It is proved that the chemical reaction induced by femtosecond laser filament in the atmosphere produces CO,HCN,and NO,and the production CO and HCN are observed for the first time.The concentrations of the products a...It is proved that the chemical reaction induced by femtosecond laser filament in the atmosphere produces CO,HCN,and NO,and the production CO and HCN are observed for the first time.The concentrations of the products are measured by mid-infrared tunable laser absorption spectroscopy.In the reduced pressure air,the decomposition of CO_(2) is enhanced by vibration excitation induced by laser filament,resulting in the enhanced production of CO and HCN.At the same time,the CO and HCN generated from the atmosphere suffer rotation excitation induced by laser filament,enhancing their absorption spectra.It is found that NO,CO,and HCN accumulate to 134 ppm,80 ppm,and 1.6 ppm in sealed air after sufficient reaction time.The atmospheric chemical reaction induced by laser filament opens the way to changing the air composition while maintaining environmental benefits.展开更多
In order to investigate the atmospheric oxidation processes and the formation of secondary organic aerosol (SOA), an indoor environmental reaction smog chamber are constructed and characterized. The system consists ...In order to investigate the atmospheric oxidation processes and the formation of secondary organic aerosol (SOA), an indoor environmental reaction smog chamber are constructed and characterized. The system consists of the collapsible ~830 L FEP Teflon film main reactor, in which the atmospheric chemical reactions take place and the formation of SOA occurs under the simulated atmospheric conditions, and the diverse on-line gas- and particle-phase instrumentation, such as the proton transfer reaction mass spectrometer, the synchrotron radiation photoionization mass spectrometer, the aerosol laser time-of-flight mass spectrometer, and other traditional commercial instruments. The initial characterization experiments are described, concerning the temperature and ultraviolet light intensity, the reactivity of the pure air, the wall loss rates of gaseous compounds and particulate matter. And the initial evaluation experiments for SOA yields from the ozonolysis of α-pinene and for mass spectra of the products resulting from the photooxidation of OH initiated isoprene are also presented, which indicate the applicability of this facility on the studies of gas-phase chemical mechanisms as well as the formation of SOA expected in the atmosphere.展开更多
As an important precursor of hydroxyl radical, nitrous acid (HONO) plays a key role in the chemistry of the lower atmosphere. Recent atmospheric measurements and model calculations show strong enhancement for HONO f...As an important precursor of hydroxyl radical, nitrous acid (HONO) plays a key role in the chemistry of the lower atmosphere. Recent atmospheric measurements and model calculations show strong enhancement for HONO formation during daytime, while they are inconsistent with the known sources in the atmosphere, suggesting that current models are lacking important sources for HONO. In this article, heterogeneous photochemical reactions of nitric acid/nitrate anion and nitrogen oxide on various aerosols were reviewed and their potential contribution to HONO formation was also discussed. It is demonstrated that HONO can be formed by photochemical reaction on surfaces with deposited HNO3 , by photocatalytic reaction of NO2 on TiO2 or TiO2 -containing materials, and by photochemical reaction of NO2 on soot, humic acids or other photosensitized organic surfaces. Although significant uncertainties still exist in the exact mechanisms and the yield of HONO, these additional sources might explain daytime observations in the atmosphere.展开更多
In this article, the NO3 radical-initiated atmospheric oxidation degradation of DDT was theoretically investigated using molecular orbital theory calculations. All the calculations of intermediates, transition states ...In this article, the NO3 radical-initiated atmospheric oxidation degradation of DDT was theoretically investigated using molecular orbital theory calculations. All the calculations of intermediates, transition states and products were performed at the MPWB1K/6-311+G(3df,2p)//MPWB1K/6- 31+G(d,p) level of theory. Several energetically favorable reaction pathways were revealed. The formation mechanisms of secondary pollutants were presented and discussed. The rate constants were deduced over the temperature range of 273-333 K using canonical variational transition-state (CVT) theory with the small curvature tunneling (SCT) method. Our study shows that H abstraction from the alkyl group and NO3 addition to the Ca atom of the benzene ring are the dominant reaction pathways. The rate-temperature formula of the overall rate constants is k(T)(DDT+NO3) = (7.21 ~ 10-15)exp(-153.81/T) cm3/(mol.sec) over the possible atmospheric temperature range of 273-333 K. The atmospheric lifetime of DDT determined by NO3 radical is about 52.5 days, which indicates that it can be degraded in the gas phase within several months.展开更多
