An improved analytical method to determine the content of 52 major, minor and trace elements in marine geological samples, using a HF-HCl-HNO_3 acid system with a high-pressure closed digestion method(HPCD), is stud...An improved analytical method to determine the content of 52 major, minor and trace elements in marine geological samples, using a HF-HCl-HNO_3 acid system with a high-pressure closed digestion method(HPCD), is studied by an inductively coupled plasma optical emission spectrometry(ICP-OES) and an inductively coupled plasma mass spectrometry(ICP-MS). The operating parameters of the instruments are optimized, and the optimal analytical parameters are determined. The influences of optical spectrum and mass spectrum interferences, digestion methods and acid systems on the analytical results are investigated. The optimal spectral lines and isotopes are chosen, and internal standard element of rhodium is selected to compensate for matrix effects and analytical signals drifting. Compared with the methods of an electric heating plate digestion and a microwave digestion, a high-pressure closed digestion method is optimized with less acid, complete digestion,less damage for digestion process. The marine geological samples are dissolved completely by a HF-HCl-HNO_3 system, the relative error(RE) for the analytical results are all less than 6.0%. The method detection limits are 2–40μg/g by the ICP-OES, and 6–80 ng/g by ICP-MS. The methods are used to determine the marine sediment reference materials(GBW07309, GBW07311, GBW07313), rock reference materials(GBW07103, GBW07104,GBW07105), and cobalt-rich crust reference materials(GBW07337, GBW07338, GBW07339), the obtained analytical results are in agreement with the certified values, and both of the relative standard deviation(RSD) and the relative error(RE) are less than 6.0%. The analytical method meets the requirements for determining 52 elements contents of bulk marine geological samples.展开更多
The intensity-time profiles of solar proton events(SPEs) are grouped into three types in the present study. The Type-I means that the intensity-time profile of an SPE has one peak, which occurs shortly after the ass...The intensity-time profiles of solar proton events(SPEs) are grouped into three types in the present study. The Type-I means that the intensity-time profile of an SPE has one peak, which occurs shortly after the associated solar flare and coronal mass ejection(CME). The Type-II means that the SPE profile has two peaks: the first peak occurs shortly after the solar eruption, the second peak occurs at the time when the CME-driven shock reaches the Earth, and the intensity of the second peak is lower than the first one.If the intensity of the second peak is higher than the first one, or the SPE intensity increases continuously until the CME-driven shock reaches the Earth, this kind of intensity-time profile is defined as Type-III. It is found that most CMEs associated with Type-I SPEs have no geoeffectiveness and only a small part of CMEs associated with Type-I SPEs can produce minor(–50 n T ≤ Dst ≤–30 n T) or moderate geomagnetic storms(–100 n T≤ Dst ≤–50 n T), but never an intense geomagnetic storm(–200 n T ≤ Dst 〈-100 n T). However,most of the CMEs associated with Type-II and Type-III SPEs can produce intense or great geomagnetic storms(Dst ≤-200 n T). The solar wind structures responsible for the geomagnetic storms associated with SPEs with different intensity-time profiles have also been investigated and discussed.展开更多
The iron and steel production process is one of the predominant anthropogenic sources of atmospheric mercury emissions worldwide. In this study, field tests were conducted to study mercury emission characteristics and...The iron and steel production process is one of the predominant anthropogenic sources of atmospheric mercury emissions worldwide. In this study, field tests were conducted to study mercury emission characteristics and mass flows at two iron and steel plants in China. It was found that low-sulfur flue gas from sintering machines could contribute up to41% of the total atmospheric mercury emissions, and desulfurization devices could remarkably help reduce the emissions. Coal gas burning accounted for 17%–49% of the total mercury emissions, and therefore the mercury control of coal gas burning, specifically for the power plant