Perovskite SrTaO_(2)N is one of the most promising narrow-bandgap photocatalysts for Z-scheme overall water splitting.However,the formation of defect states during thermal nitridation severely hinders the separation o...Perovskite SrTaO_(2)N is one of the most promising narrow-bandgap photocatalysts for Z-scheme overall water splitting.However,the formation of defect states during thermal nitridation severely hinders the separation of charges,resulting in poor photocatalytic activity.In the present study,we successfully synthesize SrTaO_(2)N photocatalyst with low density of defect states,uniform morphology and particle size by flux-assisted one-pot nitridation combined with Mg doping.Some important parameters,such as the size of unit cell,the content of nitrogen,and microstructure,prove the successful doping of Mg.The defect-related carrier recombination has been significantly reduced by Mg doping,which effectively promotes the charge separation.Moreover,Mg doping induces a change of the band edge,which makes proton reduction have a stronger driving force.After modifying with the core/shell-structured Pt/Cr_(2)O_(3)cocatalyst,the H_(2)evolution activity of the optimized SrTaO_(2)N:Mg is 10 times that of the undoped SrTaO_(2)N,with an impressive apparent quantum yield of 1.51%at 420 nm.By coupling with Au-FeCoO_(x)modified BiVO_(4)as an O_(2)-evolution photocatalyst and[Fe(CN)_(6)]_(3)−/[Fe(CN)_(6)]_(4)−as the redox couple,a redox-based Z-scheme overall water splitting system is successfully constructed with an apparent quantum yield of 1.36%at 420 nm.This work provides an alternative way to prepare oxynitride semiconductors with reduced defects to promote the conversion of solar energy.展开更多
In the present research,the NaF assisted plasma electrolytic oxidation(PEO)is designed to fabricate the high-content ZnO nanoparti-cles doped coating on AZ31B alloy.The microstructure,phase constituents and corrosion ...In the present research,the NaF assisted plasma electrolytic oxidation(PEO)is designed to fabricate the high-content ZnO nanoparti-cles doped coating on AZ31B alloy.The microstructure,phase constituents and corrosion behavior of the PEO coatings are investigated systematically.The results reveal that the introduction of NaF promotes the formation of MgF2 nanophases in the passivation layer on Mg alloy,decreasing the breakdown voltage and discharge voltage.As a result,the continuous arcing caused by high discharge voltage is alleviated.With the increasing of NaF content,the Zn content in the PEO coating is enhanced and the pore size in the coating is decreased correspondingly.Due to the high-content ZnO doping,the PEO coating protected AZ31B alloy demonstrates the better corrosion resistance.Compared with the bare AZ31B alloy,the high-content ZnO doped PEO coated sample shows an increased corrosion potential from-1.465 V to-1.008 V,a decreased corrosion current density from 3.043×10^(-5) A·cm^(-2) to 3.960×10^(-8) A·cm^(-2) and an increased charge transfer resistance from 1.213×10^(2) ohm·cm^(2) to 2.598×10^(5) ohm·cm^(2).Besides,the high-content ZnO doped PEO coated sample also has the excellent corrosion resistance in salt solution,exhibiting no obvious corrosion after more than 2000 h neutral salt spraying and 28 days’immersion testing.The improved corrosion resistance can be ascribed to the relative uniform distribution of ZnO in PEO coating which can transform to Zn(OH)2 and form a continuous protective layer along the corrosion interface.展开更多
Neutron resonance imaging(NRI)has recently emerged as an appealing technique for neutron radiography.Its complexity surpasses that of conventional transmission imaging,as it requires a high demand for both a neutron s...Neutron resonance imaging(NRI)has recently emerged as an appealing technique for neutron radiography.Its complexity surpasses that of conventional transmission imaging,as it requires a high demand for both a neutron source and detector.Consequently,the progression of NRI technology has been sluggish since its inception in the 1980s,particularly considering the limited studies analyzing the neutron energy range above keV.The white neutron source(Back-n)at the China Spallation Neutron Source(CSNS)provides favorable beam conditions for the development of the NRI technique over a wide