Rectifying circuit,as a crucial component for converting alternating current into direct current,plays a pivotal role in energy harvesting microsystems.Traditional silicon-based or germanium-based rectifier diodes hin...Rectifying circuit,as a crucial component for converting alternating current into direct current,plays a pivotal role in energy harvesting microsystems.Traditional silicon-based or germanium-based rectifier diodes hinder system integration due to their specific manufacturing processes.Conversely,metal oxide diodes,with their simple fabrication techniques,offer advantages for system integration.The oxygen vacancy defect of oxide semiconductor will greatly affect the electrical performance of the device,so the performance of the diode can be effectively controlled by adjusting the oxygen vacancy concentration.This study centers on optimizing the performance of diodes by modulating the oxygen vacancy concentration within InGaZnO films through control of oxygen flows during the sputtering process.Experimental results demonstrate that the diode exhibits a forward current density of 43.82 A·cm^(−2),with a rectification ratio of 6.94×10^(4),efficiently rectifying input sine signals with 1 kHz frequency and 5 V magnitude.These results demonstrate its potential in energy conversion and management.By adjusting the oxygen vacancy,a methodology is provided for optimizing the performance of rectifying diodes.展开更多
The influence of oxygen vacancy-dominated carrier mobility on the performance of memristors has attractedconsiderable attention.The device’s carrier mobility can be significantly improved by forming a nano-multilayer...The influence of oxygen vacancy-dominated carrier mobility on the performance of memristors has attractedconsiderable attention.The device’s carrier mobility can be significantly improved by forming a nano-multilayeredheterostructure when the individual layer thickness is below a critical value.In this work,Pt/[ZrO_(2):Y_(2)O_(3)(YSZ)/SrTiO_(3)(STO)]n/Nb:SrTiO_(3)(NSTO)memristive devices were configurated through laser pulse deposited YSZ/STO nanomultilayeredactive layer with both Pt and NSTO acting as top and counter electrodes.Specifically,the Pt/[YSZ/STO]5/NSTO device with five consecutive layers of YSZ/STO thin film shows superior memristor performance,and itscorresponding carrier mobility presents a significantly enhanced value compared to that of other periodic numbers ofYSZ/STO composed memristive devices.This can be attributed to the increase of oxygen vacancy concentration in thedevice,as evidenced by both experimental results and theoretical analysis.This work provides a significant approach inimproving the performance of memristor dominated by oxygen vacancy transporting mechanism.展开更多
On the surfaces of celestial bodies with no or thin atmospheres,such as the Moon and Mars,the solar wind irradiation process leads to the formation of hydrogen and helium enriched regions in the extraterrestrial soil ...On the surfaces of celestial bodies with no or thin atmospheres,such as the Moon and Mars,the solar wind irradiation process leads to the formation of hydrogen and helium enriched regions in the extraterrestrial soil particles.However,soil particles on the Earth with the similar composition lack such structures and properties.This discrepancy raises a key question whether there is a direct relationship between solar wind irradiation and the alterations in the structure and chemical performance of extraterrestrial materials.To address this question,this work investigates the effects of proton irradiation,simulating solar wind radiation,on the structure and photothermal catalytic properties of the classic catalyst In_(2)O_(3).It reveals that proton irradiation induces structural features in In_(2)O_(3) analogous to those characteristics of solar wind weathering observed in extraterrestrial materials.Furthermore,after proton beam irradiation with an energy of 30 keV and a dose of 3×10^(17) protons·cm^(-2),the methanol production yield of the In_(2)O_(3) catalyst increased to 2.6 times of its preirradiation level,and the methanol selectivity improved to 2.1 times of the original value.This work provides both theoretical and experimental support for the development of high-efficiency,radiation-resistant photothermal catalysts.展开更多
The conversion of urea-containing wastewater into clean hydrogen energy has gained increasing attention.However,challenges remain,particularly with sluggish catalytic kinetics and limited long-term stability of urea o...The conversion of urea-containing wastewater into clean hydrogen energy has gained increasing attention.However,challenges remain,particularly with sluggish catalytic kinetics and limited long-term stability of urea oxidation reaction(UOR).Herein,we report the loosely porous CoOOH nano-architecture(CoOOH LPNAs)with hydrophilic surface and abundant oxygen vacancies(Ov)on carbon fiber paper(CFP)by electrochemical reconstruction of the CoP nanoneedles precursor.The resulting three-dimensional electrode exhibited an impressively low potential of 1.38 V at 1000 mA·cm^(−2) and excellent durability for UOR.Furthermore,when tested in an anion exchange membrane(AEM)electrolyzer,it required only 1.53 V at 1000 mA·cm^(−2) for industrial urea-assisted water splitting and operated stably for 100 h without degrada-tion.Experimental and theoretical investigations revealed that rich oxygen vacancies effectively modulate the electronic structure of the CoOOH while creating unique Co3-triangle sites with Co atoms close together.As a result,the adsorption and desorption processes of reactants and intermediates in UOR could be finely tuned,thereby significantly reducing ther-modynamic barriers.Additionally,the superhydrophilic self-supported nanoarray structure facilitated rapid gas bubble release,improving the overall efficiency of the reaction and preventing potential catalyst detachment caused by bubble accumulation,thereby improving both catalytic activity and stability at high current densities.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
