Imidazole(IM)particles in the atmosphere affect climate,atmospheric chemical reactions,and human health.However,research on IM particles in the Sichuan Basin(SCB),one of the areas of China affected most heavily by haz...Imidazole(IM)particles in the atmosphere affect climate,atmospheric chemical reactions,and human health.However,research on IM particles in the Sichuan Basin(SCB),one of the areas of China affected most heavily by haze,remains very scarce.This study used single-particle aerosol mass spectrometry to investigate IM-containing particles in Chengdu,one of the megacities in the SCB,during summer and winter before and after implemen-tation of the Three-year Action Plan to Win the Blue-Sky Defense War(BSDW).We found that IM-containing particles accounted for 1.2%–12.0%of all detected particles,and they highly mixed with carbonaceous com-ponents,secondary inorganic species,and organic nitrogen.From before to after the BSDW,the proportion of IM-containing particles decreased by 1.8%in summer,but increased by 9.6%in winter.Ammonium/amines and carbonyl compounds were closely related to IM-containing particles;the highest proportion of IM-containing particles occurred in particles mixed with amines and carbonyls.The number fraction of IM-containing particles in all seasons was higher at night than during daytime.The potential source areas of IM-containing particles showed notable narrowing after the BSDW,and the high-value areas were found distributed closer to Chengdu and its surrounding areas.In the winter before the BSDW,most IM-containing particles(>70%)were mixed with organic carbon(OC)particles,and the contributions of OC and mixed organic–elemental carbon(OC-EC)particles increased with aggravation of pollution,whereas OC-EC and Metal particles played a more crucial role in the winter after the BSDW.展开更多
The development of efficient,cost-effective catalysts for the oxygen reduction reaction(ORR)is crucial for advancing zinc-air batteries(ZABs).This study presents Fe_(4)N nanoparticles embedded in N-doped carbon nanofi...The development of efficient,cost-effective catalysts for the oxygen reduction reaction(ORR)is crucial for advancing zinc-air batteries(ZABs).This study presents Fe_(4)N nanoparticles embedded in N-doped carbon nanofibers(Fe_(4)N@CNF-NH_(3))as a highly efficient ORR catalyst.The Fe_(4)N@CNF-NH_(3)catalyst was synthesized via electrospinning,followed by high-temperature annealing in an NH_(3)atmosphere.This electrospinning technique ensured the uniform dispersion of Fe_(4)N nanoparticles within the carbon nanofibers(CNFs),preventing agglomeration and enhancing the availability of active sites.Structural and morphological analyses confirmed the formation of Fe_(4)N nanoparticles with a lattice spacing of 0.213 nm,surrounded by graphitic carbon structures that significantly improved the material’s conductivity and stability.Electrochemical tests demonstrated that Fe_(4)N@CNF-NH_(3)exhibited superior ORR activity,with a half-wave potential of 0.904 V,surpassing that of commercial Pt/C catalysts.This enhanced performance is attributed to the synergistic effects of Fe_(4)N nanoparticles and the conductive carbon framework,which facilitated efficient charge and mass transfer during the ORR process.Density functional theory calculations further revealed that the introduction of CNFs positively shifted the d-band center of Fe atoms,optimizing oxygen intermediate adsorption and lowering energy barriers for ORR.The practical applicability of Fe_(4)N@CNF-NH_(3)was validated through the assembly of both liquid-state and solid-state ZABs,which exhibited excellent cycling stability,high power density,and superior discharge voltage.This study offers a promising strategy for developing highly active,low-cost ORR catalysts and advances the potential for the commercialization of ZABs.展开更多
针对锅炉过热汽温系统存在的大时延、强非线性和变量耦合等建模难题,建立了一种基于贝叶斯优化时间序列预测神经基扩展分析(neural basis expansion analysis for interpretable time series forecasting,N-BEATS)网络的过热汽温预测模...针对锅炉过热汽温系统存在的大时延、强非线性和变量耦合等建模难题,建立了一种基于贝叶斯优化时间序列预测神经基扩展分析(neural basis expansion analysis for interpretable time series forecasting,N-BEATS)网络的过热汽温预测模型。针对某600 MW超临界火电机组,结合机理分析确定模型的输入和输出变量,通过性能对比实验优化模型的输入/输出时延阶次、Block类型和激活函数,进一步利用贝叶斯优化算法对模型的超参数进行寻优,并与网格搜索、遗传算法的优化效果进行对比。采用该机组仿真运行数据进行建模实验,结果表明所提模型在预测精度方面优于传统优化方法及主流模型。展开更多