neutron energy range from eV to MeV.Neutron-sensitive microchannel plates(MCP)have emerged as a cutting-edge tool in the field of neutron detection owing to their high temporal and spatial resolutions,high detection efficiency,and low noise.In this study,we report the development of a 10B-doped MCP detector,along with its associated electronics,data processing system,and NRI experiments at the Back-n.Individual heavy elements such as gold,silver,tungsten,and indium can be easily identified in the transmission images by their characteristic resonance peaks in the 1–100 eV energy range;the more difficult medium-weight elements such as iron,copper,and aluminum with resonance peaks in the 1–100 keV energy range can also be identified.In particular,results in the neutron energy range of dozens of keV(Aluminum)are reported here for the first time.展开更多
Biomass‐derived carbon is a promising electrode material in energy storage devices.However,how to improve its low capacity and stability,and slow diffusion kinetics during lithium storage remains a challenge.In this ...Biomass‐derived carbon is a promising electrode material in energy storage devices.However,how to improve its low capacity and stability,and slow diffusion kinetics during lithium storage remains a challenge.In this research,we propose a“self‐assembly‐template”method to prepare B,N codoped porous carbon(BN‐C)with a nanosandwich structure and abundant pyridinic N‐B species.The nanosandwich structure can increase powder density and cycle stability by constructing a stable solid electrolyte interphase film,shortening the Li^(+) diffusion pathway,and accommodating volume expansion during repeated charging/discharging.The abundant pyridinic N‐B species can simultaneously promote the adsorption/desorption of Li^(+)/PF_(6)^(−) and reduce the diffusion barrier.The BN‐C electrode showed a high lithium‐ion storage capacity of above 1140 mAh g^(−1) at 0.05 A g^(−1) and superior stability(96.5% retained after 2000 cycles).Moreover,owing to the synergistic effect of the nanosandwich structure and pyridinic N‐B species,the assembled symmetrical BN‐C//BN‐C full cell shows a high energy density of 234.7Wh kg^(−1),high power density of 39.38 kW kg−1,and excellent cycling stability,superior to most of the other cells reported in the literature.As the density functional theory simulation demonstrated,pyridinic N‐B shows enhanced adsorption activity for Li^(+) and PF_(6)^(−),which promotes an increase in the capacity of the anode and cathode,respectively.Meanwhile,the relatively lower diffusion barrier of pyridinic N‐B promotes Li^(+) migration,resulting in good rate performance.Therefore,this study provides a new approach for the synergistic modulation of a nanostructure and an active site simultaneously to fabricate the carbon electrode material in energy storage devices.展开更多
This study delves into the charge transfer mechanism of boron (B)-doped 3C-SiC through first-principles investigations. We explore the effects of B doping on the electronic properties of 3C-SiC, focusing on a 12.5% im...This study delves into the charge transfer mechanism of boron (B)-doped 3C-SiC through first-principles investigations. We explore the effects of B doping on the electronic properties of 3C-SiC, focusing on a 12.5% impurity concentration. Our comprehensive analysis encompasses structural properties, electronic band structures, and charge density distributions. The optimized lattice constant and band gap energy of 3C-SiC were found to be 4.373 Å and 1.36 eV respectively, which is in agreement with previous research (Bui, 2012;Muchiri et al., 2018). Our results show that B doping narrows the band gap, enhances electrical conductivity, and influences charge transfer interactions. The charge density analysis reveals substantial interactions between B dopants and surrounding carbon atoms. This work not only enhances our understanding of the material’s electronic properties, but also highlights the importance of charge density analysis for characterizing charge transfer mechanisms and their implications in the 3C-SiC semiconductors.展开更多
