sector and is essential for the fulfillment of the Paris Agreement that attempts to limit the ...The green hydrogen generation powered by renewable electricity promises the potential decarbonization of the hard-to-abate sector and is essential for the fulfillment of the Paris Agreement that attempts to limit the global average temperature rise in the range of 1.5–2.0 ℃ above the pre-industrial level by the end of this century. Tremendous efforts have been devoted to the optimization of the electrocatalytic performance of the catalysts under industrial-relevant current densities via rational structure design,which induces a preferential electron distribution that favors the adsorption/desorption behavior of the key intermediates, thus accelerating the reaction kinetics. In this review, a brief introduction of the current energy status will be first presented to necessitate the importance of green hydrogen.Followed by the basic concepts and fundamental understanding of the reaction mechanisms, we present efficient strategies for the enhancement of the electrocatalytic performance of the catalysts to meet the rigorous requirement under industrial conditions and the in-depth understanding behind the reinforcement will be briefly discussed next. Then the recent advances regarding the rational design of electrocatalysts operating at an industrial scale will be summarized. Finally, the challenges and perspectives in this thriving field will be proposed from our point of view.展开更多
In the present study,split tensile strength of self-compacting concrete with different amount of CuO nanoparticles has been investigated.CuO nanoparticles with the average particle size of 15 nm were added partially t...In the present study,split tensile strength of self-compacting concrete with different amount of CuO nanoparticles has been investigated.CuO nanoparticles with the average particle size of 15 nm were added partially to self compacting concrete and split tensile strength of the specimens has been measured.The results indicate that CuO nanoparticles are able to improve the split tensile strength of self compacting concrete and recover the negative effects of polycarboxylate superplasticizer on split tensile strength.CuO nanoparticle as a partial replacement of cement up to 4 wt% could accelerate C-S-H gel formation as a result of increased crystalline Ca（OH）2 amount at the early ages of hydration.The increase of the CuO nanoparticles more than 4 wt% causes the decrease of the split tensile strength because of unsuitable dispersion of nanoparticles in the concrete matrix.Accelerated peak appearance in conduction calorimetry tests,more weight loss in thermogravimetric analysis and more rapid appearance of related peaks to hydrated products in X-ray diffraction（XRD） results all also indicate that CuO nanoparticles up to4 wt% could improve the mechanical and physical properties of the specimens.Finally,CuO nanoparticles could improve the pore structure of concrete and shift the distributed pores to harmless and few-harm pores.展开更多
Complexes Cl-RuⅡ（dppe）2（Fe Cl4）·2CH2Cl2（2） and Br-RuII（dppe）2（Fe Br4）·2CH2Cl2（3） were prepared by the reaction of trans-RuII（dppe）2Cl2（1） with FeX 3（X = Cl, Br）. More interestingly, the ce...Complexes Cl-RuⅡ（dppe）2（Fe Cl4）·2CH2Cl2（2） and Br-RuII（dppe）2（Fe Br4）·2CH2Cl2（3） were prepared by the reaction of trans-RuII（dppe）2Cl2（1） with FeX 3（X = Cl, Br）. More interestingly, the central Ru atoms of RuII（dppe）-based complexes（2 and 3） define a tetragonal pyramid with five-coordination. The temperature dependence magnetic susceptibilities indicate that the xMT values of complexes 2 and 3 are almost constant at 50~300 K, and the xMT values sharply decrease with further decreasing the temperature at low temperature due to the zero-field splitting（ZFS） of high spin Fe（III） ions.展开更多
The dynamic characteristics of the large scale coherent structures in a forced free shear layer are experi- mentally studied by means of flow visualization. The quantitative measurements are acquired by the use of a L...The dynamic characteristics of the large scale coherent structures in a forced free shear layer are experi- mentally studied by means of flow visualization. The quantitative measurements are acquired by the use of a LDV. It is shown that the development of the coherent structures can be greatly influenced by upstream artificial perturbations and as a result the mixing in the layer can be controlled. Like vortex merging, vortex splitting is also a common evolu- tion pattern in the development of the coherent structures.展开更多
