The design of cost-effective and efficient metal-free carbon-based catalysts for the hydrogen evolution reaction(HER)is of great significance for increasing the production of clean hydrogen by the electrolysis of alka...The design of cost-effective and efficient metal-free carbon-based catalysts for the hydrogen evolution reaction(HER)is of great significance for increasing the production of clean hydrogen by the electrolysis of alkaline water.Precise control of the electronic structure by heteroatom doping has proven to be efficient for increasing catalytic activity.Nevertheless,both the structural characteristics and the underlying mechanism are not well understood,especially for doping with two different atoms,thus limiting the use of these catalysts.We report the production of phosphorus and nitrogen co-doped hollow carbon nanospheres(HCNs)by the copolymerization of pyrrole and aniline at a Triton X-100 micelle-interface,followed by doping with phytic acid and carbonization.The unique pore structure and defect-rich framework of the HCNs expose numerous active sites.Crucially,the combined effect of graphitic nitrogen and phosphorus-carbon bonds modulate the local electronic structure of adjacent C atoms and facilitates electron transfer.As a res-ult,the HCN carbonized at 1100°C exhibited superior HER activity and an outstanding stability(70 h at a current density of 10 mA cm^(−2))in alkaline water,because of the large number of graphitic nitrogen and phosphorus-carbon bonds.展开更多
Solid oxide electrolysis cells(SOECs)can effectively convert CO_(2)into high value-added CO fuel.In this paper,Sc-doped Sr_(2)Fe_(1.5)Mo_(0.3)Sc_(0.2)O_(6−δ)(SFMSc)perovskite oxide material is synthesized via solid-p...Solid oxide electrolysis cells(SOECs)can effectively convert CO_(2)into high value-added CO fuel.In this paper,Sc-doped Sr_(2)Fe_(1.5)Mo_(0.3)Sc_(0.2)O_(6−δ)(SFMSc)perovskite oxide material is synthesized via solid-phase method as the cathode for CO_(2)electrolysis by SOECs.XRD confirms that SFMSc exhibits a stable cubic phase crystal structure.The experimental results of TPD,TG,EPR,CO_(2)-TPD further demonstrate that Sc-doping increases the concentration of oxygen vacancy in the material and the chemical adsorption capacity of CO_(2)molecules.Electrochemical tests reveal that SFMSc single cell achieves a current density of 2.26 A/cm^(2) and a lower polarization impedance of 0.32Ω·cm^(2) at 800°C under the applied voltage of 1.8 V.And no significant performance attenuation or carbon deposition is observed after 80 h continuous long-term stability test.This study provides a favorable support for the development of SOEC cathode materials with good electro-catalytic performance and stability.展开更多
Nitrogen doping in chemical vapor deposition-derived ultrananocrystalline diamond(UNCD)films in-creases the electronic conductivity,yet its microstructural effects on electron transport are insufficiently understood.W...Nitrogen doping in chemical vapor deposition-derived ultrananocrystalline diamond(UNCD)films in-creases the electronic conductivity,yet its microstructural effects on electron transport are insufficiently understood.We investigated the formation of nitrogen-induced diaph-ite structures(hybrid diamond-graphite phases)and their role in changing the conductivity.Nitrogen doping in a hy-drogen-rich plasma environment promotes the emergence of unique sp^(3)-sp^(2)bonding interfaces,where diamond grains are covalently integrated with graphitic domains,facilitating a structure-driven electronic transition.High-resolution transmis-sion electron microscopy and selected area electron diffraction reveal five-fold,six-fold and twelve-fold symmetries,along with an atypical{200}crystallographic reflection,confirming diaphite formation in 5%and 10%N-doped UNCD films,while high-er doping levels(15%and 20%)result in extensive graphitization.Raman spectroscopy tracks the evolution of sp^(2)bonding with increasing nitrogen content,while atomic force microscopy and X-ray diffraction indicate a consistent diamond grain size of~8 nm.Cryogenic electronic transport measurements reveal a conductivity increase from 8.72 to 708 S/cm as the nitrogen dop-ing level increases from 5%to 20%,which is attributed to defect-mediated carrier transport and 3D weak localization.The res-ulting conductivity is three orders of magnitude higher than previously reported.These findings establish a direct correlation between diaphite structural polymorphism and tunable electronic properties in nitrogen-doped UNCD films,offering new ways for defect-engineering diamond-based electronic materials.展开更多
We used the natural product chamomile as a carbon source to synthesize praseodymium(Pr) and nitrogen(N) co-doped biomass carbon dots(Pr/N-BCDs) with remarkable luminescence properties by one-step hydrothermal method.C...We used the natural product chamomile as a carbon source to synthesize praseodymium(Pr) and nitrogen(N) co-doped biomass carbon dots(Pr/N-BCDs) with remarkable luminescence properties by one-step hydrothermal method.Compared with single N-doped BCDs(N-BCDs) and Pr-doped BCDs(Pr-BCDs),Pr/N-BCDs not only showed better fluorescence properties and stability but also achieved a significant increase in quantum yield of 12%.More importantly,under certain conditions,Pr/N-BCDs and 2,4-dinitrophenylhydrazide(2,4-DNPH) had significant fluorescence internal filtration effect(IFE) and dynamic quenching effect,and in the concentration range of0.50-20 μmol·L^(-1),the concentration of 2,4-DNPH had a good linear relationship with the fluorescence quenching signal,and the detection limit was as low as 2.1 nmol·L^(-1).展开更多
The accepted doping ion in Ti^(4+)-site of PbZr_(y)Ti_(1–y)O_(3)(PZT)-based piezoelectric ceramics is a well-known method to increase mechanical quality factor(Q_(m)),since the acceptor coupled by oxygen vacancy beco...The accepted doping ion in Ti^(4+)-site of PbZr_(y)Ti_(1–y)O_(3)(PZT)-based piezoelectric ceramics is a well-known method to increase mechanical quality factor(Q_(m)),since the acceptor coupled by oxygen vacancy becomes defect dipole,which prevents the domain rotation.In this field,a serious problem is that generally,Qm decreases as the temperature(T)increases,since the oxygen vacancies are decoupled from the defect dipoles.In this work,Q_(m) of Pb_(0.95)Sr_(0.05)(Zr_(0.53)Ti_(0.47))O_(3)(PSZT)ceramics doped by 0.40%Fe_(2)O_(3)(in mole)abnormally increases as T increases,of which the Qm and piezoelectric coefficient(d_(33))at room temperature and Curie temperature(TC)are 507,292 pC/N,and 345℃,respectively.The maximum Qm of 824 was achieved in the range of 120–160℃,which is 62.52%higher than that at room temperature,while the dynamic piezoelectric constant(d_(31))was just slightly decreased by 3.85%.X-ray diffraction(XRD)and piezoresponse force microscopy results show that the interplanar spacing and the fine domains form as temperature increases,and the thermally stimulated depolarization current shows that the defect dipoles are stable even the temperature up to 240℃.It can be deduced that the aggregation of oxygen vacancies near the fine domains and defect dipole can be stable up to 240℃,which pins domain rotation,resulting in the enhanced Q_(m) with the increasing temperature.These results give a potential path to design high Q_(m) at high temperature.展开更多