Fe/N/C catalysts,synthesized through the pyrolysis of Fe-doped metal–organic framework (MOF) precursors,have attracted extensive attention owing to their promising oxygen reduction reaction (ORR) catalytic activity i...Fe/N/C catalysts,synthesized through the pyrolysis of Fe-doped metal–organic framework (MOF) precursors,have attracted extensive attention owing to their promising oxygen reduction reaction (ORR) catalytic activity in fuel cells and/or metal-air batteries.However,post-treatments (acid washing,second pyrolysis,and so on) are unavoidable to improve ORR catalytic activity and stability.The method for introducing Fe^(3+) sources (anhydrous Fe Cl_(3)) into the MOF structure,in particular,is a critical step that can avoid time-consuming post-treatments and result in more exposed Fe-N_(x) active sites.Herein,three different Fe doping strategies were systematically investigated to explore their influence on the types of active sites formed and ORR performance.Fe-NC(Zn^(2+)),synthesized by one-step pyrolysis of Fe doped ZIF-8 (Zn^(2+)) precursor which was obtained by adding the anhydrous Fe Cl_(3)source into the Zn(NO_(3))_(2)·6H_(2)O/methanol solution before mixing,possessed the highest Fe-N_(x)active sites due to the high-efficiency substitution of Zn^(2+)ions with Fe^(3+) ions during ZIF-8 growth,the strong interaction between Fe^(3+) ions and N atoms of 2-Methylimidazole (2-MIm),and ZIF-8’s micropore confinement effect.As a result,Fe-NC(Zn^(2+)) presented high ORR activity in the entire p H range (p H=1,7,and 13).At p H=13,Fe-NC(Zn^(2+)) exhibited a half-wave potential (E1/2) of 0.95 V (vs.reversible hydrogen electrode),which was 70 m V higher than that of commercial Pt/C.More importantly,Fe-NC(Zn^(2+)) showed superior ORR stability in neutral media without performance loss after 5,000 cycles.A record-high open-circuit voltage(1.9 V) was obtained when Fe-NC(Zn^(2+)) was used as a cathodic catalyst in assembled Mg-air batteries in neutral media.The assembled liquid and all-solid Mg-air batteries with high performance indicated that Fe-NC(Zn^(2+)) has enormous potential for use in flexible and wearable Mg-air batteries.展开更多
This report describes an equivalent doping profile transformation method with which the avalanche breakdown voltage of the asymmetric linearly graded junction was analytically predicted.The maximum breakdown voltage a...This report describes an equivalent doping profile transformation method with which the avalanche breakdown voltage of the asymmetric linearly graded junction was analytically predicted.The maximum breakdown voltage and the different depletion layer extension on the diffused side and substrate side are demonstrated in the report.The report shows the equivalent doping profile method is valid to predict the breakdown voltage of the complex P N junction.The analytical results agree with the experimental breakdown voltage in comparison with the abrupt junction and symmetric linearly graded junction approximations.展开更多
文摘Perovskite SrTaO_(2)N is one of the most promising narrow-bandgap photocatalysts for Z-scheme overall water splitting.However,the formation of defect states during thermal nitridation severely hinders the separation of charges,resulting in poor photocatalytic activity.In the present study,we successfully synthesize SrTaO_(2)N photocatalyst with low density of defect states,uniform morphology and particle size by flux-assisted one-pot nitridation combined with Mg doping.Some important parameters,such as the size of unit cell,the content of nitrogen,and microstructure,prove the successful doping of Mg.The defect-related carrier recombination has been significantly reduced by Mg doping,which effectively promotes the charge separation.Moreover,Mg doping induces a change of the band edge,which makes proton reduction have a stronger driving force.After modifying with the core/shell-structured Pt/Cr_(2)O_(3)cocatalyst,the H_(2)evolution activity of the optimized SrTaO_(2)N:Mg is 10 times that of the undoped SrTaO_(2)N,with an impressive apparent quantum yield of 1.51%at 420 nm.By coupling with Au-FeCoO_(x)modified BiVO_(4)as an O_(2)-evolution photocatalyst and[Fe(CN)_(6)]_(3)−/[Fe(CN)_(6)]_(4)−as the redox couple,a redox-based Z-scheme overall water splitting system is successfully constructed with an apparent quantum yield of 1.36%at 420 nm.This work provides an alternative way to prepare oxynitride semiconductors with reduced defects to promote the conversion of solar energy.