Developing bifunctional electrocatalysts with both high catalytic activity and high stability is crucial for efficient water splitting in alkaline media.Herein,a Fe-incorporated dual-metal selenide on nickel foam(Co_(...Developing bifunctional electrocatalysts with both high catalytic activity and high stability is crucial for efficient water splitting in alkaline media.Herein,a Fe-incorporated dual-metal selenide on nickel foam(Co_(0.9)Fe_(0.1)-Se/NF) is synthesized via a facile one-step electrodeposition method.As-synthesized materials could serve as self-supported bifunctional electrocatalysts with excellent catalytic activity towards oxygen evolution reaction(OER) and hydrogen evolution reaction(HER) in alkaline media.Experimental results show that delivering a 10 mA cm^(-2) water splitting current density only requires a cell voltage of 1.55 V.In addition,a very stable performance could be kept for about 36 hours,indicating their excellent working stability.Moreover,by means of phase analysis,we have identified that the evolution of the synthesized Co_(0.9)Fe_(0.1)-Se/NF experiences two entirely different processes in HER and OER,which hydroxide and oxyhydroxide are regarded as the real active sites,respectively.This work may pave the way to further understanding the relationships between the reactivity and stability of chalcogenide-based electrocatalysts and facilitating the rational design of efficient electrocatalysts for future renewable energy system applications.展开更多
In this paper,a unit cell of a single-negative metamaterial structure loaded with a meander line and defected ground structure(DGS)is investigated as the principle radiating element of an antenna.The unit cell antenna...In this paper,a unit cell of a single-negative metamaterial structure loaded with a meander line and defected ground structure(DGS)is investigated as the principle radiating element of an antenna.The unit cell antenna causes even or odd mode resonances similar to the unit cell structure depending on the orientation of the microstrip feed used to excite the unit cell.However,the orientation which gives low-frequency resonance is considered here.The unit cell antenna is then loaded with a meander line which is parallel to the split bearing side and connects the other two sides orthogonal to the split bearing side.This modified structure excites another mode of resonance at high frequency when a meander line defect is loaded on the metallic ground plane.Specific parameters of the meander line structure,the DGS shape,and the unit cell are optimized to place these two resonances at different frequencies with proper frequency intervals to enhance the bandwidth.Finally,the feed is placed in an offset position for better impedance matching without affecting the bandwidth The compact dimension of the antenna is 0.25λL×0.23λL×0.02λL,whereλL is the free space wavelength with respect to the center frequency of the impedance bandwidth.The proposed antenna is fabricated and measured.Experimental results reveal that the modified design gives monopole like radiation patterns which achieves a fractional operating bandwidth of 26.6%,from 3.26 to 4.26 GHz for|S11|<−10 dB and a pick gain of 1.26 dBi is realized.In addition,the simulated and measured crosspolarization levels are both less than−15 dB in the horizontal plane.展开更多
基金sponsored by the National Natural Science Foundation of China(Nos.5210125 and 52375422)the Science Research Project of Hebei Education Department(No.BJK2023058)the Natural Science Foundation of Hebei Province(Nos.E2020208069,B2020208083 and E202320801).
文摘The stability and electrocatalytic efficiency of transition metal oxides for water splitting is determined by geometric and electronic structure,especially under high current densities.Herein,a newly designed lamella-heterostructured nanoporous CoFe/CoFe_(2)O_(4) and CeO_(2−x),in situ grown on nickel foam(NF),holds great promise as a high-efficient bifunctional electrocatalyst(named R-CoFe/Ce/NF)for water splitting.Experimental characterization verifies surface reconstruction from CoFe alloy/oxide to highly active CoFeOOH during in situ electrochemical polarization.By virtues of three-dimensional nanoporous architecture and abundant electroactive CoFeOOH/CeO_(2−x) heterostructure interfaces,the R-CoFe/Ce/NF electrode achieves low overpotentials for oxygen evolution(η_(10)=227 mV;η_(500)=450 mV)and hydrogen evolution(η_(10)=35 mV;η_(408)=560 mV)reactions with high normalized electrochemical active surface areas,respectively.Additionally,the alkaline full water splitting electrolyzer of R-CoFe/Ce/NF||R-CoFe/Ce/NF achieves a current density of 50 mA·cm^(−2) only at 1.75 V;the decline of activity is satisfactory after 100-h durability test at 300 mA·cm^(−2).Density functional theory also demonstrates that the electron can transfer from CeO_(2−x) by virtue of O atom to CoFeOOH at CoFeOOH/CeO_(2−x) heterointerfaces and enhancing the adsorption of reactant,thus optimizing electronic structure and Gibbs free energies for the improvement of the activity for water splitting.