In a high heat flux ablative environment,the surface temperature of aircraft rises rapidly,leading to traditional high thermal conductivity materials being ineffective at protecting internal metal components.In this s...In a high heat flux ablative environment,the surface temperature of aircraft rises rapidly,leading to traditional high thermal conductivity materials being ineffective at protecting internal metal components.In this study,continuous carbon fiber reinforced Li_(2)O-Al_(2)O_(3)-SiO_(2)(C_(f)/LAS)glass ceramic composites doped with SiC particles(SiC_(p))were prepared by slurry immersion winding and hot pressing sintering.Effect of matrix crystallinity on ablative properties of the composites under ultra-high heat flux was investigated.By utilizing heat absorption and low thermal conductivity characteristics associated with SiO_(2)gasification within composite materials,both surface and internal temperatures of these materials are effectively reduced,thereby ensuring the safe operation of aircraft and electronic devices.Results indicate that the average linear ablation rate of composites doped with 10%(in mass)of SiC_(p)significantly decreases at a heat flux of 20 MW/m^(2).Transmission electron microscope observation reveals that the doped glass matrix exhibits increased crystallinity,reduced internal stress,and minimized lattice distortion,thereby enhancing the composites’high-temperature performance.However,excessive SiC_(p)doping leads to reduced crystallinity and deteriorated ablation performance.Ultimately,the average linear ablation rate of C_(f)/LAS composites with 10%(in mass)SiC_(p)at 20 MW/m^(2)heat flux is comparable to that of commercial carbon/carbon composites,accompanied by providing lower thermal conductivity and higher bending strength.This novel high-performance C_(f)/LAS composite is cost-effective,short-cycled,and suitable for mass production,offering promising potential for widespread application in ablation-resistant components of hypersonic vehicles.展开更多
Al-doped manganese dioxide(MnO_(2))was synthesized by simple hydrothermal method,and a controllable phase transition of the MnO_(2)crystal phase fromβtoδwas achieved.The effects of Al doping concentration on the str...Al-doped manganese dioxide(MnO_(2))was synthesized by simple hydrothermal method,and a controllable phase transition of the MnO_(2)crystal phase fromβtoδwas achieved.The effects of Al doping concentration on the structure and electrochemical properties of electrode materials were studied in detail.The results show that the controlled synthesis requires a synergy between KMnO_(4),MnCl_(2)and AlCl_(3),and that Al^(3+)plays an important role.Compared with the pure phase MnO_(2),the crystallinity of Al-doped MnO_(2)decreases and the specific surface area increases,which provides more active sites for the electrode material.When 3 mmol Al^(3+)is added,the prepared MnO_(2)-3 has the largest specific capacitance and the highest rate performance.The energy density of the asymmetric supercapacitor(ASC)with MnO_(2)-3 as the positive electrode and activated carbon(AC)as the negative electrode can reach 18.4 W·h/kg at the power density of 400 W/kg,and the capacity can maintain 90%of the initial value after 20000 cycles,indicating that Al-doped MnO_(2)has certain practical application value.This study provides favorable guidance for MnO_(2)as a high performance electrode material.展开更多
Nitrogen doping has significant effects on the photocatalytic performance of ceria(CeO_(2)),and the possible synergistic effect with the inevitably introduced abundant oxygen vacancies(OVs)is of great significance for...Nitrogen doping has significant effects on the photocatalytic performance of ceria(CeO_(2)),and the possible synergistic effect with the inevitably introduced abundant oxygen vacancies(OVs)is of great significance for further investigation,and the specifically exposed crystal faces of CeO_(2)may have an impact on the performance of nitrogen doped CeO_(2).Herein,nitrogen-doped CeO_(2)with different morphologies and exposed crystal faces was prepared,and its performances in the photocatalytic degradation of tetracycline(TC)or hydrogen production via water splitting were evaluated.Density functional theory(DFT)was used to simulate the band structures,density of states,and oxygen defect properties of different CeO_(2)structures.It was found that nitrogen doping and OVs synergistically promoted the catalytic activity of nitrogen-doped CeO_(2).In addition,the exposed crystal faces of CeO_(2)have significant effects on the introduction of nitrogen and the ease of OV generation,as well as the synergistic effect of nitrogen doping with OVs.Among them,the rod-like nitrogen-doped CeO_(2)with exposed(110)face(R-CeO_(2)-NH_(3))showed a photocatalytic degradation ratio of 73.59%for TC and hydrogen production of 156.89μmol/g,outperforming other prepared photocatalysts.展开更多
Aiming at wind turbines,the opportunistic maintenance optimization is carried out for multi-component system,where minimal repair,imperfect repair,replacement as well as their effects on component’s effective age are...Aiming at wind turbines,the opportunistic maintenance optimization is carried out for multi-component system,where minimal repair,imperfect repair,replacement as well as their effects on component’s effective age are considered.At each inspection point,appropriate maintenance mode is selected according to the component’s effective age and its maintenance threshold.To utilize the maintenance opportunities for the components among the wind turbines,opportunistic maintenance approach is adopted.Meanwhile,the influence of seasonal factor on the component’s failure rate and improvement factor’s decrease with the increase of repair’s times are also taken into account.The maintenance threshold is set as the decision variable,and an opportunistic maintenance optimization model is proposed to minimize wind turbine’s life-cycle maintenance cost.Moreover,genetic algorithm is adopted to solve the model,and the effectiveness is verified with a case study.The results show that based on the component’s inherent reliability and maintainability,the proposed model can provide optimal maintenance plans accordingly.Furthermore,the higher the component’s reliability and maintainability are,the less the times of repair and replacement will be.展开更多
