Heterogeneous reactions of NO2 on different surfaces play an important role in atmospheric NOxremoval and HONO formation,having profound impacts on photochemistry in polluted urban areas.Previous studies have suggeste...Heterogeneous reactions of NO2 on different surfaces play an important role in atmospheric NOxremoval and HONO formation,having profound impacts on photochemistry in polluted urban areas.Previous studies have suggested that the NO2 uptake on the ground or aerosol surfaces could be a dominant source for elevated HONO during the daytime.However,the uptake behavior of NO2 varies with different surfaces,and different uptake coefficients were used or derived in different studies.To obtain a more holistic picture of heterogeneous NO2 uptake on different surfaces,a series of laboratory experiments using different flow tube reactors was conducted,and the NO2 uptake coefficients(γ)were determined on inorganic particles,sea water and urban grime.The results showed that heterogeneous reactions on those surfaces were generally weak in dark conditions,with the measuredγvaried from<10-8 to 3.2×10-7 under different humidity.A photo-enhanced uptake of NO2 on urban grime was observed,with the obvious formation of HONO and NO from the heterogeneous reaction.The photo-enhancedγwas measured to be 1.9×10-6 at 5%relative humidity(RH)and 5.8×10-6 at 70%RH on urban grime,showing a positive RH dependence for both NO2 uptake and HONO formation.The results demonstrate an important role of urban grime in the daytime NO2-to-HONO conversion,and could be helpful to explain the unknown daytime HONO source in the polluted urban area.展开更多
The heterogeneous uptake processes of hydrogen peroxide on Arizona test dust and two types of authentic Chinese mineral dusts, i.e., Inner Mongolia desert dust and Xinjiang calciferous dust, were investigated using a ...The heterogeneous uptake processes of hydrogen peroxide on Arizona test dust and two types of authentic Chinese mineral dusts, i.e., Inner Mongolia desert dust and Xinjiang calciferous dust, were investigated using a Knudsen cell reactor coupled with a quadrupole mass spectrometer. The uptake coefficients were measured as a function of the initial concentration of H_2O_2 from 2.6 × 10^(11) to 1.2 × 10^(12)molecules/cm^3, and the temperature dependence of the uptake coefficients was investigated over a range from 253 to 313 K. The concentration of H_2O_2 showed little effect on the uptake coefficients of these heterogeneous processes. As a function of temperature, the initial uptake coefficients decrease with increasing temperature, whereas the steady state uptake coefficients of Arizona test dust and Inner Mongolia desert dust increase with increasing temperature. Implications for the understanding of the uptake processes onto mineral dust samples were also discussed.展开更多
In this study, the temperature dependence of the heterogeneous uptake of acrylic acid on Arizona test dust (ATD) has been investigated within a temperature range of 255-315 K using a Knudsen cell reactor. Combined w...In this study, the temperature dependence of the heterogeneous uptake of acrylic acid on Arizona test dust (ATD) has been investigated within a temperature range of 255-315 K using a Knudsen cell reactor. Combined with diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) experiment, it was found that acrylic acid could adsorb on ATD via surface OH groups and convert to carboxylate on the particle surface. The kinetics study suggests that the initial true uptake coefficient (yt) of acrylic acid on ATD decreases from (4.02 ± 0.12) x 10-5 to (1.73 ± 0.05) x 10-5 with a temperature increase from 255 to 315 K. According to the temperature dependence of uptake coefficients, the enthalpy (AHobs) and entropy (ASobs) of uptake processes were determined to be -(9.60± 0.38) KJ/mol and -(121.55 ± 1.33) l.K/mol, respectively. The activation energy for desorption (Edes) was calculated to be (14.57 ± 0.60) KJ/mol. These results indicated that the heterogeneous uptake of acrylic acid on ATD surface was sensitive to temperature. The heterogeneous uptake on ATD could affect the concentration of acrylic acid in the atmosphere, especially at low temperature.展开更多
Rare-earth Sm^(3+)-doped Pb(Mg_(1/3)Nb_(2/3))O_(3)-0.25PbTiO_(3)(PMN-0.25PT)ferroelectric ceramics with doping amounts between 0%-3%were developed via a conventional solid-state method.The doping effect of Sm^(3+)ions...Rare-earth Sm^(3+)-doped Pb(Mg_(1/3)Nb_(2/3))O_(3)-0.25PbTiO_(3)(PMN-0.25PT)ferroelectric ceramics with doping amounts between 0%-3%were developed via a conventional solid-state method.The doping effect of Sm^(3+)ions on the PMN-0.25PT matrix was systematically investigated on the basis of the phase structure,temperature-dependent dielectric,ferroelectric,and electrotechnical properties.Due to the disruption of long-range ferroelectric order,the addition of Sm^(3+)ions effectively lowers the Tm(temperature corresponding to maximum permittivity)of the samples,leading to enhanced relaxor ferroelectric(RFE)characteristic and superior electric field-induced strain(electrostrain)properties at room temperature.Intriguingly,a considerable large-signal equivalent piezoelectric coefficient d∗_(33)of 2376 pm/V and a very small hysteresis were attained in the PMN-0.25PT component doped with 2.5 mol.%Sm^(3+).The findings of piezoelectric force microscopy indicate that the addition of Sm^(3+)increases the local structural heterogeneity of the PMN-0.25PT matrix and that the enhanced electromechanical performance is due to the dynamic behavior of polar nanoregions.Importantly,strong temperature-dependent electrostrain and electrostrictive coefficient Q33 are observed in the critical region around Tm in all Sm^(3+)-modified PMN-0.25PT ceramic samples studied.This work elucidates the phase transition behavior of Sm^(3+)-doped PMN-0.25PT and reveals a critical region where electrostrictive properties can be greatly improved due to a strong temperature-dependent characteristic.展开更多