基金Supported by Program for Changjiang Scholars and Innovative Research Team in University,Ministry of Education of China(PCSIRT)
文摘DC-inverter split air-conditioner is widely used in Chinese homes as a result of its high-efficiency and energy-saving. Recently, the researches on its outdoor unit have focused on the influence of surrounding structures upon the aerodynamic and acoustic performance, however they are only limited to the influence of a few parameters on the performance, and practical design of the unit requires more detailed parametric analysis. Three-dimensional computational fluid dynamics（CFD） and computational aerodynamic acoustics（CAA） simulation based on FLUENT solver is used to study the influence of surrounding structures upon the aforementioned properties of the unit. The flow rate and sound pressure level are predicted for different rotating speed, and agree well with the experimental results. The parametric influence of three main surrounding structures（i.e. the heat sink, the bell-mouth type shroud and the outlet grille） upon the aerodynamic performance of the unit is analyzed thoroughly. The results demonstrate that the tip vortex plays a major role in the flow fields near the blade tip and has a great effect on the flow field of the unit. The inlet ring＇s size and throat＇s depth of the bell-mouth type shroud, and the through-flow area and configuration of upwind and downwind sections of the outlet grille are the most important factors that affect the aerodynamic performance of the unit. Furthermore, two improved schemes against the existing prototype of the unit are developed, which both can significantly increase the flow rate more than 6 %（i.e. 100 m3·h～（-1）） at given rotating speeds. The inevitable increase of flow noise level when flow rate is increased and the advantage of keeping a lower rotating speed are also discussed. The presented work could be a useful guideline in designing the aerodynamic and acoustic performance of the split air-conditioner in engineering practice.
基金financially supported by the National Natural Science Foundation of China(No.51804216)。
文摘Constructing heterointerface engineering has becoming an effective and general strategy for developing highly efficient and durable nonnoble electrocatalysts for catalyzing both hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).In this work,we synthesized a self-supporting heterogeneous NiSe@Co_(0.85)Se/NF electrocatalyst using a facile in situ selenization of transition metal precursors that coated on the nickel foam(NF)in polyol solution.The NF was used as both conductive substrate and nickel source,ensuring superior electronic conductivity for catalyzing.The NiSe@-Co_(0.85)Se/NF exhibited remarkable bifunctional electrocatalytic activities with HER overpotential of 168 mV and OER overpotential of 258 mV to achieve 10 mA·cm-2.The water splitting system using NiSe@Co_(0.85)Se/NF as both anode and cathode electrodes achieved a current density of 10 mA·cm^(-2) at 1.61 V with nearly 100% faradaic efficiency and impressively long-term stability.The efficient bifunctional catalytic performance of NiSe@-Co_(0.85)Se/NF should be attributed to the electronic modulation and synergistic effect between NiSe and Co_(0.85)Se,the intrinsic metallic conductivity and the enlarged active sites exposure.This work provides a facile method for developing heterogeneous bifunctional catalysts for advanced electrochemical energy conversion technologies.
基金financially supported by the National Natural Science Foundation of China (Nos. 51874020 and 52004022)
文摘Stable non-noble metal bifunctional electrocatalysts are one of the challenges to the fluctuating overall water splitting driven by re-newable energy.Herein,a novel self-supporting hierarchically porous Ni_(x)Fe-S/NiFe_(2)O_(4) heterostructure as bifunctional electrocatalyst was constructed based on porous Ni-Fe electrodeposition on three-dimensional(3D)carbon fiber cloth,in situ oxidation,and chemical sulfuration.Results showed that the Ni_(x)Fe-S/NiFe_(2)O_(4) heterostructure with a large specific surface area exhibits good bifunctional activity and stability for both hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)because of the abundance of active sites,synergistic effect of the heterostructure,superhydrophilic surface,and stable,self-supporting structure.The results further confirmed that the Ni_(x)Fe-S phase in the heterostructure is transformed into metal oxides/hydroxides and Ni_(3)S_(2) during OER.Compared with the commercial 20wt%Pt/C||IrO_(2)-Ta_(2)O_(5) electrolyzer,the self-supporting Ni1/5Fe-S/NiFe_(2)O_(4)||Ni1/2Fe-S/NiFe_(2)O_(4) electrolyzer exhibits better stability and lower cell voltage in the fluctu-ating current density range of 10-500 mA/cm^(2).Particularly,the cell voltage of Ni1/5Fe-S/NiFe_(2)O_(4)||Ni1/2Fe-S/NiFe_(2)O_(4) is only approximately 3.91 V at an industrial current density of 500 mA/cm^(2),which is lower than that of the 20wt%Pt/C||IrO_(2)-Ta_(2)O_(5) electrolyzer(i.e.,approximately 4.79 V).This work provides a promising strategy to develop excellent bifunctional electrocatalysts for fluctuating overall water splitting.