burning coal gas to generate electricity, was significantly important. The emissions from limestone and dolomite production and electric furnaces can contribute29.3% and 4.2% of the total mercury emissions from iron and steel production. More attention should be paid to mercury emissions from these two processes. Blast furnace dust accounted for 27%–36% of the total mercury output for the whole iron and steel production process. The recycling of blast furnace dust could greatly increase the atmospheric mercury emissions and should not be conducted. The mercury emission factors for the coke oven,sintering machine and blast furnace were 0.039–0.047 g Hg/ton steel, and for the electric furnace it was 0.021 g Hg/ton steel. The predominant emission species was oxidized mercury, accounting for 59%–73% of total mercury emissions to air.展开更多
Nitrogen(N) loss from fertilization in agricultural fields has an unavoidable negative impact on the environment and a better understanding of the major pathways can assist in developing the best management practice...Nitrogen(N) loss from fertilization in agricultural fields has an unavoidable negative impact on the environment and a better understanding of the major pathways can assist in developing the best management practices. The aim of this study was to evaluate the fate of N fertilizers applied to acidic red soil(Ferralic Cambisol) after 19 years of mineral(synthetic) and manure fertilizer treatments under a cropping system with wheat-maize rotations. Five field treatments were examined: control(CK), chemical nitrogen and potash fertilizer(NK), chemical nitrogen and phosphorus fertilizer(NP), chemical nitrogen, phosphorus and potash fertilizer(NPK) and the NPK with manure(NPKM, 70% N from manure). Based on the soil total N storage change in 0–100 cm depth, ammonia(NH_3) volatilization, nitrous oxide(N_2O) emission, N plant uptake, and the potential N leaching loss were estimated using a mass balance approach. In contrast to the NPKM, all mineral fertilizer treatments(NK, NP and NPK) showed increased nitrate(NO_3~–) concentration with increasing soil depth, indicating higher leaching potential. However, total NH_3 volatilization loss was much higher in the NPKM(19.7%) than other mineral fertilizer treatments(≤4.2%). The N_2O emissions were generally low(0.2–0.9%, the highest from the NPKM). Total gaseous loss accounted for 1.7, 3.3, 5.1, and 21.9% for NK, NP, NPK, and NPKM treatments, respectively. Estimated N leaching loss from the NPKM was only about 5% of the losses from mineral fertilizer treatments. All data demonstrated that manure incorporation improved soil productivity, increased yield, and reduced potential leaching, but with significantly higher NH_3 volatilization, which could be reduced by improving the application method. This study confirms that manure incorporationis an essential strategy in N fertilization management in upland red soil cropping system.展开更多
Recently, S. W. Kahler studied the timescales of solar energetic particle (SEP) events asso- ciated with coronal mass ejections (CMEs) from analysis of spacecraft data. They obtained different timescales for SEP e...Recently, S. W. Kahler studied the timescales of solar energetic particle (SEP) events asso- ciated with coronal mass ejections (CMEs) from analysis of spacecraft data. They obtained different timescales for SEP events, such as TO, the onset time from CME launch to SEP onset, TR, the rise time from onset to half the peak intensity (0.5/p), and TD, the duration of the SEP intensity above 0.5Ip. In this work, we solve the transport equation for SEPs considering interplanetary coronal mass ejection (ICME) shocks as energetic particle sources. With our modeling assumptions, our simulations show similar results to Kahler's analysis of spacecraft data, that the weighted average of TD increases with both CME speed and width. Moreover, from our simulation results, we suggest TD is directly dependent on CME speed, but not dependent on CME width, which were not found in the analysis of observational data.展开更多