基金supported by the 2022 Shenzhen sustainable supporting funds for colleges and universities(20220810143642004)Shenzhen Basic Research Project(JCYJ20200109144608205 and JCYJ20210324120001003)+5 种基金Peking University Shenzhen Graduate School Research Startup Fund of Introducing Talent(No.1270110273)Shenzhen postdoctoral research fund project after outbound(No.2129933651)Shenzhen-Hong Kong Research and Development Fund(No.SGDX20201103095406024)City University of Hong Kong Strategic Research Grants(SRG)(Nos.7005264 and 7005505)Guangdong-Hong Kong Technology Cooperation Funding Scheme(TCFS)(No.GHP/085/18SZ)IER Foundation(IERF2020001 and IERF2019002).
文摘In the present research,the NaF assisted plasma electrolytic oxidation(PEO)is designed to fabricate the high-content ZnO nanoparti-cles doped coating on AZ31B alloy.The microstructure,phase constituents and corrosion behavior of the PEO coatings are investigated systematically.The results reveal that the introduction of NaF promotes the formation of MgF2 nanophases in the passivation layer on Mg alloy,decreasing the breakdown voltage and discharge voltage.As a result,the continuous arcing caused by high discharge voltage is alleviated.With the increasing of NaF content,the Zn content in the PEO coating is enhanced and the pore size in the coating is decreased correspondingly.Due to the high-content ZnO doping,the PEO coating protected AZ31B alloy demonstrates the better corrosion resistance.Compared with the bare AZ31B alloy,the high-content ZnO doped PEO coated sample shows an increased corrosion potential from-1.465 V to-1.008 V,a decreased corrosion current density from 3.043×10^(-5) A·cm^(-2) to 3.960×10^(-8) A·cm^(-2) and an increased charge transfer resistance from 1.213×10^(2) ohm·cm^(2) to 2.598×10^(5) ohm·cm^(2).Besides,the high-content ZnO doped PEO coated sample also has the excellent corrosion resistance in salt solution,exhibiting no obvious corrosion after more than 2000 h neutral salt spraying and 28 days’immersion testing.The improved corrosion resistance can be ascribed to the relative uniform distribution of ZnO in PEO coating which can transform to Zn(OH)2 and form a continuous protective layer along the corrosion interface.
基金supported by the National Natural Science Foundation of China(No.12035017)the Guangdong Basic and Applied Basic Research Foundation(No.2023A1515030074)。
文摘Neutron resonance imaging(NRI)has recently emerged as an appealing technique for neutron radiography.Its complexity surpasses that of conventional transmission imaging,as it requires a high demand for both a neutron source and detector.Consequently,the progression of NRI technology has been sluggish since its inception in the 1980s,particularly considering the limited studies analyzing the neutron energy range above keV.The white neutron source(Back-n)at the China Spallation Neutron Source(CSNS)provides favorable beam conditions for the development of the NRI technique over a wide neutron energy range from eV to MeV.Neutron-sensitive microchannel plates(MCP)have emerged as a cutting-edge tool in the field of neutron detection owing to their high temporal and spatial resolutions,high detection efficiency,and low noise.In this study,we report the development of a 10B-doped MCP detector,along with its associated electronics,data processing system,and NRI experiments at the Back-n.Individual heavy elements such as gold,silver,tungsten,and indium can be easily identified in the transmission images by their characteristic resonance peaks in the 1–100 eV energy range;the more difficult medium-weight elements such as iron,copper,and aluminum with resonance peaks in the 1–100 keV energy range can also be identified.In particular,results in the neutron energy range of dozens of keV(Aluminum)are reported here for the first time.