To improve the mainlainability design efficiency and quality, a layout optimization method for maintainability of multi-component systems was proposed. The impact of the component layout design on system maintainabili...To improve the mainlainability design efficiency and quality, a layout optimization method for maintainability of multi-component systems was proposed. The impact of the component layout design on system maintainability was analyzed, and the layout problem for maintainability was presented. It was formulated as an optimization problem, where maintainability, layout space and distance requirement were formulated as objective functions. A multi-objective particle swarm optimization algorithm, in which the constrained-domination relationship and the update strategy of the global best were simply modified, was then used to obtain Pareto optimal solutions for the maintainability layout design problem. Finally, application in oxygen generation system of a spacecraft was studied in detail to illustrate the effectiveness and usefulness of the proposed method. The results show that the concurrent maintainability design can be carried out during the layout design process by solving the layout optimization problem for maintainability.展开更多
Although opportunistic maintenance strategies are widely used for multi-component systems, all opportunistic mainte- nance strategies only consider economic dependence and do not take structural dependence into accoun...Although opportunistic maintenance strategies are widely used for multi-component systems, all opportunistic mainte- nance strategies only consider economic dependence and do not take structural dependence into account. An opportunistic main- tenance strategy is presented for a multi-component system that considers both structural dependence and economic dependence. The cost relation and time relation among components based on structural dependence are developed. The maintenance strategy for each component of a multi-component system involves one of five maintenance actions, namely, no-maintenance, a minimal maintenance action, an imperfect maintenance action, a perfect maintenance action, and a replacement action. The maintenance action is determined by the virtual age of the component, the life expectancy of the component, and the age threshold values. Monte Carlo simulation is designed to obtain the optimal oppor- tunistic maintenance strategy of the system over its lifetime. The simulation result reveals that the minimum maintenance cost with a strategy that considers structural dependence is less than that with a strategy that does not consider structural dependence. The availability with a strategy that considers structural dependence is greater than that with a strategy that does not consider structural dependence under the same conditions.展开更多
For unacceptable computational efficiency and accuracy on the probabilistic analysis of multi-component system with multi-failure modes,this paper proposed multi-extremum response surface method(MERSM).MERSM model was...For unacceptable computational efficiency and accuracy on the probabilistic analysis of multi-component system with multi-failure modes,this paper proposed multi-extremum response surface method(MERSM).MERSM model was established based on quadratic polynomial function by taking extremum response surface model as the sub-model of multi-response surface method.The dynamic probabilistic analysis of an aeroengine turbine blisk with two components,and their reliability of deformation and stress failures was obtained,based on thermal-structural coupling technique,by considering the nonlinearity of material parameters and the transients of gas flow,gas temperature and rotational speed.The results show that the comprehensive reliability of structure is 0.9904 when the allowable deformations and stresses of blade and disk are 4.78×10–3 m and 1.41×109 Pa,and 1.64×10–3 m and 1.04×109 Pa,respectively.Besides,gas temperature and rotating speed severely influence the comprehensive reliability of system.Through the comparison of methods,it is shown that the MERSM holds higher computational precision and speed in the probabilistic analysis of turbine blisk,and MERSM computational precision satisfies the requirement of engineering design.The efforts of this study address the difficulties on transients and multiple models coupling for the dynamic probabilistic analysis of multi-component system with multi-failure modes.展开更多
In this paper,the combined addition of copper or iron and sulphate ions onto TiO_(2) prepared by a simple sol-gel method is studied for formic acid photocatalytic conversion.A wide structural and morphological charact...In this paper,the combined addition of copper or iron and sulphate ions onto TiO_(2) prepared by a simple sol-gel method is studied for formic acid photocatalytic conversion.A wide structural and morphological characterization of the different photocatalysts was performed by X-ray diffraction(XRD),N_(2)-physisorption for BET surface area measurements,scanning and transmission electronic microscopies(SEM and TEM),UV-Vis diffuse spectroscopy(DRS)and X-ray photoelectron spectroscopy(XPS),in order to correlate the physico-chemical properties of the materials to their photocatalytic efficiencies for formic acid oxidation.Results have shown important differences among the catalysts depending on the metal added.Sulphated TiO_(2)/Cu(1%Cu)was the best photocatalyst obtaining about 100% formic acid conversion in only 5 min.The appropriate physico-chemical features of this photocatalyst,given by the addition of combined copper and sulphate ions,explain its excellence in photocatalytic reaction.展开更多