基金Youth Innovation Promotion Association of the Chinese Academy of Sciences,Grant/Award Number:2021174National Natural Science Foundation of China,Grant/Award Number:51902326Natural Science Foundation of Shanxi Province,Grant/Award Numbers:201901D211588,20210302124421。
文摘Transition-metal phosphides(TMPs)with high catalytic activity are widely used in the design of electrodes for water splitting.However,a major challenge is how to achieve the trade-off between activity and stability of TMPs.Herein,a novel method for synthesizing CoP nanoparticles encapsu-lated in a rich-defect carbon shell(CoP/DCS)is developed through the self-assembly of modified polycyclic aromatic molecules.The graft and removal of high-activity C-N bonds of aromatic molecules render the controllable design of crystallite defects of carbon shell.The density functional theory calculation indicates that the carbon defects with unpaired electrons could effectively tailor the band structure of CoP.Benefiting from the improved activity and corrosion resistance,the CoP/DCS delivers outstanding difunctional hydrogen evolution reaction(88 mV)and oxygen evolution reaction(251 mV)performances at 10 mA cm^(−2)current density.Furthermore,the coupled water electrolyzer with CoP/DCS as both the cathode and anode presents ultralow cell voltages of 1.49 V to achieve 10 mA cm^(−2)with long-time stability.This strategy to improve TMPs electrocatalyst with rich-DCS and heterogeneous structure will inspire the design of other transition metal compound electrocatalysts for water splitting.
基金This work was financially supported by the National Key Research and Development Program of China(No.2016YFB0700300)the National Natural Science Foundation of China(Nos.51503014 and 51501008)the Fundamental Research Funds for the Central Universities of China(No.230201818-002A3).
文摘Photoelectrochemical(PEC) water splitting offers the capability of harvesting, storing, and converting solar energy into clean and sustainable hydrogen energy. Metal oxides are appealing photoelectrode materials because of their easy manufacturing and relatively high stability. In particular, metal oxides prepared by electrochemical anodization are typical of ordered nanostructures, which are beneficial for light harvesting, charge transfer and transport, and the adsorption and desorption of reactive species due to their high specific surface area and rich channels. However, bare anodic oxides still suffer from low charge separation and sunlight absorption efficiencies. Accordingly, many strategies of modifying anodic oxides have been explored and investigated. In this review, we attempt to summarize the recent advances in the rational design and modifications of these oxides from processes before, during, and after anodization. Rational design strategies are thoroughly addressed for each part with an aim to boost overall PEC performance. The ongoing efforts and challenges for future development of practical PEC electrodes are also presented.
基金financially supported by the National Natural Science Foundation of China(Nos.62001189 and 51802177)the Joint Funds of the National Natural Science Foundation of China(No.U22A20140)+2 种基金the Youth Innovation Group Plan of Shandong Province(No.2022KJ095)the Plan for the Introduction and Cultivation of Young Innovative Talent in the Colleges and Universities of Shandong ProvinceSupported by Guiding Fund of Zaozhuang Industrial Technology Research Institute of University of Jinan。
文摘To effectively address energy challenges,it is crucial to explore efficient and stable bifunctional nonprecious metal catalysts.In this study,a Mo-doped nickeliron layered double hydroxide with flower-cluster architecture was successfully prepared by a one-step hydrothermal method,which demonstrated a good water splitting performance.After an appropriate amount of Mo doping,some lattice distortions in the material provided reactive sites for the adsorption and conversion of intermediates,thus optimising the charge distribution of the material.Moreover,the multidimensional void structures formed after doping had a larger specific surface area and accelerated the penetration of the electrolyte,which significantly improved the activity of the catalyst in alkaline media.At 10 mA·cm^(-2),the hydrogen and oxygen evolution overpotentials of Mo-doped nickel-iron double hydroxides(Mo-NiFe LDH/NF-0.2)were 167 and 220 mV,respectively,with an excellent durability up to 24 h.When the Mo-NiFe LDH/NF-0,2 catalyst was used as the cathode and anode of an electrolytic cell,the catalyst achieved a current density of 10 mA·cm^(-2)at an applied voltage of 1.643 V.This study provides a novel approach for designing excellent bifunctional electrocatalysts containing nonprecious metals.