Using carbon felt, polytetrafluoroethylene latex and powder catalyst to assembly a light energy conversion device, the photocatalytic activity of catalyst 2.0%WO3-TiO2 （2%WO3 compounding TiO2） with oxygen vacancies ...Using carbon felt, polytetrafluoroethylene latex and powder catalyst to assembly a light energy conversion device, the photocatalytic activity of catalyst 2.0%WO3-TiO2 （2%WO3 compounding TiO2） with oxygen vacancies was studied through the water splitting for O2 evolution, using a high pressure mercury lamp as the light source and Fe^3＋ as the electron acceptor in two different devices： an ordinary photolysis device with catalyst powder suspending through a magnetic stirrer and a self-assembly light energy conversion device. The results show that after 12 h irradiation, the photocatalytic activity of 2.0%WO3-TiO2 with oxygen vacancies in the self-assembly light energy conversion device is higher than that of the ordinary photolysis device, and the amount of oxygen evolution is about 12 and 9 mmol/L respectively in these two devices. After 12 h, the rates of 02 evolution are slow in each device and the photocatalyst almost loses the photoactivity in the ordinary photolysis device. So, compared with the ordinary photocatalytic device, the rate of oxygen evolution and the life time of the catalyst are improved in the self-assembly light energy conversion device.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
High-temperature piezoelectric vibration sensors are the preferred choice for structural health monitoring in harsh environments such as high temperatures and complex vibrations.Bismuth layer-structured CaBi_(4)Ti_(4)...High-temperature piezoelectric vibration sensors are the preferred choice for structural health monitoring in harsh environments such as high temperatures and complex vibrations.Bismuth layer-structured CaBi_(4)Ti_(4)O_(15)(CBT)high-temperature piezoelectric ceramics,with high Curie temperature(TC),are the key components for piezoelectric vibration sensors operating at temperatures exceeding 500℃.However,their low piezoelectric coefficient(d_(33))greatly limits their high-temperature applications.In this work,a novel Bi^(3+)self-doping strategy was employed to enhance the piezoelectric performance of CBT ceramics.The enhancement is attributed to an increase in the number of grain boundaries,providing more sites for space charge accumulation and promoting formation of space charge polarization.Furthermore,given that space charge polarization predominantly occurs at low frequencies,dielectric temperature spectra at different frequencies were used to elucidate the mechanism by which space charge polarization enhances piezoelectric properties of CBT ceramics.Excellent overall performance was achieved for the CBT-based high-temperature piezoelectric ceramics.Among them,TC reached 778℃,d_(33) increased by more than 30%,reaching 20.1 pC/N,and the electrical resistivity improved by one order of magnitude(reaching 6.33×10^(6)Ω·cm at 500℃).These advancements provide a key functional material with excellent performance for practical applications of piezoelectric vibration sensors at 500℃and above.展开更多
The conversion of CO_(2)to dimethyl carbonate(DMC)offers a promising route for CO_(2)utilization.In this study,four CeO2 catalysts with distinct nanostructures were synthesized via a template-free hydrothermal method ...The conversion of CO_(2)to dimethyl carbonate(DMC)offers a promising route for CO_(2)utilization.In this study,four CeO2 catalysts with distinct nanostructures were synthesized via a template-free hydrothermal method by systematically varying the types and concentrations of precipitants as well as the hydrothermal reaction conditions,and they were employed for DMC synthesis from CO_(2)and methanol.The atomic arrangements of CeO_(2)varied significantly with its morphology,leading to differences in lattice distortion,which directly influenced the concentration of oxygen vacancies.Notably,the CeO_(2)nanospheres,which exhibited the highest lattice distortion and oxygen vacancy concentration,achieved a DMC yield(11.12 mmol/g)48 times greater than that of the nanocubes(0.23 mmol/g).The results indicated that oxygen vacancies played a pivotal role in the catalytic process by facilitating the adsorption and activation of CO_(2)to form bidentate carbonates,as well as activating methanol to generate methoxy species.These processes collectively promoted the formation of the key intermediate(*CH3OCOO).This study proposes a strategy to enhance the oxygen vacancy concentration by increasing lattice distortion,providing valuable insights for designing high-performance CeO_(2)catalysts for DMC synthesis.展开更多
文摘Rectifying circuit,as a crucial component for converting alternating current into direct current,plays a pivotal role in energy harvesting microsystems.Traditional silicon-based or germanium-based rectifier diodes hinder system integration due to their specific manufacturing processes.Conversely,metal oxide diodes,with their simple fabrication techniques,offer advantages for system integration.The oxygen vacancy defect of oxide semiconductor will greatly affect the electrical performance of the device,so the performance of the diode can be effectively controlled by adjusting the oxygen vacancy concentration.This study centers on optimizing the performance of diodes by modulating the oxygen vacancy concentration within InGaZnO films through control of oxygen flows during the sputtering process.Experimental results demonstrate that the diode exhibits a forward current density of 43.82 A·cm^(−2),with a rectification ratio of 6.94×10^(4),efficiently rectifying input sine signals with 1 kHz frequency and 5 V magnitude.These results demonstrate its potential in energy conversion and management.By adjusting the oxygen vacancy,a methodology is provided for optimizing the performance of rectifying diodes.