Objective:The aim of this study was to clarify the differences between the prostatic levels of chemical elements in patients with benign prostatic hyperplasia(BPH)and healthy male.Methods:We evaluated the prostatic le...Objective:The aim of this study was to clarify the differences between the prostatic levels of chemical elements in patients with benign prostatic hyperplasia(BPH)and healthy male.Methods:We evaluated the prostatic level of 66 chemical elements in 43 patients with BPH and 37 healthy males.Measurements were performed using five instrumental analytical methods.Results:In the hyperplastic prostates,we have observed a significant increase in the mean level of Bi,Cr,Hg,K,Sb,and Se accompanied a significant decrease in the mean level of Al,Ce,Cs,Dy,Er,Gd,Ho,La,Mo,Nd,Pb,Pr,Sm,Sn,Tb,Tm,U,and Y.No differences were found in the mean prostatic level of other chemical elements including Ag,Al,Au,B,Ba,Be,Br,Ca,Cd,Co,Cu,Fe,Li,Mg,Mn,Na,Nb,Ni,P,Rb,S,Sc,Si,Th,Ti,Tl,Yb,Zn,and Zr between BPH patients and healthy males.Conclusions:The finding of chemical element contents and correlation between pairs of chemical element mass fractions indicates that there is a great disturbance of prostatic chemical element metabolism in BPH gland.Trace elements Bi,Cr,Hg,K,Sb,and Se may be regarded as the possible tissue biomarkers of hyperplastic transformation of prostate gland.Obtained data did not confirm a critical role of Cd and Pb accumulation in the pathogenesis of BPH.A potential age-related Zn,Fe,and Se deficiency in the prostate tissue has not been found as being involved in the etiology of BPH.展开更多
In DMSO/water(4:1),photolysis of the dihydroxy-Sn(IV)-rnesoporphyrin dimethyl ester (SnP)/methyl viologen(MV^(2+))/ethylene diamine tetraacetic acid(EDTA)ternary system produces methyl viologen cation radical with a q...In DMSO/water(4:1),photolysis of the dihydroxy-Sn(IV)-rnesoporphyrin dimethyl ester (SnP)/methyl viologen(MV^(2+))/ethylene diamine tetraacetic acid(EDTA)ternary system produces methyl viologen cation radical with a quantum yield of 0.67,much higher than that of systems with other metal complexes of rnesoporphyrin dimethyl ester.Neither EDTA nor MV^(2+) quenches the stationary fluorescence of SnP,implying that the reaction does not take place at the singlet state.With flash photolysis we obtain the T-T absorption spectrum of SnP(λ_(max)-440 nm).By following the decay of this absorption,the triplet life time of SnP is estimated to be 41 μs.The life time is related to the concentration of either MV^(2+) or EDTA.Good linear relationships are obtained by plotting τ_0/τ vs.the concentration of MV^(2+) or EDTA(Stern-Volmer plot),from which we determine the quenching constants:k_q(MV^(2+))=5.5×10~7 mol^(-7) s^(-1);kq(EDTA)=2.7×10~7 mol^(-1),s^(-1).The data suggests that upon photolysis of the above ternary system,both oxidative quenching and reductive quenching of the triplet state of the sensitizer are occurring.From the measured phosphorescence spectrum(λ_(max) 704nm)and the ground state redox potentials (E_(1/2)^(red)~-0.84V,E_(1/2)^(ox)~ Ag/AgCl,KCl(sat.)),we obtain the redox potential of triplet SnP to be E (P^+/P)~-0.33 V, E(P/P-)~+0.92 V.Matching this data with the redox potential of MV^(2+) and EDTA,we establish the fact that during the photolysis of the SnP/MV^(2+)/EDTA ternary system,both oxidative and reductive quenching are thermodynamically favorable processes.This is also the reason why the SnP sensitized reaction is much more efficient relative to other mesoporphyrin derivatives.展开更多
In congested urban roads, cars must stop at intersections because of city traffic lights. As a result, pedestri- ans and traffic police personnel are exposed to pollutants emanating from the tailpipe of various vehicl...In congested urban roads, cars must stop at intersections because of city traffic lights. As a result, pedestri- ans and traffic police personnel are exposed to pollutants emanating from the tailpipe of various vehicles at such city trafficjunctions. In this study, various gasoline- and diesel-fueled cars complying with differ- ent emission standards were tested for their emissions in simulated city traffic junction conditions. The engine exhaust from these cars was subjected to physicochemical characterization at different engine speeds under no-load conditions. These engine conditions were chosen because the cars idle at differ- ent engine speeds at a city traffic junction. Gravimetric and real-time measurements were performed for the tailpipe exhaust sampled from these vehicles. Exhaust particles were collected on 47 mm diameter quartz filter papers and subjected to gravimetric analysis for determining