基金Jiangsu Key Lab of Biomass Energy and Material,Grant/Award Number:JSBEMS‐202101National Natural Science Foundation of China,Grant/Award Numbers:51902162,51902162+4 种基金National Key R&D Program of China,Grant/Award Number:2022YFB4201904Foundation of Jiangsu Key Lab of Biomass Energy and Material,Grant/Award Number:JSBEM‐S‐202101National Key R&D Program,Grant/Award Number:2022YFB4201904Jiangsu Co‐Innovation Center of Efficient Processing and Utilization of Forest Resources,the International Innovation Center for Forest Chemicals and Materialsanjing Forestry University。
文摘Biomass‐derived carbon is a promising electrode material in energy storage devices.However,how to improve its low capacity and stability,and slow diffusion kinetics during lithium storage remains a challenge.In this research,we propose a“self‐assembly‐template”method to prepare B,N codoped porous carbon(BN‐C)with a nanosandwich structure and abundant pyridinic N‐B species.The nanosandwich structure can increase powder density and cycle stability by constructing a stable solid electrolyte interphase film,shortening the Li^(+) diffusion pathway,and accommodating volume expansion during repeated charging/discharging.The abundant pyridinic N‐B species can simultaneously promote the adsorption/desorption of Li^(+)/PF_(6)^(−) and reduce the diffusion barrier.The BN‐C electrode showed a high lithium‐ion storage capacity of above 1140 mAh g^(−1) at 0.05 A g^(−1) and superior stability(96.5% retained after 2000 cycles).Moreover,owing to the synergistic effect of the nanosandwich structure and pyridinic N‐B species,the assembled symmetrical BN‐C//BN‐C full cell shows a high energy density of 234.7Wh kg^(−1),high power density of 39.38 kW kg−1,and excellent cycling stability,superior to most of the other cells reported in the literature.As the density functional theory simulation demonstrated,pyridinic N‐B shows enhanced adsorption activity for Li^(+) and PF_(6)^(−),which promotes an increase in the capacity of the anode and cathode,respectively.Meanwhile,the relatively lower diffusion barrier of pyridinic N‐B promotes Li^(+) migration,resulting in good rate performance.Therefore,this study provides a new approach for the synergistic modulation of a nanostructure and an active site simultaneously to fabricate the carbon electrode material in energy storage devices.
文摘This study delves into the charge transfer mechanism of boron (B)-doped 3C-SiC through first-principles investigations. We explore the effects of B doping on the electronic properties of 3C-SiC, focusing on a 12.5% impurity concentration. Our comprehensive analysis encompasses structural properties, electronic band structures, and charge density distributions. The optimized lattice constant and band gap energy of 3C-SiC were found to be 4.373 Å and 1.36 eV respectively, which is in agreement with previous research (Bui, 2012;Muchiri et al., 2018). Our results show that B doping narrows the band gap, enhances electrical conductivity, and influences charge transfer interactions. The charge density analysis reveals substantial interactions between B dopants and surrounding carbon atoms. This work not only enhances our understanding of the material’s electronic properties, but also highlights the importance of charge density analysis for characterizing charge transfer mechanisms and their implications in the 3C-SiC semiconductors.