For land seismic surveys, the surface waves are the dominant noises that mask the effective signals on seismograms.The conventional methods isolate surface waves from the effective signals by the differences in freque...For land seismic surveys, the surface waves are the dominant noises that mask the effective signals on seismograms.The conventional methods isolate surface waves from the effective signals by the differences in frequencies or apparent velocities,but may not perform well when these differences are not obvious. Since the original seismic interferometry can only predict inter-receiver surface waves, we propose the use of super-virtual interferometry(SVI), which is a totally data-driven method, to predict shot-to-receiver surface waves, since this method relieves the limitation that a real shot should collocate with one of the receivers for adaptive subtraction. We further develop the adaptive weighted SVI(AWSVI) to improve the prediction of dispersive surface waves, which may be generated from heterogeneous media at the near surface. Numerical examples demonstrate the effectiveness of AWSVI to predict dispersive surface waves and its applicability to the complex near surface. The application of AWSVI on the field data from a land survey in the east of China improves the suppression of the residual surface waves compared to the conventional methods.展开更多
基金supported by the French National Research Agency/Research Grants Council of Hong Kong Special Administrative Region,China(ANR/RGC)Joint Research Scheme(project A-PolyU502/16-SEAM)National Natural Science Foundation of China(Nos.91744204,91844301)+1 种基金the Research Grants Council of Hong Kong Special Administrative Region,China(Nos.T24/504/17,15265516,C5022-14G)。
文摘Heterogeneous reactions of NO2 on different surfaces play an important role in atmospheric NOxremoval and HONO formation,having profound impacts on photochemistry in polluted urban areas.Previous studies have suggested that the NO2 uptake on the ground or aerosol surfaces could be a dominant source for elevated HONO during the daytime.However,the uptake behavior of NO2 varies with different surfaces,and different uptake coefficients were used or derived in different studies.To obtain a more holistic picture of heterogeneous NO2 uptake on different surfaces,a series of laboratory experiments using different flow tube reactors was conducted,and the NO2 uptake coefficients(γ)were determined on inorganic particles,sea water and urban grime.The results showed that heterogeneous reactions on those surfaces were generally weak in dark conditions,with the measuredγvaried from<10-8 to 3.2×10-7 under different humidity.A photo-enhanced uptake of NO2 on urban grime was observed,with the obvious formation of HONO and NO from the heterogeneous reaction.The photo-enhancedγwas measured to be 1.9×10-6 at 5%relative humidity(RH)and 5.8×10-6 at 70%RH on urban grime,showing a positive RH dependence for both NO2 uptake and HONO formation.The results demonstrate an important role of urban grime in the daytime NO2-to-HONO conversion,and could be helpful to explain the unknown daytime HONO source in the polluted urban area.
基金supported by the Strategic Priority Research Program (B) of the Chinese Academy of Sciences (No.XDB05010400)the National Basic Research Program of China (973 Program) (No.2011CB403401) of Ministry of Science and Technology of China,the National Natural Science Foundation of China (Nos.41173112,21477134)
文摘The heterogeneous uptake processes of hydrogen peroxide on Arizona test dust and two types of authentic Chinese mineral dusts, i.e., Inner Mongolia desert dust and Xinjiang calciferous dust, were investigated using a Knudsen cell reactor coupled with a quadrupole mass spectrometer. The uptake coefficients were measured as a function of the initial concentration of H_2O_2 from 2.6 × 10^(11) to 1.2 × 10^(12)molecules/cm^3, and the temperature dependence of the uptake coefficients was investigated over a range from 253 to 313 K. The concentration of H_2O_2 showed little effect on the uptake coefficients of these heterogeneous processes. As a function of temperature, the initial uptake coefficients decrease with increasing temperature, whereas the steady state uptake coefficients of Arizona test dust and Inner Mongolia desert dust increase with increasing temperature. Implications for the understanding of the uptake processes onto mineral dust samples were also discussed.