WC particles reinforced CoCrFeNiMo high-entropy alloy(HEA)composite coatings were prepared on Cr12MoV steel successfully by laser cladding technology to improve the wear resistance of substrates.Effect of WC content o...WC particles reinforced CoCrFeNiMo high-entropy alloy(HEA)composite coatings were prepared on Cr12MoV steel successfully by laser cladding technology to improve the wear resistance of substrates.Effect of WC content on microstructure and wear property of the composite coatings was studied in detail.Large numbers of carbides with four main types:primary carbide crystals,eutectic structures,massive crystals growing along the periphery of the remaining WC particles and incompletely fused WC particles,were found to exist in the WC/CoCrFeNiMo composite coatings.With increasing WC content,the microhardness of coatings is gradually improved while the average friction coefficients follow the opposite trend due to solid solution strengthening and second phase strengthening effect.The maximum microhardness and minimum friction coefficient are HV_(0.2)689.7 and 0.72,respectively,for the composite coating with 30 wt.%WC,the wear resistance of the substrate is improved significantly,the wear mechanisms are spalling wear and abrasive wear due to their high microhardness.展开更多
Polybrominated biphenyl ethers(PBDEs)and polycyclic aromatic hydrocarbons(PAHs)are commonly detected contaminants at e-waste recycling sites.Against the conventional wisdom that PBDEs and PAHs are highly immobile and ...Polybrominated biphenyl ethers(PBDEs)and polycyclic aromatic hydrocarbons(PAHs)are commonly detected contaminants at e-waste recycling sites.Against the conventional wisdom that PBDEs and PAHs are highly immobile and persist primarily in shallowsurface soils,increasing evidence shows that these compounds can leach into the groundwater.Herein,we compare the leachabilities of PBDEs vs.PAHs from contaminated soils collected at an e-waste recycling site in Tianjin,China.Considerable amounts of BDE-209(0.3–2 ng/L)and phenanthrene(42–106 ng/L),the most abundant PBDE and PAH at the site,are detected in the effluents of columns packed with contaminated soils,with the specific concentrations varying with hydrodynamic and solution chemistry conditions.Interestingly,the leaching potential of BDE-209 appears to be closely related to the release of colloidal mineral particles,whereas the leachability of phenanthrene correlates well with the concentration of dissolved organic carbon in the effluent,but showing essentially no correlation with the concentration of mineral particles.The surprisingly different trends of the leachability observed between BDE-209 and phenanthrene is counterintuitive,as PBDEs and PAHs often co-exist at e-waste recycling sites(particularly at the sites wherein incineration is being practiced)and share many similarities in terms of physicochemical properties.One possible explanation is that due to its extremely low solubility,BDE-209 predominantly exists in free-phase(i.e.,as solid(nano)particles),whereas the more soluble phenanthrene is mainly sorbed to soil organic matter.Findings in this study underscore the need to better understand the mobility of highly hydrophobic organic contaminants at contaminated sites for improved risk management.展开更多
Densely distributed coherent nanoparticles(DCN)in steel matrix can enhance the work-hardening ability and ductility of steel simultaneously.All the routes to this end can be generally classified into the liquid-solid ...Densely distributed coherent nanoparticles(DCN)in steel matrix can enhance the work-hardening ability and ductility of steel simultaneously.All the routes to this end can be generally classified into the liquid-solid route and the solid-solid route.However,the formation of DCN structures in steel requires long processes and complex steps.So far,obtaining steel with coherent particle enhancement in a short time remains a bottleneck,and some necessary steps remain unavoidable.Here,we show a high-efficiency liquid-phase refining process reinforced by a dynamic magnetic field.Ti-Y-Mn-O particles had an average size of around(3.53±1.21)nm and can be obtained in just around 180 s.These small nanoparticles were coherent with the matrix,implying no accumulated dislocations between the particles and the steel matrix.Our findings have a potential application for improving material machining capacity,creep resistance,and radiation resistance.展开更多