基金supported by the National Natural Science Foundation of China(22171266)the FJIRSM&IUE Joint Research Fund(RHZX-2019-002)+2 种基金the STS Project(KFJ-STS-QYZD-2021-09002)the National Key Basic Research Program of China(2017YFA0403402)the Project of the National Natural Science Foundation of China(U1932119)。
文摘Fe/N/C catalysts,synthesized through the pyrolysis of Fe-doped metal–organic framework (MOF) precursors,have attracted extensive attention owing to their promising oxygen reduction reaction (ORR) catalytic activity in fuel cells and/or metal-air batteries.However,post-treatments (acid washing,second pyrolysis,and so on) are unavoidable to improve ORR catalytic activity and stability.The method for introducing Fe^(3+) sources (anhydrous Fe Cl_(3)) into the MOF structure,in particular,is a critical step that can avoid time-consuming post-treatments and result in more exposed Fe-N_(x) active sites.Herein,three different Fe doping strategies were systematically investigated to explore their influence on the types of active sites formed and ORR performance.Fe-NC(Zn^(2+)),synthesized by one-step pyrolysis of Fe doped ZIF-8 (Zn^(2+)) precursor which was obtained by adding the anhydrous Fe Cl_(3)source into the Zn(NO_(3))_(2)·6H_(2)O/methanol solution before mixing,possessed the highest Fe-N_(x)active sites due to the high-efficiency substitution of Zn^(2+)ions with Fe^(3+) ions during ZIF-8 growth,the strong interaction between Fe^(3+) ions and N atoms of 2-Methylimidazole (2-MIm),and ZIF-8’s micropore confinement effect.As a result,Fe-NC(Zn^(2+)) presented high ORR activity in the entire p H range (p H=1,7,and 13).At p H=13,Fe-NC(Zn^(2+)) exhibited a half-wave potential (E1/2) of 0.95 V (vs.reversible hydrogen electrode),which was 70 m V higher than that of commercial Pt/C.More importantly,Fe-NC(Zn^(2+)) showed superior ORR stability in neutral media without performance loss after 5,000 cycles.A record-high open-circuit voltage(1.9 V) was obtained when Fe-NC(Zn^(2+)) was used as a cathodic catalyst in assembled Mg-air batteries in neutral media.The assembled liquid and all-solid Mg-air batteries with high performance indicated that Fe-NC(Zn^(2+)) has enormous potential for use in flexible and wearable Mg-air batteries.
文摘目的分析体质量指数(Body mass index,BMI)与老年慢性心力衰竭(Chronic heart failure,CHF)患者血浆胱抑素C(cystatinC,Cys-C)、N末端B型利钠肽原(N-terminal pro-B-type natriuretic peptide,NT-proBNP)水平相关性,并分析血浆Cys-C、NT-proBNP评估老年CHF患者预后价值。方法选择2021年7月—2022年10月在本院接受治疗的192例老年慢性心力衰竭(CHF)患者作为研究对象,按照BMI指数分为肥胖组(49例)、超重组(68例)和正常组(75例)三组。对比各亚组患者血浆Cys-C、NT-proBNP水平差异,采用Pearson相关性分析的方式探究老年CHF患者BMI指数与血浆Cys-C、NT-proBNP相关性,对入组患者实施12个月随访,将患者按照预后情况区分为死亡组和存活组,对比两亚组患者血浆Cys-C、NT-proBNP水平差异并评估预后评估价值。结果肥胖组患者血浆Cys-C、NT-proBNP水平高于超重组,超重组患者血浆Cys-C、NT-proBNP水平高于正常组,差异具有统计学意义(P<0.05);入组老年CHF患者的BMI指数与其血浆Cys-C、NT-proBN水平均呈现明显的正相关性(r=0.7104,P<0.0001)(r=0.6603,P<0.0001);随访12个月显示,死亡组患者的血浆Cys-C、NT-proBNP水平显著高于存活组患者,差异具有统计学意义(P<0.05);血浆Cys-C、NT-proBNP对老年CHF预后评估曲线下面积(area under curv,AUC)为0.6930(P=0.0009)、0.7982(P<0.0001)。结论老年CHF患者随BMI指数升高,血浆Cys-C、NT-proBNP水平逐渐升高,血浆Cys-C、NT-proBNP对老年CHF临床结局具有一定的预测价值,进一步研究有推广应用于老年CHF预后评估潜力。
文摘This report describes an equivalent doping profile transformation method with which the avalanche breakdown voltage of the asymmetric linearly graded junction was analytically predicted.The maximum breakdown voltage and the different depletion layer extension on the diffused side and substrate side are demonstrated in the report.The report shows the equivalent doping profile method is valid to predict the breakdown voltage of the complex P N junction.The analytical results agree with the experimental breakdown voltage in comparison with the abrupt junction and symmetric linearly graded junction approximations.