文摘Photoelectrocatalytic(PEC)seawater splitting as a green and sustainable route to harvest hydrogen is attractive yet hampered by low activity of photoanodes and unexpected high selectivity to the corrosive and toxic chlorine.Especially,it is full of challenges to unveil the key factors influencing the selectivity of such complex PEC processes.Herein,by regulating the energy band and surface structure of the anatase TiO_(2) nanotube array photoanode via nitrogen-doping,the seawater PEC oxidation shifts from Cl^(-)oxidation reaction(ClOR)dominant on the TiO_(2) photoanode(61.6%)to oxygen evolution reaction(OER)dominant on the N-TiO_(2) photoanode(62.9%).Comprehensive investigations including operando photoelectrochemical FTIR and DFT calculations unveil that the asymmetric hydrogen-bonding water at the N-TiO_(2) electrode/electrolyte interface enriches under illumination,facilitating proton transfer and moderate adsorption strength of oxygen-intermediates,which lowers the energy barrier for the OER yet elevates the energy barrier for the ClOR,resulting to a promoted selectivity towards the OER.The work sheds light on the underlying mechanism of the PEC water oxidation processes,and highlights the crucial role of interfacial water on the PEC selectivity,which could be regulated by controlling the energy band and the surface structure of semiconductors.
基金supported by the National Natural Science Foundations of China(No.11972267 and 11802214)the Fundamental Research Funds for the Central Universities(No.104972024JYS0022)the Open Fund of the Hubei Longzhong Laboratory(No.2024KF-30).
文摘This study investigates the dynamic compressive behavior of three periodic lattice structures fabricated from Ti-6Al-4V titanium alloy,each with distinct topologies:simple cubic(SC),body-centered cubic(BCC),and face-centered cubic(FCC).Dynamic compression experiments were conducted using a Split Hopkinson Pressure Bar(SHPB)system,complemented by high-speed imaging to capture real-time deformation and failure mechanisms under impact loading.The influence of cell topology,relative density,and strain rate on dynamic mechanical properties,failure behavior,and stress wave propagation was systematically examined.Finite element modeling was performed,and the simulated results showed good agreement with experimental data.The findings reveal that the dynamic mechanical properties of the lattice structures are generally insensitive to strain rate variations,while failure behavior is predominantly governed by structural configuration.The SC structure exhibited strut buckling and instability-induced fracture,whereas the BCC and FCC structures displayed layer-by-layer crushing with lower strain rate sensitivity.Regarding stress wave propagation,all structures demonstrated significant attenuation capabilities,with the BCC structure achieving the greatest reduction in transmitted wave amplitude and energy.Across all configurations,wave reflection was identified as the primary energy dissipation mechanism.These results provide critical insights into the design of lattice structures for impact mitigation and energy absorption applications.
基金supported by the National Natural Science Foundation of China(Grant Nos.11076009 and 11374062)the Chinese Association of Atomic and Molecular Data+1 种基金the Chinese National Fusion Project for ITER(Grant No.2015GB117000)the Leading Academic Discipline Project of Shanghai City,China(Grant No.B107)
文摘A comprehensive theoretical study of correlation effects on the fine-structure splitting within the ground configuration 3d9 of the Co-like HI45＋, Ta46＋, W47＋, and Au52＋ ions is performed by employing the multi-configuration Dirac-Hartree- Fock method in the active space approximation. It shows that the core-valence correlation with the inner-core 2p electron is more significant than with the outer 3p and 3s electrons, and the correlation with the 2s electron is also noticeable. The core-core correlation seems to be small and can be ignored. The calculated 2D3/2,5/2 splitting energies agree with the recent electron-beam ion-trap measurements [Phys. Rev. A 83 032517 （2011）, Eur. Phys. J. D 66 286 （2012）] to within the experimental uncertainties.