In order to investigate whether endohedral He-doping is possible or not in CL-20,a density functional treatment has been carried out at the levels of B3LYP/6-31++G(d,p)and B3PW91/6-31++G(d,p).Some physicochemical and ...In order to investigate whether endohedral He-doping is possible or not in CL-20,a density functional treatment has been carried out at the levels of B3LYP/6-31++G(d,p)and B3PW91/6-31++G(d,p).Some physicochemical and quantum chemical properties of the helium-doped CL-20 (He@CL-20)are compared with the respective values of the parent explosive CL-20.The helium doping caused swelling of CL-20cage but no bond rupture occurred.Doped helium acquired some positive charge.展开更多
The effects of CaO content in the range from 0 to 4.0%, and sintering temperature on the phase composition, relative density and electrical conductivity of 10NiO-NiFe2O4 composites doped with CaO were studied. The res...The effects of CaO content in the range from 0 to 4.0%, and sintering temperature on the phase composition, relative density and electrical conductivity of 10NiO-NiFe2O4 composites doped with CaO were studied. The results show that there is no change of structure for NiO or NiFe2O4; there is apparent oxygen absorbing and releasing behavior during the heating process in air for 10NiO-NiFe2O4 composites. Introduction of CaO can accelerate the densification of 10NiO-NiFe2O4 composites. The maximum value of relative density is 98.75% for composite doped with 2.0% CaO and sintered at 1 200 ℃, which is beyond about 20% for the undoped composites. The sintering activated energy of sample containing 2% CaO decreases by 15.87 kJ/mol, compared with that of the undoped sample.展开更多
Nitrogen doping has been widely used to improve the performance of carbon electrodes in supercapacitors,particularly in terms of their high-frequency response.However,the charge storage and electrolyte ion response me...Nitrogen doping has been widely used to improve the performance of carbon electrodes in supercapacitors,particularly in terms of their high-frequency response.However,the charge storage and electrolyte ion response mechanisms of different nitrogen dopants at high frequencies are still unclear.In this study,melamine foam carbons with different configurations of surfacedoped N were formed by gradient carbonization,and the effects of the configurations on the high-frequency response behavior of the supercapacitors were analyzed.Using a combination of experiments and first-principle calculations,we found that pyrrolic N,characterized by a higher adsorption energy,increases the charge storage capacity of the electrode at high frequencies.On the other hand,graphitic N,with a lower adsorption energy,increases the speed of ion response.We propose the use of adsorption energy as a practical descriptor for electrode/electrolyte design in high-frequency applications,offering a more universal approach for improving the performance of N-doped carbon materials in supercapacitors.展开更多
Polyaniline（PANI） nanofiber was synthesized by interfacial polymerization utilizing the interface between HC1 and CCl4. The hybrid type supercapacitors （PLi/C） based on Li-doping polyaniline and activated carbon e...Polyaniline（PANI） nanofiber was synthesized by interfacial polymerization utilizing the interface between HC1 and CCl4. The hybrid type supercapacitors （PLi/C） based on Li-doping polyaniline and activated carbon electrode were fabricated and compared with the redox type capacitors （PLi/PLi） based on two uniformly Li-doping polyaniline electrodes. The electrochemical performances of the two types of supercapacitors were characterized in non-aqueous electrolyte. PLi/C supercapacitors have a wider effective energy storage potential range and a higher upper potential. At the same time, the PLi/C supercapacitor exhibits a specific capacity of 120.93 F/g at initial discharge and retains 80% after 500 cycles. The ohmic internal resistance （REs） of PLi/C supercapacitor is 5.0 Ω, which is smaller than that of PLi/PLi capacitor （5.5 Ω）. Moreover, it can be seen that EtgNBF4 organic solution is more suitable for using as organic electrolyte of PLi/C capacitor compared with organic solution containing LiPFr.展开更多
Shuttle effect,poor conductivity and large volume expansion are the main factors that hinder the practical application of sulfur cathodes.Currently,rational structure designing of carbon-based sulfur hosts is the most...Shuttle effect,poor conductivity and large volume expansion are the main factors that hinder the practical application of sulfur cathodes.Currently,rational structure designing of carbon-based sulfur hosts is the most effective strategy to address the above issues.However,the preparation process of carbon-based sulfur hosts is usually complex and costly.Therefore,it is necessary to develop an efficient and cost-effective method to fabricate carbon hosts for high-performance sulfur cathodes.Herein,we reported the fabrication of a bio-derived nitrogen doped porous carbon materials(BNPC)via a molten-salt method for high performance sulfur cathodes.The long-range-ordered honeycomb structure of BNPC is favorable for the trapping of polysulfide(PS)species and accommodates the volumetric variation of sulfur during cycling,while the high graphitization degree of BNPC favors the redox kinetics of sulfur cathodes.Moreover,the nitrogen doping content not only enhances the electrical conductivity of BNPC,but also provides ample anchoring sites for the immobilization of PS,which plays a key role in suppressing the shuttle effect.As a result,the S@BNPC cathode exhibits a high initial specific capacity of 1189.4 mA·h/g at 0.2C.After 300 cycles,S@BNPC still maintains a capacity of 703.2 mA·h/g which corresponds to a fading rate of 0.13%per cycle after the second cycle.This work offers vast opportunities for the large-scale application of high performance carbon-based sulfur hosts.展开更多
Martensitic transformation behavior was studied for zirconia containing 4%～10% CeO2 (in mole fraction) by using a dilatometric method. The Ms (Martensite start temperature) decreased near linearly with increasing CeO...Martensitic transformation behavior was studied for zirconia containing 4%～10% CeO2 (in mole fraction) by using a dilatometric method. The Ms (Martensite start temperature) decreased near linearly with increasing CeO2. Different transformation modes were observed depending on the composition and cooling rate. ZrO2 containing 6% CeO2 showed isothermal transformation behavior, whereas ZrO2 containing 9% and 10% CeO2 showed athermal transformation behavior. However, ZrO2 containing 8% CeO2 showed either isothermal or athermal transformations behavior depending on the cooling rate. A TTT (Time-Temperature-Transformation) diagram was proposed for ZrO2 containing 8% CeO2.展开更多