the total particulate mass (TPM) and trace metals while the engines were operated at two different engine idling speeds, 1500 rpm (representing low idling) and 2500 rpm (representing high idling). At similar engine operating condi- tions, TPM and trace metals were lower for the exhaust from gasoline engines compared to the exhaust from diesel engines. Real-time measurements were performed for particle-bound poly-aromatic hydro- carbons (PAHs), particle number and size distribution, regulated gaseous emissions and smoke opacity of the exhaust at four different engine speeds, 1500, 2000, 2500, and 3000 rpm. Particle-bound PAHs showed a decreasing trend for the vehicles that complied with stricter vehicular emission standards. Higher particle peak number concentrations were observed for diesel exhausts compared to the results for gasoline exhaust. Regulated gaseous emissions were also comoared.展开更多
In order to evaluate the secondary aerosol formation potential at a suburban site of Beijing,in situ perturbation experiments in a potential aerosol mass(PAM) reactor were carried out in the winter of 2014.The varia...In order to evaluate the secondary aerosol formation potential at a suburban site of Beijing,in situ perturbation experiments in a potential aerosol mass(PAM) reactor were carried out in the winter of 2014.The variations of secondary aerosol formation as a function of time,OH exposure,and the concentrations of gas phase pollutants and particles were reported in this study.Two periods with distinct secondary aerosol formation potentials,marked as Period Ⅰ and Period Ⅱ,were identified during the observation.In Period Ⅰ,the secondary aerosol formation potential was high,and correlated well to the air pollutants,i.e.,SO2,NO2,and CO.The maximal secondary aerosol formation was observed with an aging time equivalent to about 3 days of atmospheric oxidation.In period Ⅱ,the secondary aerosol formation potential was low,with no obvious correlation with the air pollutants.Meanwhile,the aerosol mass decreased,instead of showing a peak,with increasing aging time.Backward trajectory analysis during the two periods confirmed that the air mass in Period Ⅰwas mainly from local sources,while it was attributed mostly to long distance transport in Period Ⅱ.The air lost its reactivity during the long transport and the particles became highly aged,resulting in a low secondary aerosol formation potential.Our experimental results indicated that the in situ measurement of the secondary aerosol formation potential could provide important information for evaluating the contributions of local emission and long distance transport to the aerosol pollution.展开更多
Coronal mass ejections(CMEs) and solar flares are the large-scale and most energetic eruptive phenomena in our solar system and able to release a large quantity of plasma and magnetic flux from the solar atmosphere in...Coronal mass ejections(CMEs) and solar flares are the large-scale and most energetic eruptive phenomena in our solar system and able to release a large quantity of plasma and magnetic flux from the solar atmosphere into the solar wind. When these high-speed magnetized plasmas along with the energetic particles arrive at the Earth, they may interact with the magnetosphere and ionosphere, and seriously affect the safety of human high-tech activities in outer space. The travel time of a CME to 1 AU is about 1–3 days, while energetic particles from the eruptions arrive even earlier. An efficient forecast of these phenomena therefore requires a clear detection of CMEs/flares at the stage as early as possible. To estimate the possibility of an eruption leading to a CME/flare, we need to elucidate some fundamental but elusive processes including in particular the origin and structures of CMEs/flares. Understanding these processes can not only improve the prediction of the occurrence of CMEs/flares and their effects on geospace and the heliosphere but also help understand the mass ejections and flares on other solar-type stars. The main purpose of this review is to address the origin and early structures of CMEs/flares, from multi-wavelength observational perspective. First of all, we start with the ongoing debate of whether the pre-eruptive configuration, i.e., a helical magnetic flux rope(MFR), of CMEs/flares exists before the eruption and then emphatically introduce observational manifestations of the MFR. Secondly, we elaborate on the possible formation mechanisms of the MFR through distinct ways. Thirdly, we discuss the initiation of the MFR and associated dynamics during its evolution toward the CME/flare. Finally, we come to some conclusions and put forward some prospects in the future.展开更多