基金supported by the National Natural Science Foundation of China(Grant Nos.11274235 and 11104190)the Doctoral Education Fund of Education Ministry of China(Grant No.20110181120112)
文摘The inter-relation between zero-field splitting （ZFS） parameters and local lattice structures of the （CrSe4）6 clusters in ZnSe semiconductors has been established by using the complete diagonalization （of the energy matrix） method. On the basis of this, the local lattice distortions, the ZFS parameters D, a, F and the optical spectrum for Cr2＋ ions doped into ZnSe are theoretically investigated, and the contributions of the spin singlets have been taken into account. The calculated ZFS parameters are in good agreement with the experimental values. From our calculations, the tetragonal distortion parameters AR = 0.091A and Aθ = 4.28° of Cr2＋ in ZnSe are acquired, and the results suggest that there exists a tetragonal expansion distortion for the local lattice structure of （CrSe4）6- clusters in ZnSe crystals. The influence of the spin singlets on ZFS parameters is also discussed, indicating that the contributions to ZFS parameters a and F cannot be ignored.
基金The National Natural Science Foundation of China (No.50738001,51078086)
文摘In order to find the main factors that influence the urban traffic structure,a relational model between the travelers＇ characteristics and the trip mode choice is built.The data of urban residents＇ characteristics are obtained from statistical data,while the trip mode split data is collected through a trip survey in Bengbu.In addition,the discrete choice model is adopted to build the functional relationship between the mode choice and the travelers＇ personal characteristics,as well as family characteristics and trip characteristics.The model shows that the relationship between the mode split and the personal,as well as family and trip characteristics is stable and changes little as the time changes.Deduced by the discrete model,the mode split result is relatively accurate and can be feasibly used for trip mode structure forecasts.Furthermore,the proposed model can also contribute to find the key influencing factors on trip mode choice,and restructure or optimize the urban trip mode structure.
文摘The high order compact d if ference method is developed for solving the perturbation equations based on Navi er Stokes equations, and is used in studying complex evolution processes from w all negative pulse to the turbulent coherent structure in the channel flow. Th is method contains three dimensional coupling difference scheme with high accur acy and high resolution, and the high order time splitting methods. Compared with the general spectral method, the method can be used to research turbule nt coherent structure under more general boundary conditions and in flow domains . In this paper, the generation and evolution of the turbulent coherent structur es ind uced by wall pulse in the channel flow are simulated, and the basic characterist ics and rules of the turbulent coherent structure are shown. Computational r esults indicate that a wall negative pulse is more convenient than the resonant three wave model.
基金supported by the Program for Innovative Research Team in University of Henan Province(21IRTSTHN009)the Science and Technology Development Plan of Henan Province(212300410029,202300410087,202102210251)+2 种基金the Central Government of Shenzhen Guided the Local Science and Technology Exhibition Special Funds(2021Szvup031)the National Natural Science Foundation of China(52102166)the China Postdoctoral Science Foundation(2019M663058,2021M701065,2019M652749,2021M701071)。
文摘The green hydrogen generation powered by renewable electricity promises the potential decarbonization of the hard-to-abate sector and is essential for the fulfillment of the Paris Agreement that attempts to limit the global average temperature rise in the range of 1.5–2.0 ℃ above the pre-industrial level by the end of this century. Tremendous efforts have been devoted to the optimization of the electrocatalytic performance of the catalysts under industrial-relevant current densities via rational structure design,which induces a preferential electron distribution that favors the adsorption/desorption behavior of the key intermediates, thus accelerating the reaction kinetics. In this review, a brief introduction of the current energy status will be first presented to necessitate the importance of green hydrogen.Followed by the basic concepts and fundamental understanding of the reaction mechanisms, we present efficient strategies for the enhancement of the electrocatalytic performance of the catalysts to meet the rigorous requirement under industrial conditions and the in-depth understanding behind the reinforcement will be briefly discussed next. Then the recent advances regarding the rational design of electrocatalysts operating at an industrial scale will be summarized. Finally, the challenges and perspectives in this thriving field will be proposed from our point of view.