Thermodynamic modeling is still themostwidely usedmethod to characterize aerosol acidity,a critical physicochemical property of atmospheric aerosols.However,it remains unclear whether gas-aerosol partitioning should b...Thermodynamic modeling is still themostwidely usedmethod to characterize aerosol acidity,a critical physicochemical property of atmospheric aerosols.However,it remains unclear whether gas-aerosol partitioning should be incorporated when thermodynamicmodels are employed to estimate the acidity of coarse particles.In this work,field measurements were conducted at a coastal city in northern China across three seasons,and covered wide ranges of temperature,relative humidity and NH_(3) concentrations.We examined the performance of different modes of ISORROPIA-II(a widely used aerosol thermodynamic model)in estimating aerosol acidity of coarse and fine particles.The M0 mode,which incorporates gas-phase data and runs the model in the forward mode,provided reasonable estimation of aerosol acidity for coarse and fine particles.Compared to M0,the M1 mode,which runs the model in the forward mode but does not include gas-phase data,may capture the general trend of aerosol acidity but underestimates pH for both coarse and fine particles;M2,which runs the model in the reverse mode,results in large errors in estimated aerosol pH for both coarse and fine particles and should not be used for aerosol acidity calculations.However,M1 significantly underestimates liquid water contents for both fine and coarse particles,while M2 provides reliable estimation of liquid water contents.In summary,our work highlights the importance of incorporating gas-aerosol partitioning when estimating coarse particle acidity,and thus may help improve our understanding of acidity of coarse particles.展开更多
基金supported by Sichuan Science and Technology Program(No.2024NSFSC0060)the National Natural Science Foundation of China(No.U23A2030)the Basic Research Cultivation Support Plan of Southwest Jiaotong University(No.2682023ZTPY016).
文摘Imidazole(IM)particles in the atmosphere affect climate,atmospheric chemical reactions,and human health.However,research on IM particles in the Sichuan Basin(SCB),one of the areas of China affected most heavily by haze,remains very scarce.This study used single-particle aerosol mass spectrometry to investigate IM-containing particles in Chengdu,one of the megacities in the SCB,during summer and winter before and after implemen-tation of the Three-year Action Plan to Win the Blue-Sky Defense War(BSDW).We found that IM-containing particles accounted for 1.2%–12.0%of all detected particles,and they highly mixed with carbonaceous com-ponents,secondary inorganic species,and organic nitrogen.From before to after the BSDW,the proportion of IM-containing particles decreased by 1.8%in summer,but increased by 9.6%in winter.Ammonium/amines and carbonyl compounds were closely related to IM-containing particles;the highest proportion of IM-containing particles occurred in particles mixed with amines and carbonyls.The number fraction of IM-containing particles in all seasons was higher at night than during daytime.The potential source areas of IM-containing particles showed notable narrowing after the BSDW,and the high-value areas were found distributed closer to Chengdu and its surrounding areas.In the winter before the BSDW,most IM-containing particles(>70%)were mixed with organic carbon(OC)particles,and the contributions of OC and mixed organic–elemental carbon(OC-EC)particles increased with aggravation of pollution,whereas OC-EC and Metal particles played a more crucial role in the winter after the BSDW.
基金supported by the National Natural Science Foundation of China(No.11904208the Project of Shandong Province Higher Educational Science and Technology Program(No.J18KB098).