基金The China Ocean Mineral Resources Research and Development Association Research Program of the State Oceanic Administration of China under contract No.DY125-13-R-07the National Natural Science Foundation of China under contract Nos 41322036 and 41230960+1 种基金the Shandong Provincial Natural Science Foundation of China under contract No.ZR2014DP009the Special Basic Research Funds for Central Public Research Institutes for The First Institute of Oceanography,State Oceanic Administration of China under contract Nos GY0213G06 and GY02-2012G35
文摘An improved analytical method to determine the content of 52 major, minor and trace elements in marine geological samples, using a HF-HCl-HNO_3 acid system with a high-pressure closed digestion method(HPCD), is studied by an inductively coupled plasma optical emission spectrometry(ICP-OES) and an inductively coupled plasma mass spectrometry(ICP-MS). The operating parameters of the instruments are optimized, and the optimal analytical parameters are determined. The influences of optical spectrum and mass spectrum interferences, digestion methods and acid systems on the analytical results are investigated. The optimal spectral lines and isotopes are chosen, and internal standard element of rhodium is selected to compensate for matrix effects and analytical signals drifting. Compared with the methods of an electric heating plate digestion and a microwave digestion, a high-pressure closed digestion method is optimized with less acid, complete digestion,less damage for digestion process. The marine geological samples are dissolved completely by a HF-HCl-HNO_3 system, the relative error(RE) for the analytical results are all less than 6.0%. The method detection limits are 2–40μg/g by the ICP-OES, and 6–80 ng/g by ICP-MS. The methods are used to determine the marine sediment reference materials(GBW07309, GBW07311, GBW07313), rock reference materials(GBW07103, GBW07104,GBW07105), and cobalt-rich crust reference materials(GBW07337, GBW07338, GBW07339), the obtained analytical results are in agreement with the certified values, and both of the relative standard deviation(RSD) and the relative error(RE) are less than 6.0%. The analytical method meets the requirements for determining 52 elements contents of bulk marine geological samples.
基金supported by the National Basic Research Program of China (973 Program,Grant No.2012CB957801)the National Natural Science Foundation of China (Grant Nos.41074132,41274193,41674166,41031064 and 11303017)+1 种基金the National Standard Research Program (Grant No.200710123)the project 985 of Nanjing University,the Advanced Discipline Construction Project of Jiangsu Province and the NKBRSF (Grant No.2014CB744203)
文摘The intensity-time profiles of solar proton events(SPEs) are grouped into three types in the present study. The Type-I means that the intensity-time profile of an SPE has one peak, which occurs shortly after the associated solar flare and coronal mass ejection(CME). The Type-II means that the SPE profile has two peaks: the first peak occurs shortly after the solar eruption, the second peak occurs at the time when the CME-driven shock reaches the Earth, and the intensity of the second peak is lower than the first one.If the intensity of the second peak is higher than the first one, or the SPE intensity increases continuously until the CME-driven shock reaches the Earth, this kind of intensity-time profile is defined as Type-III. It is found that most CMEs associated with Type-I SPEs have no geoeffectiveness and only a small part of CMEs associated with Type-I SPEs can produce minor(–50 n T ≤ Dst ≤–30 n T) or moderate geomagnetic storms(–100 n T≤ Dst ≤–50 n T), but never an intense geomagnetic storm(–200 n T ≤ Dst 〈-100 n T). However,most of the CMEs associated with Type-II and Type-III SPEs can produce intense or great geomagnetic storms(Dst ≤-200 n T). The solar wind structures responsible for the geomagnetic storms associated with SPEs with different intensity-time profiles have also been investigated and discussed.