Fig.1 3D X-ray tomography reconstruction and element distribution in Ti,Mg and Al co-doped LiCoO2.3D spatial distributions of (a) Al,(b) Co and (c) Ti probed by fluorescence-yield scanning transmission X-ray microscop...Fig.1 3D X-ray tomography reconstruction and element distribution in Ti,Mg and Al co-doped LiCoO2.3D spatial distributions of (a) Al,(b) Co and (c) Ti probed by fluorescence-yield scanning transmission X-ray microscopy;elemental distributions of (d) Al,(e) Co and (f) Ti over the virtual x-z slice through the center of the particle;(g) identified and visualized subdomain formation Fig.2 (a) Comparison of cycling stabilities of Ti,Mg and Al co-doped LiCoO2 and pristine LiCoO2 half cells,charge-discharge profiles of (b) pristine LiCoO2 and (c) Ti,Mg and Al co-doped LiCoO2 half cells,(d) cycle stabilities of Ti,Mg and Al co-doped LiCoO2 and pristine LiCoO2 full batteries (graphite was used anode) and (e) discharge voltage of the full batteries and energy density of the both materials as a function of cycle number Layered lithium cobalt oxide (LiCoO2) with a theoretical capacity of 274 mAh·g^-1 has become a dominant cathode material for lithium-ion batteries of “3C” market (cellular phones,portable computers,camcorders)[1-2].Nevertheless,the actually attained capacity is merely about 140 mAh·g^-1 with a charge cut-off vol- tage of about 4.2 V (vs Li +/Li)[3].展开更多
基金financially supported by the project of the National Natural Science Foundation of China(52322203)the Key Research and Development Program of Shaanxi Province(2024GHZDXM-21)。
文摘The design of cost-effective and efficient metal-free carbon-based catalysts for the hydrogen evolution reaction(HER)is of great significance for increasing the production of clean hydrogen by the electrolysis of alkaline water.Precise control of the electronic structure by heteroatom doping has proven to be efficient for increasing catalytic activity.Nevertheless,both the structural characteristics and the underlying mechanism are not well understood,especially for doping with two different atoms,thus limiting the use of these catalysts.We report the production of phosphorus and nitrogen co-doped hollow carbon nanospheres(HCNs)by the copolymerization of pyrrole and aniline at a Triton X-100 micelle-interface,followed by doping with phytic acid and carbonization.The unique pore structure and defect-rich framework of the HCNs expose numerous active sites.Crucially,the combined effect of graphitic nitrogen and phosphorus-carbon bonds modulate the local electronic structure of adjacent C atoms and facilitates electron transfer.As a res-ult,the HCN carbonized at 1100°C exhibited superior HER activity and an outstanding stability(70 h at a current density of 10 mA cm^(−2))in alkaline water,because of the large number of graphitic nitrogen and phosphorus-carbon bonds.
基金supported by National Key R&D Program of China(2021YFB4001401)National Natural Science Foundation of China(52272190,22178023).
文摘Solid oxide electrolysis cells(SOECs)can effectively convert CO_(2)into high value-added CO fuel.In this paper,Sc-doped Sr_(2)Fe_(1.5)Mo_(0.3)Sc_(0.2)O_(6−δ)(SFMSc)perovskite oxide material is synthesized via solid-phase method as the cathode for CO_(2)electrolysis by SOECs.XRD confirms that SFMSc exhibits a stable cubic phase crystal structure.The experimental results of TPD,TG,EPR,CO_(2)-TPD further demonstrate that Sc-doping increases the concentration of oxygen vacancy in the material and the chemical adsorption capacity of CO_(2)molecules.Electrochemical tests reveal that SFMSc single cell achieves a current density of 2.26 A/cm^(2) and a lower polarization impedance of 0.32Ω·cm^(2) at 800°C under the applied voltage of 1.8 V.And no significant performance attenuation or carbon deposition is observed after 80 h continuous long-term stability test.This study provides a favorable support for the development of SOEC cathode materials with good electro-catalytic performance and stability.
文摘Nitrogen doping in chemical vapor deposition-derived ultrananocrystalline diamond(UNCD)films in-creases the electronic conductivity,yet its microstructural effects on electron transport are insufficiently understood.We investigated the formation of nitrogen-induced diaph-ite structures(hybrid diamond-graphite phases)and their role in changing the conductivity.Nitrogen doping in a hy-drogen-rich plasma environment promotes the emergence of unique sp^(3)-sp^(2)bonding interfaces,where diamond grains are covalently integrated with graphitic domains,facilitating a structure-driven electronic transition.High-resolution transmis-sion electron microscopy and selected area electron diffraction reveal five-fold,six-fold and twelve-fold symmetries,along with an atypical{200}crystallographic reflection,confirming diaphite formation in 5%and 10%N-doped UNCD films,while high-er doping levels(15%and 20%)result in extensive graphitization.Raman spectroscopy tracks the evolution of sp^(2)bonding with increasing nitrogen content,while atomic force microscopy and X-ray diffraction indicate a consistent diamond grain size of~8 nm.Cryogenic electronic transport measurements reveal a conductivity increase from 8.72 to 708 S/cm as the nitrogen dop-ing level increases from 5%to 20%,which is attributed to defect-mediated carrier transport and 3D weak localization.The res-ulting conductivity is three orders of magnitude higher than previously reported.These findings establish a direct correlation between diaphite structural polymorphism and tunable electronic properties in nitrogen-doped UNCD films,offering new ways for defect-engineering diamond-based electronic materials.
基金supported by the National Natural Science Foundation of China (Grant No.22063010)the Natural Science Foundation of Shaanxi Province (Grant No.2022QFY07-05)Yan'an Science and Technology Plan Project (Grants No.2022SLJBZ-002, 2023-CYL-193)。
文摘We used the natural product chamomile as a carbon source to synthesize praseodymium(Pr) and nitrogen(N) co-doped biomass carbon dots(Pr/N-BCDs) with remarkable luminescence properties by one-step hydrothermal method.Compared with single N-doped BCDs(N-BCDs) and Pr-doped BCDs(Pr-BCDs),Pr/N-BCDs not only showed better fluorescence properties and stability but also achieved a significant increase in quantum yield of 12%.More importantly,under certain conditions,Pr/N-BCDs and 2,4-dinitrophenylhydrazide(2,4-DNPH) had significant fluorescence internal filtration effect(IFE) and dynamic quenching effect,and in the concentration range of0.50-20 μmol·L^(-1),the concentration of 2,4-DNPH had a good linear relationship with the fluorescence quenching signal,and the detection limit was as low as 2.1 nmol·L^(-1).