文摘The development of efficient,cost-effective catalysts for the oxygen reduction reaction(ORR)is crucial for advancing zinc-air batteries(ZABs).This study presents Fe_(4)N nanoparticles embedded in N-doped carbon nanofibers(Fe_(4)N@CNF-NH_(3))as a highly efficient ORR catalyst.The Fe_(4)N@CNF-NH_(3)catalyst was synthesized via electrospinning,followed by high-temperature annealing in an NH_(3)atmosphere.This electrospinning technique ensured the uniform dispersion of Fe_(4)N nanoparticles within the carbon nanofibers(CNFs),preventing agglomeration and enhancing the availability of active sites.Structural and morphological analyses confirmed the formation of Fe_(4)N nanoparticles with a lattice spacing of 0.213 nm,surrounded by graphitic carbon structures that significantly improved the material’s conductivity and stability.Electrochemical tests demonstrated that Fe_(4)N@CNF-NH_(3)exhibited superior ORR activity,with a half-wave potential of 0.904 V,surpassing that of commercial Pt/C catalysts.This enhanced performance is attributed to the synergistic effects of Fe_(4)N nanoparticles and the conductive carbon framework,which facilitated efficient charge and mass transfer during the ORR process.Density functional theory calculations further revealed that the introduction of CNFs positively shifted the d-band center of Fe atoms,optimizing oxygen intermediate adsorption and lowering energy barriers for ORR.The practical applicability of Fe_(4)N@CNF-NH_(3)was validated through the assembly of both liquid-state and solid-state ZABs,which exhibited excellent cycling stability,high power density,and superior discharge voltage.This study offers a promising strategy for developing highly active,low-cost ORR catalysts and advances the potential for the commercialization of ZABs.
文摘针对锅炉过热汽温系统存在的大时延、强非线性和变量耦合等建模难题,建立了一种基于贝叶斯优化时间序列预测神经基扩展分析(neural basis expansion analysis for interpretable time series forecasting,N-BEATS)网络的过热汽温预测模型。针对某600 MW超临界火电机组,结合机理分析确定模型的输入和输出变量,通过性能对比实验优化模型的输入/输出时延阶次、Block类型和激活函数,进一步利用贝叶斯优化算法对模型的超参数进行寻优,并与网格搜索、遗传算法的优化效果进行对比。采用该机组仿真运行数据进行建模实验,结果表明所提模型在预测精度方面优于传统优化方法及主流模型。
基金Project(2021YFC2801904)supported by the National Key R&D Program of ChinaProject(KY10100230067)supported by the Basic Product Innovation Research Project,China+3 种基金Projects(52271130,52305344)supported by the National Natural Science Foundation of ChinaProjects(ZR2020ME017,ZR2020QE186)supported by the Natural Science Foundation of Shandong Province,ChinaProjects(AMGM2024F11,AMGM2021F10,AMGM2023F06)supported by the Science Fund of Shandong Laboratory of Advanced Materials and Green Manufacturing at Yantai,ChinaProject(KY90200210015)supported by Leading Scientific Research Project of China National Nuclear Corporation(CNNC),China。
文摘WC particles reinforced CoCrFeNiMo high-entropy alloy(HEA)composite coatings were prepared on Cr12MoV steel successfully by laser cladding technology to improve the wear resistance of substrates.Effect of WC content on microstructure and wear property of the composite coatings was studied in detail.Large numbers of carbides with four main types:primary carbide crystals,eutectic structures,massive crystals growing along the periphery of the remaining WC particles and incompletely fused WC particles,were found to exist in the WC/CoCrFeNiMo composite coatings.With increasing WC content,the microhardness of coatings is gradually improved while the average friction coefficients follow the opposite trend due to solid solution strengthening and second phase strengthening effect.The maximum microhardness and minimum friction coefficient are HV_(0.2)689.7 and 0.72,respectively,for the composite coating with 30 wt.%WC,the wear resistance of the substrate is improved significantly,the wear mechanisms are spalling wear and abrasive wear due to their high microhardness.
基金supported by the National Key Research and Development Program of China(No.2019YFC1804202)the National Natural Science Foundation of China(Nos.22020102004 and 22125603)+1 种基金Tianjin Municipal Science and Technology Bureau(No.21JCZDJC00280)the Fundamental Research Funds for the Central Universities,and the Ministry of Education of China(No.T2017002).