文摘In the present study,split tensile strength of self-compacting concrete with different amount of CuO nanoparticles has been investigated.CuO nanoparticles with the average particle size of 15 nm were added partially to self compacting concrete and split tensile strength of the specimens has been measured.The results indicate that CuO nanoparticles are able to improve the split tensile strength of self compacting concrete and recover the negative effects of polycarboxylate superplasticizer on split tensile strength.CuO nanoparticle as a partial replacement of cement up to 4 wt% could accelerate C-S-H gel formation as a result of increased crystalline Ca（OH）2 amount at the early ages of hydration.The increase of the CuO nanoparticles more than 4 wt% causes the decrease of the split tensile strength because of unsuitable dispersion of nanoparticles in the concrete matrix.Accelerated peak appearance in conduction calorimetry tests,more weight loss in thermogravimetric analysis and more rapid appearance of related peaks to hydrated products in X-ray diffraction（XRD） results all also indicate that CuO nanoparticles up to4 wt% could improve the mechanical and physical properties of the specimens.Finally,CuO nanoparticles could improve the pore structure of concrete and shift the distributed pores to harmless and few-harm pores.
文摘Complexes Cl-RuⅡ（dppe）2（Fe Cl4）·2CH2Cl2（2） and Br-RuII（dppe）2（Fe Br4）·2CH2Cl2（3） were prepared by the reaction of trans-RuII（dppe）2Cl2（1） with FeX 3（X = Cl, Br）. More interestingly, the central Ru atoms of RuII（dppe）-based complexes（2 and 3） define a tetragonal pyramid with five-coordination. The temperature dependence magnetic susceptibilities indicate that the xMT values of complexes 2 and 3 are almost constant at 50~300 K, and the xMT values sharply decrease with further decreasing the temperature at low temperature due to the zero-field splitting（ZFS） of high spin Fe（III） ions.
文摘The dynamic characteristics of the large scale coherent structures in a forced free shear layer are experi- mentally studied by means of flow visualization. The quantitative measurements are acquired by the use of a LDV. It is shown that the development of the coherent structures can be greatly influenced by upstream artificial perturbations and as a result the mixing in the layer can be controlled. Like vortex merging, vortex splitting is also a common evolu- tion pattern in the development of the coherent structures.
基金financial support from the National Natural Science Foundation of China (Grant Nos. 51972191, 51722207)。
文摘Developing bifunctional electrocatalysts with both high catalytic activity and high stability is crucial for efficient water splitting in alkaline media.Herein,a Fe-incorporated dual-metal selenide on nickel foam(Co_(0.9)Fe_(0.1)-Se/NF) is synthesized via a facile one-step electrodeposition method.As-synthesized materials could serve as self-supported bifunctional electrocatalysts with excellent catalytic activity towards oxygen evolution reaction(OER) and hydrogen evolution reaction(HER) in alkaline media.Experimental results show that delivering a 10 mA cm^(-2) water splitting current density only requires a cell voltage of 1.55 V.In addition,a very stable performance could be kept for about 36 hours,indicating their excellent working stability.Moreover,by means of phase analysis,we have identified that the evolution of the synthesized Co_(0.9)Fe_(0.1)-Se/NF experiences two entirely different processes in HER and OER,which hydroxide and oxyhydroxide are regarded as the real active sites,respectively.This work may pave the way to further understanding the relationships between the reactivity and stability of chalcogenide-based electrocatalysts and facilitating the rational design of efficient electrocatalysts for future renewable energy system applications.
文摘In this paper,a unit cell of a single-negative metamaterial structure loaded with a meander line and defected ground structure(DGS)is investigated as the principle radiating element of an antenna.The unit cell antenna causes even or odd mode resonances similar to the unit cell structure depending on the orientation of the microstrip feed used to excite the unit cell.However,the orientation which gives low-frequency resonance is considered here.The unit cell antenna is then loaded with a meander line which is parallel to the split bearing side and connects the other two sides orthogonal to the split bearing side.This modified structure excites another mode of resonance at high frequency when a meander line defect is loaded on the metallic ground plane.Specific parameters of the meander line structure,the DGS shape,and the unit cell are optimized to place these two resonances at different frequencies with proper frequency intervals to enhance the bandwidth.Finally,the feed is placed in an offset position for better impedance matching without affecting the bandwidth The compact dimension of the antenna is 0.25λL×0.23λL×0.02λL,whereλL is the free space wavelength with respect to the center frequency of the impedance bandwidth.The proposed antenna is fabricated and measured.Experimental results reveal that the modified design gives monopole like radiation patterns which achieves a fractional operating bandwidth of 26.6%,from 3.26 to 4.26 GHz for|S11|<−10 dB and a pick gain of 1.26 dBi is realized.In addition,the simulated and measured crosspolarization levels are both less than−15 dB in the horizontal plane.