基金National Natural Science Foundation of China(U2241242)National Key R&D Program of China(2023YFB3812000,2021YFA0716502)。
文摘The accepted doping ion in Ti^(4+)-site of PbZr_(y)Ti_(1–y)O_(3)(PZT)-based piezoelectric ceramics is a well-known method to increase mechanical quality factor(Q_(m)),since the acceptor coupled by oxygen vacancy becomes defect dipole,which prevents the domain rotation.In this field,a serious problem is that generally,Qm decreases as the temperature(T)increases,since the oxygen vacancies are decoupled from the defect dipoles.In this work,Q_(m) of Pb_(0.95)Sr_(0.05)(Zr_(0.53)Ti_(0.47))O_(3)(PSZT)ceramics doped by 0.40%Fe_(2)O_(3)(in mole)abnormally increases as T increases,of which the Qm and piezoelectric coefficient(d_(33))at room temperature and Curie temperature(TC)are 507,292 pC/N,and 345℃,respectively.The maximum Qm of 824 was achieved in the range of 120–160℃,which is 62.52%higher than that at room temperature,while the dynamic piezoelectric constant(d_(31))was just slightly decreased by 3.85%.X-ray diffraction(XRD)and piezoresponse force microscopy results show that the interplanar spacing and the fine domains form as temperature increases,and the thermally stimulated depolarization current shows that the defect dipoles are stable even the temperature up to 240℃.It can be deduced that the aggregation of oxygen vacancies near the fine domains and defect dipole can be stable up to 240℃,which pins domain rotation,resulting in the enhanced Q_(m) with the increasing temperature.These results give a potential path to design high Q_(m) at high temperature.
基金National Natural Science Foundation of China(U23A6014,52103357)。
文摘In a high heat flux ablative environment,the surface temperature of aircraft rises rapidly,leading to traditional high thermal conductivity materials being ineffective at protecting internal metal components.In this study,continuous carbon fiber reinforced Li_(2)O-Al_(2)O_(3)-SiO_(2)(C_(f)/LAS)glass ceramic composites doped with SiC particles(SiC_(p))were prepared by slurry immersion winding and hot pressing sintering.Effect of matrix crystallinity on ablative properties of the composites under ultra-high heat flux was investigated.By utilizing heat absorption and low thermal conductivity characteristics associated with SiO_(2)gasification within composite materials,both surface and internal temperatures of these materials are effectively reduced,thereby ensuring the safe operation of aircraft and electronic devices.Results indicate that the average linear ablation rate of composites doped with 10%(in mass)of SiC_(p)significantly decreases at a heat flux of 20 MW/m^(2).Transmission electron microscope observation reveals that the doped glass matrix exhibits increased crystallinity,reduced internal stress,and minimized lattice distortion,thereby enhancing the composites’high-temperature performance.However,excessive SiC_(p)doping leads to reduced crystallinity and deteriorated ablation performance.Ultimately,the average linear ablation rate of C_(f)/LAS composites with 10%(in mass)SiC_(p)at 20 MW/m^(2)heat flux is comparable to that of commercial carbon/carbon composites,accompanied by providing lower thermal conductivity and higher bending strength.This novel high-performance C_(f)/LAS composite is cost-effective,short-cycled,and suitable for mass production,offering promising potential for widespread application in ablation-resistant components of hypersonic vehicles.
基金Project(202203021221138)supported by the Collaborative Innovation Center for Shanxi Advanced Permanent Materials and Technologythe 1331 Engineering of Shanxi ProvinceFundamental Research Program of Shanxi Province,China。
文摘Al-doped manganese dioxide(MnO_(2))was synthesized by simple hydrothermal method,and a controllable phase transition of the MnO_(2)crystal phase fromβtoδwas achieved.The effects of Al doping concentration on the structure and electrochemical properties of electrode materials were studied in detail.The results show that the controlled synthesis requires a synergy between KMnO_(4),MnCl_(2)and AlCl_(3),and that Al^(3+)plays an important role.Compared with the pure phase MnO_(2),the crystallinity of Al-doped MnO_(2)decreases and the specific surface area increases,which provides more active sites for the electrode material.When 3 mmol Al^(3+)is added,the prepared MnO_(2)-3 has the largest specific capacitance and the highest rate performance.The energy density of the asymmetric supercapacitor(ASC)with MnO_(2)-3 as the positive electrode and activated carbon(AC)as the negative electrode can reach 18.4 W·h/kg at the power density of 400 W/kg,and the capacity can maintain 90%of the initial value after 20000 cycles,indicating that Al-doped MnO_(2)has certain practical application value.This study provides favorable guidance for MnO_(2)as a high performance electrode material.
基金Project(52164025)supported by the National Natural Science Foundation of ChinaProject([2020]1Y219)supported by the Basic Research Program from the Science&Technology Department of Guizhou Province,China+2 种基金Project([2019]30)supported by the Training Project from Guizhou University,ChinaProject([2023]04)supported by the Guizhou University Innovation Talent Team Project,ChinaProject([2022]041)supported by the Natural Science Research Project of Guizhou Provincial Department of Education,China。
文摘Nitrogen doping has significant effects on the photocatalytic performance of ceria(CeO_(2)),and the possible synergistic effect with the inevitably introduced abundant oxygen vacancies(OVs)is of great significance for further investigation,and the specifically exposed crystal faces of CeO_(2)may have an impact on the performance of nitrogen doped CeO_(2).Herein,nitrogen-doped CeO_(2)with different morphologies and exposed crystal faces was prepared,and its performances in the photocatalytic degradation of tetracycline(TC)or hydrogen production via water splitting were evaluated.Density functional theory(DFT)was used to simulate the band structures,density of states,and oxygen defect properties of different CeO_(2)structures.It was found that nitrogen doping and OVs synergistically promoted the catalytic activity of nitrogen-doped CeO_(2).In addition,the exposed crystal faces of CeO_(2)have significant effects on the introduction of nitrogen and the ease of OV generation,as well as the synergistic effect of nitrogen doping with OVs.Among them,the rod-like nitrogen-doped CeO_(2)with exposed(110)face(R-CeO_(2)-NH_(3))showed a photocatalytic degradation ratio of 73.59%for TC and hydrogen production of 156.89μmol/g,outperforming other prepared photocatalysts.