基金supported by the Major State Basic Research Development Program of China (973 Program) (No. 2013CB430001)the Natural Science Foundation of China (No. 21077065)
文摘The iron and steel production process is one of the predominant anthropogenic sources of atmospheric mercury emissions worldwide. In this study, field tests were conducted to study mercury emission characteristics and mass flows at two iron and steel plants in China. It was found that low-sulfur flue gas from sintering machines could contribute up to41% of the total atmospheric mercury emissions, and desulfurization devices could remarkably help reduce the emissions. Coal gas burning accounted for 17%–49% of the total mercury emissions, and therefore the mercury control of coal gas burning, specifically for the power plant burning coal gas to generate electricity, was significantly important. The emissions from limestone and dolomite production and electric furnaces can contribute29.3% and 4.2% of the total mercury emissions from iron and steel production. More attention should be paid to mercury emissions from these two processes. Blast furnace dust accounted for 27%–36% of the total mercury output for the whole iron and steel production process. The recycling of blast furnace dust could greatly increase the atmospheric mercury emissions and should not be conducted. The mercury emission factors for the coke oven,sintering machine and blast furnace were 0.039–0.047 g Hg/ton steel, and for the electric furnace it was 0.021 g Hg/ton steel. The predominant emission species was oxidized mercury, accounting for 59%–73% of total mercury emissions to air.
基金supported by the National Key Research and Development Program of China(2016YFD0200301)the open fund of Key Laboratory of Non-point Source Pollution Control,Ministry of Agriculture,China(20130104)the Key Technologies R&D Program of China during the 12th Five-year Plan period(2012BAD14B04)
文摘Nitrogen(N) loss from fertilization in agricultural fields has an unavoidable negative impact on the environment and a better understanding of the major pathways can assist in developing the best management practices. The aim of this study was to evaluate the fate of N fertilizers applied to acidic red soil(Ferralic Cambisol) after 19 years of mineral(synthetic) and manure fertilizer treatments under a cropping system with wheat-maize rotations. Five field treatments were examined: control(CK), chemical nitrogen and potash fertilizer(NK), chemical nitrogen and phosphorus fertilizer(NP), chemical nitrogen, phosphorus and potash fertilizer(NPK) and the NPK with manure(NPKM, 70% N from manure). Based on the soil total N storage change in 0–100 cm depth, ammonia(NH_3) volatilization, nitrous oxide(N_2O) emission, N plant uptake, and the potential N leaching loss were estimated using a mass balance approach. In contrast to the NPKM, all mineral fertilizer treatments(NK, NP and NPK) showed increased nitrate(NO_3~–) concentration with increasing soil depth, indicating higher leaching potential. However, total NH_3 volatilization loss was much higher in the NPKM(19.7%) than other mineral fertilizer treatments(≤4.2%). The N_2O emissions were generally low(0.2–0.9%, the highest from the NPKM). Total gaseous loss accounted for 1.7, 3.3, 5.1, and 21.9% for NK, NP, NPK, and NPKM treatments, respectively. Estimated N leaching loss from the NPKM was only about 5% of the losses from mineral fertilizer treatments. All data demonstrated that manure incorporation improved soil productivity, increased yield, and reduced potential leaching, but with significantly higher NH_3 volatilization, which could be reduced by improving the application method. This study confirms that manure incorporationis an essential strategy in N fertilization management in upland red soil cropping system.
基金partly supported by the National Natural Science Foundation of China(Grant Nos.41304135,41574172,41374177 and 41125016)the CMA(Grant GYHY201106011)the Specialized Research Fund for State Key Laboratories of China
文摘Recently, S. W. Kahler studied the timescales of solar energetic particle (SEP) events asso- ciated with coronal mass ejections (CMEs) from analysis of spacecraft data. They obtained different timescales for SEP events, such as TO, the onset time from CME launch to SEP onset, TR, the rise time from onset to half the peak intensity (0.5/p), and TD, the duration of the SEP intensity above 0.5Ip. In this work, we solve the transport equation for SEPs considering interplanetary coronal mass ejection (ICME) shocks as energetic particle sources. With our modeling assumptions, our simulations show similar results to Kahler's analysis of spacecraft data, that the weighted average of TD increases with both CME speed and width. Moreover, from our simulation results, we suggest TD is directly dependent on CME speed, but not dependent on CME width, which were not found in the analysis of observational data.