基金supported by the National Natural Science Foundation of China(Nos.41405118 and 91544227)the Strategic Priority Research Program(B)of the Chinese Academy of Sciences(No.XDB05010400)+1 种基金the National Key Technology Support Plan Projects(No.2014BAC16B01)the Basic Scientific Research Progress of the Chinese Academy of Meteorological Sciences(No.2014Y007)
文摘In this study, the temperature dependence of the heterogeneous uptake of acrylic acid on Arizona test dust (ATD) has been investigated within a temperature range of 255-315 K using a Knudsen cell reactor. Combined with diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) experiment, it was found that acrylic acid could adsorb on ATD via surface OH groups and convert to carboxylate on the particle surface. The kinetics study suggests that the initial true uptake coefficient (yt) of acrylic acid on ATD decreases from (4.02 ± 0.12) x 10-5 to (1.73 ± 0.05) x 10-5 with a temperature increase from 255 to 315 K. According to the temperature dependence of uptake coefficients, the enthalpy (AHobs) and entropy (ASobs) of uptake processes were determined to be -(9.60± 0.38) KJ/mol and -(121.55 ± 1.33) l.K/mol, respectively. The activation energy for desorption (Edes) was calculated to be (14.57 ± 0.60) KJ/mol. These results indicated that the heterogeneous uptake of acrylic acid on ATD surface was sensitive to temperature. The heterogeneous uptake on ATD could affect the concentration of acrylic acid in the atmosphere, especially at low temperature.
基金the National Natural Science Foundation of China(Grant No.52261135548)the Key Research and Development Program of Shaanxi(Program No.2022KWZ-22)+3 种基金the National Key Research and Development Program of China(Grant Nos.2021YFE0115000 and 2021YFB3800602)Russian Science Foundation(Project No.23-42-00116)the Ural Center for Shared Use“Modern nanotechnology”Ural Federal University(Reg.No.2968)which is supported by the Ministry of Science and Higher Education RF(Project No.075-15-2021-677)was used.The SEM work was done at International Center for Dielectric Research(ICDR),Xi’an Jiaotong University,Xi’an,China.
文摘Rare-earth Sm^(3+)-doped Pb(Mg_(1/3)Nb_(2/3))O_(3)-0.25PbTiO_(3)(PMN-0.25PT)ferroelectric ceramics with doping amounts between 0%-3%were developed via a conventional solid-state method.The doping effect of Sm^(3+)ions on the PMN-0.25PT matrix was systematically investigated on the basis of the phase structure,temperature-dependent dielectric,ferroelectric,and electrotechnical properties.Due to the disruption of long-range ferroelectric order,the addition of Sm^(3+)ions effectively lowers the Tm(temperature corresponding to maximum permittivity)of the samples,leading to enhanced relaxor ferroelectric(RFE)characteristic and superior electric field-induced strain(electrostrain)properties at room temperature.Intriguingly,a considerable large-signal equivalent piezoelectric coefficient d∗_(33)of 2376 pm/V and a very small hysteresis were attained in the PMN-0.25PT component doped with 2.5 mol.%Sm^(3+).The findings of piezoelectric force microscopy indicate that the addition of Sm^(3+)increases the local structural heterogeneity of the PMN-0.25PT matrix and that the enhanced electromechanical performance is due to the dynamic behavior of polar nanoregions.Importantly,strong temperature-dependent electrostrain and electrostrictive coefficient Q33 are observed in the critical region around Tm in all Sm^(3+)-modified PMN-0.25PT ceramic samples studied.This work elucidates the phase transition behavior of Sm^(3+)-doped PMN-0.25PT and reveals a critical region where electrostrictive properties can be greatly improved due to a strong temperature-dependent characteristic.
基金supported by the National Basic Research Program of China (Grant No. 2013CB228602)the National Science and Technology Major Project of China (Grant No. 2016ZX05004003-002)the National High Technology Research and Development Program of China (Grant No. 2013AA064202)
文摘For land seismic surveys, the surface waves are the dominant noises that mask the effective signals on seismograms.The conventional methods isolate surface waves from the effective signals by the differences in frequencies or apparent velocities,but may not perform well when these differences are not obvious. Since the original seismic interferometry can only predict inter-receiver surface waves, we propose the use of super-virtual interferometry(SVI), which is a totally data-driven method, to predict shot-to-receiver surface waves, since this method relieves the limitation that a real shot should collocate with one of the receivers for adaptive subtraction. We further develop the adaptive weighted SVI(AWSVI) to improve the prediction of dispersive surface waves, which may be generated from heterogeneous media at the near surface. Numerical examples demonstrate the effectiveness of AWSVI to predict dispersive surface waves and its applicability to the complex near surface. The application of AWSVI on the field data from a land survey in the east of China improves the suppression of the residual surface waves compared to the conventional methods.