基金Project(71671035)supported by the National Natural Science Foundation of ChinaProjects(ZK15-03-01,ZK16-03-07)supported by Open Fund of Jiangsu Wind Power Engineering Technology Center of China
文摘Aiming at wind turbines,the opportunistic maintenance optimization is carried out for multi-component system,where minimal repair,imperfect repair,replacement as well as their effects on component’s effective age are considered.At each inspection point,appropriate maintenance mode is selected according to the component’s effective age and its maintenance threshold.To utilize the maintenance opportunities for the components among the wind turbines,opportunistic maintenance approach is adopted.Meanwhile,the influence of seasonal factor on the component’s failure rate and improvement factor’s decrease with the increase of repair’s times are also taken into account.The maintenance threshold is set as the decision variable,and an opportunistic maintenance optimization model is proposed to minimize wind turbine’s life-cycle maintenance cost.Moreover,genetic algorithm is adopted to solve the model,and the effectiveness is verified with a case study.The results show that based on the component’s inherent reliability and maintainability,the proposed model can provide optimal maintenance plans accordingly.Furthermore,the higher the component’s reliability and maintainability are,the less the times of repair and replacement will be.
基金Project(51005238)supported by the National Natural Science Foundation of China
文摘To improve the mainlainability design efficiency and quality, a layout optimization method for maintainability of multi-component systems was proposed. The impact of the component layout design on system maintainability was analyzed, and the layout problem for maintainability was presented. It was formulated as an optimization problem, where maintainability, layout space and distance requirement were formulated as objective functions. A multi-objective particle swarm optimization algorithm, in which the constrained-domination relationship and the update strategy of the global best were simply modified, was then used to obtain Pareto optimal solutions for the maintainability layout design problem. Finally, application in oxygen generation system of a spacecraft was studied in detail to illustrate the effectiveness and usefulness of the proposed method. The results show that the concurrent maintainability design can be carried out during the layout design process by solving the layout optimization problem for maintainability.
基金supported by the Postdoctoral Science Foundation of China(20080431380)
文摘Although opportunistic maintenance strategies are widely used for multi-component systems, all opportunistic mainte- nance strategies only consider economic dependence and do not take structural dependence into account. An opportunistic main- tenance strategy is presented for a multi-component system that considers both structural dependence and economic dependence. The cost relation and time relation among components based on structural dependence are developed. The maintenance strategy for each component of a multi-component system involves one of five maintenance actions, namely, no-maintenance, a minimal maintenance action, an imperfect maintenance action, a perfect maintenance action, and a replacement action. The maintenance action is determined by the virtual age of the component, the life expectancy of the component, and the age threshold values. Monte Carlo simulation is designed to obtain the optimal oppor- tunistic maintenance strategy of the system over its lifetime. The simulation result reveals that the minimum maintenance cost with a strategy that considers structural dependence is less than that with a strategy that does not consider structural dependence. The availability with a strategy that considers structural dependence is greater than that with a strategy that does not consider structural dependence under the same conditions.
基金Projects (51275138,51605016) supported by the National Natural Science Foundation of ChinaProject (12531109) supported by the Science Foundation of Heilongjiang Provincial Department of Education,ChinaProject supported by Research Start-up Funding of Fudan University,China
文摘For unacceptable computational efficiency and accuracy on the probabilistic analysis of multi-component system with multi-failure modes,this paper proposed multi-extremum response surface method(MERSM).MERSM model was established based on quadratic polynomial function by taking extremum response surface model as the sub-model of multi-response surface method.The dynamic probabilistic analysis of an aeroengine turbine blisk with two components,and their reliability of deformation and stress failures was obtained,based on thermal-structural coupling technique,by considering the nonlinearity of material parameters and the transients of gas flow,gas temperature and rotational speed.The results show that the comprehensive reliability of structure is 0.9904 when the allowable deformations and stresses of blade and disk are 4.78×10–3 m and 1.41×109 Pa,and 1.64×10–3 m and 1.04×109 Pa,respectively.Besides,gas temperature and rotating speed severely influence the comprehensive reliability of system.Through the comparison of methods,it is shown that the MERSM holds higher computational precision and speed in the probabilistic analysis of turbine blisk,and MERSM computational precision satisfies the requirement of engineering design.The efforts of this study address the difficulties on transients and multiple models coupling for the dynamic probabilistic analysis of multi-component system with multi-failure modes.
文摘In this paper,the combined addition of copper or iron and sulphate ions onto TiO_(2) prepared by a simple sol-gel method is studied for formic acid photocatalytic conversion.A wide structural and morphological characterization of the different photocatalysts was performed by X-ray diffraction(XRD),N_(2)-physisorption for BET surface area measurements,scanning and transmission electronic microscopies(SEM and TEM),UV-Vis diffuse spectroscopy(DRS)and X-ray photoelectron spectroscopy(XPS),in order to correlate the physico-chemical properties of the materials to their photocatalytic efficiencies for formic acid oxidation.Results have shown important differences among the catalysts depending on the metal added.Sulphated TiO_(2)/Cu(1%Cu)was the best photocatalyst obtaining about 100% formic acid conversion in only 5 min.The appropriate physico-chemical features of this photocatalyst,given by the addition of combined copper and sulphate ions,explain its excellence in photocatalytic reaction.
文摘In order to investigate whether endohedral He-doping is possible or not in CL-20,a density functional treatment has been carried out at the levels of B3LYP/6-31++G(d,p)and B3PW91/6-31++G(d,p).Some physicochemical and quantum chemical properties of the helium-doped CL-20 (He@CL-20)are compared with the respective values of the parent explosive CL-20.The helium doping caused swelling of CL-20cage but no bond rupture occurred.Doped helium acquired some positive charge.