文摘Objective:The aim of this study was to clarify the differences between the prostatic levels of chemical elements in patients with benign prostatic hyperplasia(BPH)and healthy male.Methods:We evaluated the prostatic level of 66 chemical elements in 43 patients with BPH and 37 healthy males.Measurements were performed using five instrumental analytical methods.Results:In the hyperplastic prostates,we have observed a significant increase in the mean level of Bi,Cr,Hg,K,Sb,and Se accompanied a significant decrease in the mean level of Al,Ce,Cs,Dy,Er,Gd,Ho,La,Mo,Nd,Pb,Pr,Sm,Sn,Tb,Tm,U,and Y.No differences were found in the mean prostatic level of other chemical elements including Ag,Al,Au,B,Ba,Be,Br,Ca,Cd,Co,Cu,Fe,Li,Mg,Mn,Na,Nb,Ni,P,Rb,S,Sc,Si,Th,Ti,Tl,Yb,Zn,and Zr between BPH patients and healthy males.Conclusions:The finding of chemical element contents and correlation between pairs of chemical element mass fractions indicates that there is a great disturbance of prostatic chemical element metabolism in BPH gland.Trace elements Bi,Cr,Hg,K,Sb,and Se may be regarded as the possible tissue biomarkers of hyperplastic transformation of prostate gland.Obtained data did not confirm a critical role of Cd and Pb accumulation in the pathogenesis of BPH.A potential age-related Zn,Fe,and Se deficiency in the prostate tissue has not been found as being involved in the etiology of BPH.
文摘In DMSO/water(4:1),photolysis of the dihydroxy-Sn(IV)-rnesoporphyrin dimethyl ester (SnP)/methyl viologen(MV^(2+))/ethylene diamine tetraacetic acid(EDTA)ternary system produces methyl viologen cation radical with a quantum yield of 0.67,much higher than that of systems with other metal complexes of rnesoporphyrin dimethyl ester.Neither EDTA nor MV^(2+) quenches the stationary fluorescence of SnP,implying that the reaction does not take place at the singlet state.With flash photolysis we obtain the T-T absorption spectrum of SnP(λ_(max)-440 nm).By following the decay of this absorption,the triplet life time of SnP is estimated to be 41 μs.The life time is related to the concentration of either MV^(2+) or EDTA.Good linear relationships are obtained by plotting τ_0/τ vs.the concentration of MV^(2+) or EDTA(Stern-Volmer plot),from which we determine the quenching constants:k_q(MV^(2+))=5.5×10~7 mol^(-7) s^(-1);kq(EDTA)=2.7×10~7 mol^(-1),s^(-1).The data suggests that upon photolysis of the above ternary system,both oxidative quenching and reductive quenching of the triplet state of the sensitizer are occurring.From the measured phosphorescence spectrum(λ_(max) 704nm)and the ground state redox potentials (E_(1/2)^(red)~-0.84V,E_(1/2)^(ox)~ Ag/AgCl,KCl(sat.)),we obtain the redox potential of triplet SnP to be E (P^+/P)~-0.33 V, E(P/P-)~+0.92 V.Matching this data with the redox potential of MV^(2+) and EDTA,we establish the fact that during the photolysis of the SnP/MV^(2+)/EDTA ternary system,both oxidative and reductive quenching are thermodynamically favorable processes.This is also the reason why the SnP sensitized reaction is much more efficient relative to other mesoporphyrin derivatives.
文摘In congested urban roads, cars must stop at intersections because of city traffic lights. As a result, pedestri- ans and traffic police personnel are exposed to pollutants emanating from the tailpipe of various vehicles at such city trafficjunctions. In this study, various gasoline- and diesel-fueled cars complying with differ- ent emission standards were tested for their emissions in simulated city traffic junction conditions. The engine exhaust from these cars was subjected to physicochemical characterization at different engine speeds under no-load conditions. These engine conditions were chosen because the cars idle at differ- ent engine speeds at a city traffic junction. Gravimetric and real-time measurements were performed for the tailpipe exhaust sampled from these vehicles. Exhaust particles were collected on 47 mm diameter quartz filter papers and subjected to gravimetric analysis for determining the total particulate mass (TPM) and trace metals while the engines were operated at two different engine idling speeds, 1500 rpm (representing low idling) and 2500 rpm (representing high idling). At similar engine operating condi- tions, TPM and trace metals were lower for the exhaust from gasoline engines compared to the exhaust from diesel engines. Real-time measurements were performed for particle-bound poly-aromatic hydro- carbons (PAHs), particle number and size distribution, regulated gaseous emissions and smoke opacity of the exhaust at four different engine speeds, 1500, 2000, 2500, and 3000 rpm. Particle-bound PAHs showed a decreasing trend for the vehicles that complied with stricter vehicular emission standards. Higher particle peak number concentrations were observed for diesel exhausts compared to the results for gasoline exhaust. Regulated gaseous emissions were also comoared.