基金Projects(2023JJ30690,2022JJ30722)supported by the Natural Science Foundation of Hunan Province,ChinaProject(kq2202093)supported by the Natural Science Foundation of Changsha,ChinaProject(SKL202202SIC)supported by the Opening Project of State Key Laboratory of High Performance Ceramics and Superfine Microstructure,China。
文摘The influence of oxygen vacancy-dominated carrier mobility on the performance of memristors has attractedconsiderable attention.The device’s carrier mobility can be significantly improved by forming a nano-multilayeredheterostructure when the individual layer thickness is below a critical value.In this work,Pt/[ZrO_(2):Y_(2)O_(3)(YSZ)/SrTiO_(3)(STO)]n/Nb:SrTiO_(3)(NSTO)memristive devices were configurated through laser pulse deposited YSZ/STO nanomultilayeredactive layer with both Pt and NSTO acting as top and counter electrodes.Specifically,the Pt/[YSZ/STO]5/NSTO device with five consecutive layers of YSZ/STO thin film shows superior memristor performance,and itscorresponding carrier mobility presents a significantly enhanced value compared to that of other periodic numbers ofYSZ/STO composed memristive devices.This can be attributed to the increase of oxygen vacancy concentration in thedevice,as evidenced by both experimental results and theoretical analysis.This work provides a significant approach inimproving the performance of memristor dominated by oxygen vacancy transporting mechanism.
基金National Key Research and Development Program of China(2020YFA0710302)The Major Research Plan of the National Natural Science Foundation of China(91963206)+2 种基金The National Natural Science Foundation of China(52072169,51972164,51972167,22279053)The Fundamental Research Funds for the Central Universities(14380193)The Program for Guangdong Introducing Innovative and Entrepreneurial Teams(2019ZT08L101).
文摘On the surfaces of celestial bodies with no or thin atmospheres,such as the Moon and Mars,the solar wind irradiation process leads to the formation of hydrogen and helium enriched regions in the extraterrestrial soil particles.However,soil particles on the Earth with the similar composition lack such structures and properties.This discrepancy raises a key question whether there is a direct relationship between solar wind irradiation and the alterations in the structure and chemical performance of extraterrestrial materials.To address this question,this work investigates the effects of proton irradiation,simulating solar wind radiation,on the structure and photothermal catalytic properties of the classic catalyst In_(2)O_(3).It reveals that proton irradiation induces structural features in In_(2)O_(3) analogous to those characteristics of solar wind weathering observed in extraterrestrial materials.Furthermore,after proton beam irradiation with an energy of 30 keV and a dose of 3×10^(17) protons·cm^(-2),the methanol production yield of the In_(2)O_(3) catalyst increased to 2.6 times of its preirradiation level,and the methanol selectivity improved to 2.1 times of the original value.This work provides both theoretical and experimental support for the development of high-efficiency,radiation-resistant photothermal catalysts.
基金supported by the Applied Basic Research Program of Yunnan Province(202101BE070001-032)Yunnan Major Scientific and Technological Projects(No.202202AG050001).