文摘Polybrominated biphenyl ethers(PBDEs)and polycyclic aromatic hydrocarbons(PAHs)are commonly detected contaminants at e-waste recycling sites.Against the conventional wisdom that PBDEs and PAHs are highly immobile and persist primarily in shallowsurface soils,increasing evidence shows that these compounds can leach into the groundwater.Herein,we compare the leachabilities of PBDEs vs.PAHs from contaminated soils collected at an e-waste recycling site in Tianjin,China.Considerable amounts of BDE-209(0.3–2 ng/L)and phenanthrene(42–106 ng/L),the most abundant PBDE and PAH at the site,are detected in the effluents of columns packed with contaminated soils,with the specific concentrations varying with hydrodynamic and solution chemistry conditions.Interestingly,the leaching potential of BDE-209 appears to be closely related to the release of colloidal mineral particles,whereas the leachability of phenanthrene correlates well with the concentration of dissolved organic carbon in the effluent,but showing essentially no correlation with the concentration of mineral particles.The surprisingly different trends of the leachability observed between BDE-209 and phenanthrene is counterintuitive,as PBDEs and PAHs often co-exist at e-waste recycling sites(particularly at the sites wherein incineration is being practiced)and share many similarities in terms of physicochemical properties.One possible explanation is that due to its extremely low solubility,BDE-209 predominantly exists in free-phase(i.e.,as solid(nano)particles),whereas the more soluble phenanthrene is mainly sorbed to soil organic matter.Findings in this study underscore the need to better understand the mobility of highly hydrophobic organic contaminants at contaminated sites for improved risk management.
基金financially supported by the National Natural Science Foundation of China(No.51771125)the Sichuan Province Science and Technology Support Program(No.2020YFG0102)。
文摘Densely distributed coherent nanoparticles(DCN)in steel matrix can enhance the work-hardening ability and ductility of steel simultaneously.All the routes to this end can be generally classified into the liquid-solid route and the solid-solid route.However,the formation of DCN structures in steel requires long processes and complex steps.So far,obtaining steel with coherent particle enhancement in a short time remains a bottleneck,and some necessary steps remain unavoidable.Here,we show a high-efficiency liquid-phase refining process reinforced by a dynamic magnetic field.Ti-Y-Mn-O particles had an average size of around(3.53±1.21)nm and can be obtained in just around 180 s.These small nanoparticles were coherent with the matrix,implying no accumulated dislocations between the particles and the steel matrix.Our findings have a potential application for improving material machining capacity,creep resistance,and radiation resistance.
基金supported by the National Natural Science Foundation of China (Nos.42022050 and 42277088)the Guangdong Basic and Applied Basic Research Fund Committee (Nos.2021A1515011248 and 2023A1515012010)the Guangdong Foundation for the Program of Science and Technology Research (No.2020B1212060053).
文摘Thermodynamic modeling is still themostwidely usedmethod to characterize aerosol acidity,a critical physicochemical property of atmospheric aerosols.However,it remains unclear whether gas-aerosol partitioning should be incorporated when thermodynamicmodels are employed to estimate the acidity of coarse particles.In this work,field measurements were conducted at a coastal city in northern China across three seasons,and covered wide ranges of temperature,relative humidity and NH_(3) concentrations.We examined the performance of different modes of ISORROPIA-II(a widely used aerosol thermodynamic model)in estimating aerosol acidity of coarse and fine particles.The M0 mode,which incorporates gas-phase data and runs the model in the forward mode,provided reasonable estimation of aerosol acidity for coarse and fine particles.Compared to M0,the M1 mode,which runs the model in the forward mode but does not include gas-phase data,may capture the general trend of aerosol acidity but underestimates pH for both coarse and fine particles;M2,which runs the model in the reverse mode,results in large errors in estimated aerosol pH for both coarse and fine particles and should not be used for aerosol acidity calculations.However,M1 significantly underestimates liquid water contents for both fine and coarse particles,while M2 provides reliable estimation of liquid water contents.In summary,our work highlights the importance of incorporating gas-aerosol partitioning when estimating coarse particle acidity,and thus may help improve our understanding of acidity of coarse particles.