基金supported by the Key Research Program of Chinese Academy of Sciences (No. KJZD-EW-TZ-G06-01-15)the National Natural Science Foundation of China (No. 21407158)the Strategic Priority Research Program (B) of the Chinese Academy of Sciences (No. XDB05010300)
文摘In order to evaluate the secondary aerosol formation potential at a suburban site of Beijing,in situ perturbation experiments in a potential aerosol mass(PAM) reactor were carried out in the winter of 2014.The variations of secondary aerosol formation as a function of time,OH exposure,and the concentrations of gas phase pollutants and particles were reported in this study.Two periods with distinct secondary aerosol formation potentials,marked as Period Ⅰ and Period Ⅱ,were identified during the observation.In Period Ⅰ,the secondary aerosol formation potential was high,and correlated well to the air pollutants,i.e.,SO2,NO2,and CO.The maximal secondary aerosol formation was observed with an aging time equivalent to about 3 days of atmospheric oxidation.In period Ⅱ,the secondary aerosol formation potential was low,with no obvious correlation with the air pollutants.Meanwhile,the aerosol mass decreased,instead of showing a peak,with increasing aging time.Backward trajectory analysis during the two periods confirmed that the air mass in Period Ⅰwas mainly from local sources,while it was attributed mostly to long distance transport in Period Ⅱ.The air lost its reactivity during the long transport and the particles became highly aged,resulting in a low secondary aerosol formation potential.Our experimental results indicated that the in situ measurement of the secondary aerosol formation potential could provide important information for evaluating the contributions of local emission and long distance transport to the aerosol pollution.
基金supported by the Fundamental Research Funds for the Central Universitiesthe National Natural Science Foundation of China (Grant Nos. 11303016, 11373023, 11533005, 11203014)National Key Basic Research Special Foundation (Grant No. 2014CB744203)
文摘Coronal mass ejections(CMEs) and solar flares are the large-scale and most energetic eruptive phenomena in our solar system and able to release a large quantity of plasma and magnetic flux from the solar atmosphere into the solar wind. When these high-speed magnetized plasmas along with the energetic particles arrive at the Earth, they may interact with the magnetosphere and ionosphere, and seriously affect the safety of human high-tech activities in outer space. The travel time of a CME to 1 AU is about 1–3 days, while energetic particles from the eruptions arrive even earlier. An efficient forecast of these phenomena therefore requires a clear detection of CMEs/flares at the stage as early as possible. To estimate the possibility of an eruption leading to a CME/flare, we need to elucidate some fundamental but elusive processes including in particular the origin and structures of CMEs/flares. Understanding these processes can not only improve the prediction of the occurrence of CMEs/flares and their effects on geospace and the heliosphere but also help understand the mass ejections and flares on other solar-type stars. The main purpose of this review is to address the origin and early structures of CMEs/flares, from multi-wavelength observational perspective. First of all, we start with the ongoing debate of whether the pre-eruptive configuration, i.e., a helical magnetic flux rope(MFR), of CMEs/flares exists before the eruption and then emphatically introduce observational manifestations of the MFR. Secondly, we elaborate on the possible formation mechanisms of the MFR through distinct ways. Thirdly, we discuss the initiation of the MFR and associated dynamics during its evolution toward the CME/flare. Finally, we come to some conclusions and put forward some prospects in the future.