文摘The conversion of urea-containing wastewater into clean hydrogen energy has gained increasing attention.However,challenges remain,particularly with sluggish catalytic kinetics and limited long-term stability of urea oxidation reaction(UOR).Herein,we report the loosely porous CoOOH nano-architecture(CoOOH LPNAs)with hydrophilic surface and abundant oxygen vacancies(Ov)on carbon fiber paper(CFP)by electrochemical reconstruction of the CoP nanoneedles precursor.The resulting three-dimensional electrode exhibited an impressively low potential of 1.38 V at 1000 mA·cm^(−2) and excellent durability for UOR.Furthermore,when tested in an anion exchange membrane(AEM)electrolyzer,it required only 1.53 V at 1000 mA·cm^(−2) for industrial urea-assisted water splitting and operated stably for 100 h without degrada-tion.Experimental and theoretical investigations revealed that rich oxygen vacancies effectively modulate the electronic structure of the CoOOH while creating unique Co3-triangle sites with Co atoms close together.As a result,the adsorption and desorption processes of reactants and intermediates in UOR could be finely tuned,thereby significantly reducing ther-modynamic barriers.Additionally,the superhydrophilic self-supported nanoarray structure facilitated rapid gas bubble release,improving the overall efficiency of the reaction and preventing potential catalyst detachment caused by bubble accumulation,thereby improving both catalytic activity and stability at high current densities.
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(2010CL04) supported by the Hunan Provincial Key Laboratory of Materials Protection for Electric Power and Transportation, ChinaProject(K-081025) supported by State Key Laboratory Breeding Base of Photocatalysis,Fuzhou University,China
文摘Using carbon felt, polytetrafluoroethylene latex and powder catalyst to assembly a light energy conversion device, the photocatalytic activity of catalyst 2.0%WO3-TiO2 （2%WO3 compounding TiO2） with oxygen vacancies was studied through the water splitting for O2 evolution, using a high pressure mercury lamp as the light source and Fe^3＋ as the electron acceptor in two different devices： an ordinary photolysis device with catalyst powder suspending through a magnetic stirrer and a self-assembly light energy conversion device. The results show that after 12 h irradiation, the photocatalytic activity of 2.0%WO3-TiO2 with oxygen vacancies in the self-assembly light energy conversion device is higher than that of the ordinary photolysis device, and the amount of oxygen evolution is about 12 and 9 mmol/L respectively in these two devices. After 12 h, the rates of 02 evolution are slow in each device and the photocatalyst almost loses the photoactivity in the ordinary photolysis device. So, compared with the ordinary photocatalytic device, the rate of oxygen evolution and the life time of the catalyst are improved in the self-assembly light energy conversion device.
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 (51932010)。
文摘High-temperature piezoelectric vibration sensors are the preferred choice for structural health monitoring in harsh environments such as high temperatures and complex vibrations.Bismuth layer-structured CaBi_(4)Ti_(4)O_(15)(CBT)high-temperature piezoelectric ceramics,with high Curie temperature(TC),are the key components for piezoelectric vibration sensors operating at temperatures exceeding 500℃.However,their low piezoelectric coefficient(d_(33))greatly limits their high-temperature applications.In this work,a novel Bi^(3+)self-doping strategy was employed to enhance the piezoelectric performance of CBT ceramics.The enhancement is attributed to an increase in the number of grain boundaries,providing more sites for space charge accumulation and promoting formation of space charge polarization.Furthermore,given that space charge polarization predominantly occurs at low frequencies,dielectric temperature spectra at different frequencies were used to elucidate the mechanism by which space charge polarization enhances piezoelectric properties of CBT ceramics.Excellent overall performance was achieved for the CBT-based high-temperature piezoelectric ceramics.Among them,TC reached 778℃,d_(33) increased by more than 30%,reaching 20.1 pC/N,and the electrical resistivity improved by one order of magnitude(reaching 6.33×10^(6)Ω·cm at 500℃).These advancements provide a key functional material with excellent performance for practical applications of piezoelectric vibration sensors at 500℃and above.
基金National Natural Science Foundation of China(22008166)Fundamental Research Program of Shanxi Province(202403021211029,201901D211047).
文摘The conversion of CO_(2)to dimethyl carbonate(DMC)offers a promising route for CO_(2)utilization.In this study,four CeO2 catalysts with distinct nanostructures were synthesized via a template-free hydrothermal method by systematically varying the types and concentrations of precipitants as well as the hydrothermal reaction conditions,and they were employed for DMC synthesis from CO_(2)and methanol.The atomic arrangements of CeO_(2)varied significantly with its morphology,leading to differences in lattice distortion,which directly influenced the concentration of oxygen vacancies.Notably,the CeO_(2)nanospheres,which exhibited the highest lattice distortion and oxygen vacancy concentration,achieved a DMC yield(11.12 mmol/g)48 times greater than that of the nanocubes(0.23 mmol/g).The results indicated that oxygen vacancies played a pivotal role in the catalytic process by facilitating the adsorption and activation of CO_(2)to form bidentate carbonates,as well as activating methanol to generate methoxy species.These processes collectively promoted the formation of the key intermediate(*CH3OCOO).This study proposes a strategy to enhance the oxygen vacancy concentration by increasing lattice distortion,providing valuable insights for designing high-performance CeO_(2)catalysts for DMC synthesis.