基金Project (2005CB623703) supported by the National Key Fundamental Research and Development Program of ChinaProject (50474051) supported by the National Natural Science Foundation of ChinaProject (03JJY3080) supported by the Natural Science Foundation of Hunan Province, China
文摘The effects of CaO content in the range from 0 to 4.0%, and sintering temperature on the phase composition, relative density and electrical conductivity of 10NiO-NiFe2O4 composites doped with CaO were studied. The results show that there is no change of structure for NiO or NiFe2O4; there is apparent oxygen absorbing and releasing behavior during the heating process in air for 10NiO-NiFe2O4 composites. Introduction of CaO can accelerate the densification of 10NiO-NiFe2O4 composites. The maximum value of relative density is 98.75% for composite doped with 2.0% CaO and sintered at 1 200 ℃, which is beyond about 20% for the undoped composites. The sintering activated energy of sample containing 2% CaO decreases by 15.87 kJ/mol, compared with that of the undoped sample.
文摘Nitrogen doping has been widely used to improve the performance of carbon electrodes in supercapacitors,particularly in terms of their high-frequency response.However,the charge storage and electrolyte ion response mechanisms of different nitrogen dopants at high frequencies are still unclear.In this study,melamine foam carbons with different configurations of surfacedoped N were formed by gradient carbonization,and the effects of the configurations on the high-frequency response behavior of the supercapacitors were analyzed.Using a combination of experiments and first-principle calculations,we found that pyrrolic N,characterized by a higher adsorption energy,increases the charge storage capacity of the electrode at high frequencies.On the other hand,graphitic N,with a lower adsorption energy,increases the speed of ion response.We propose the use of adsorption energy as a practical descriptor for electrode/electrolyte design in high-frequency applications,offering a more universal approach for improving the performance of N-doped carbon materials in supercapacitors.
基金Project(2008AA03Z207) supported by the National High-Tech Research and Development Program of China
文摘Polyaniline（PANI） nanofiber was synthesized by interfacial polymerization utilizing the interface between HC1 and CCl4. The hybrid type supercapacitors （PLi/C） based on Li-doping polyaniline and activated carbon electrode were fabricated and compared with the redox type capacitors （PLi/PLi） based on two uniformly Li-doping polyaniline electrodes. The electrochemical performances of the two types of supercapacitors were characterized in non-aqueous electrolyte. PLi/C supercapacitors have a wider effective energy storage potential range and a higher upper potential. At the same time, the PLi/C supercapacitor exhibits a specific capacity of 120.93 F/g at initial discharge and retains 80% after 500 cycles. The ohmic internal resistance （REs） of PLi/C supercapacitor is 5.0 Ω, which is smaller than that of PLi/PLi capacitor （5.5 Ω）. Moreover, it can be seen that EtgNBF4 organic solution is more suitable for using as organic electrolyte of PLi/C capacitor compared with organic solution containing LiPFr.
基金Project(2018YFB0104300)supported by the National Key R&D Program of ChinaProject(51774150)supported by the National Natural Science Foundation of China
文摘Shuttle effect,poor conductivity and large volume expansion are the main factors that hinder the practical application of sulfur cathodes.Currently,rational structure designing of carbon-based sulfur hosts is the most effective strategy to address the above issues.However,the preparation process of carbon-based sulfur hosts is usually complex and costly.Therefore,it is necessary to develop an efficient and cost-effective method to fabricate carbon hosts for high-performance sulfur cathodes.Herein,we reported the fabrication of a bio-derived nitrogen doped porous carbon materials(BNPC)via a molten-salt method for high performance sulfur cathodes.The long-range-ordered honeycomb structure of BNPC is favorable for the trapping of polysulfide(PS)species and accommodates the volumetric variation of sulfur during cycling,while the high graphitization degree of BNPC favors the redox kinetics of sulfur cathodes.Moreover,the nitrogen doping content not only enhances the electrical conductivity of BNPC,but also provides ample anchoring sites for the immobilization of PS,which plays a key role in suppressing the shuttle effect.As a result,the S@BNPC cathode exhibits a high initial specific capacity of 1189.4 mA·h/g at 0.2C.After 300 cycles,S@BNPC still maintains a capacity of 703.2 mA·h/g which corresponds to a fading rate of 0.13%per cycle after the second cycle.This work offers vast opportunities for the large-scale application of high performance carbon-based sulfur hosts.
文摘Martensitic transformation behavior was studied for zirconia containing 4%～10% CeO2 (in mole fraction) by using a dilatometric method. The Ms (Martensite start temperature) decreased near linearly with increasing CeO2. Different transformation modes were observed depending on the composition and cooling rate. ZrO2 containing 6% CeO2 showed isothermal transformation behavior, whereas ZrO2 containing 9% and 10% CeO2 showed athermal transformation behavior. However, ZrO2 containing 8% CeO2 showed either isothermal or athermal transformations behavior depending on the cooling rate. A TTT (Time-Temperature-Transformation) diagram was proposed for ZrO2 containing 8% CeO2.
文摘Fig.1 3D X-ray tomography reconstruction and element distribution in Ti,Mg and Al co-doped LiCoO2.3D spatial distributions of (a) Al,(b) Co and (c) Ti probed by fluorescence-yield scanning transmission X-ray microscopy;elemental distributions of (d) Al,(e) Co and (f) Ti over the virtual x-z slice through the center of the particle;(g) identified and visualized subdomain formation Fig.2 (a) Comparison of cycling stabilities of Ti,Mg and Al co-doped LiCoO2 and pristine LiCoO2 half cells,charge-discharge profiles of (b) pristine LiCoO2 and (c) Ti,Mg and Al co-doped LiCoO2 half cells,(d) cycle stabilities of Ti,Mg and Al co-doped LiCoO2 and pristine LiCoO2 full batteries (graphite was used anode) and (e) discharge voltage of the full batteries and energy density of the both materials as a function of cycle number Layered lithium cobalt oxide (LiCoO2) with a theoretical capacity of 274 mAh·g^-1 has become a dominant cathode material for lithium-ion batteries of “3C” market (cellular phones,portable computers,camcorders)[1-2].Nevertheless,the actually attained capacity is merely about 140 mAh·g^-1 with a charge cut-off vol- tage of about 4.2 V (vs Li +/Li)[3].