To explore the effect of biochar on alleviating plant drought stress after being applied to soil,we prepared biochar using rice straw as raw material according to different pyrolysis temperatures(400,600 and 800°...To explore the effect of biochar on alleviating plant drought stress after being applied to soil,we prepared biochar using rice straw as raw material according to different pyrolysis temperatures(400,600 and 800°C)and reaction atmosphere(CO_(2)and N_(2)).The effect of different pyrolysis conditions on the water retention performance of biochar was studied.The early high water-retaining biochar materials were selected and wheat seeds were selected for the verification experiment of returning to the field in pots.Biochar with high porosity(specific surface area and total pore volume)and more surface hydrophilic functional groups(mainly-OH and-COOH)can indeed improve soil water retention performance.It is mainly reflected in the increase in the dry weight and fresh weight of wheat and the soil moisture content in the treatment group with the addition of biochar water retention agent.Among them,the growth rates of fresh weight and dry weight of wheat in the C800 treatment group were 11.51%and 10.64%,and the soil moisture content increased by 1.89%.It is worth noting that the application of biochar cannot completely alleviate the impact of drought stress on plants,but it can reduce the amount of water irrigation to a certain extent.Considering the quality of biochar,the biochar material(C800)prepared under the pyrolysis temperature of 800°C and the reaction atmosphere of CO_(2)has high water retention performance.展开更多
During fluidized bed gasification,sulfur in coal will be released,which will lead to environmental pollution.The release behavior of sulfur in fluidized bed gasification has not been fully studied,although fluidized b...During fluidized bed gasification,sulfur in coal will be released,which will lead to environmental pollution.The release behavior of sulfur in fluidized bed gasification has not been fully studied,although fluidized bed gasification technology has a promising prospect.Thus the release behaviors of sulfur during fluidized bed gasification were investigated comprehensively through two aspects:temperature and reaction atmosphere.During air gasification,the main gaseous sulfur is H_(2)S,followed by COS,and the yield of SO_(2)and CS_(2)is low.With the increase of temperature,both of the released sulfur and the percentage of inorganic sulfur in gas phase increase.Under the same working condition,the distributions of sulfur forms in gasification residues are analogous.Organic sulfur is the dominate sulfur forms in the gasification residues.Sulfate in residues increases while organic sulfur decreases with increasing temperature.Among three reaction atmospheres(CO_(2)/steam/air)studied,the yield of H_(2)S is the most among the above four kinds of gaseous sulfur.The percentage of H_(2)S in gaseous sulfur(H_(2)S/Sg)is the highest in the process of steam gasification,while most sulfur is released during air gasification.The sequencing of H_(2)/CO is the same as that of H_(2)S/Sg,while the trend of sulfur release rate is consistent with that of carbon conversion rate.The distributions of sulfur species in the fly ash of CO_(2)gasification and steam gasification are similar,while the sulfate content in the fly ash of air gasification is the highest.展开更多
基金Project supported by the National Natural Science Foundation of China(Grant Nos.1625501 and 62027822)the Research Funds of Happiness Flower ECNU,China(Grant No.2021ST2110).
文摘It is proved that the chemical reaction induced by femtosecond laser filament in the atmosphere produces CO,HCN,and NO,and the production CO and HCN are observed for the first time.The concentrations of the products are measured by mid-infrared tunable laser absorption spectroscopy.In the reduced pressure air,the decomposition of CO_(2) is enhanced by vibration excitation induced by laser filament,resulting in the enhanced production of CO and HCN.At the same time,the CO and HCN generated from the atmosphere suffer rotation excitation induced by laser filament,enhancing their absorption spectra.It is found that NO,CO,and HCN accumulate to 134 ppm,80 ppm,and 1.6 ppm in sealed air after sufficient reaction time.The atmospheric chemical reaction induced by laser filament opens the way to changing the air composition while maintaining environmental benefits.
基金This work was supported by the Natural Science Foundation of Anhui Province, China (No.1208085MD59), the National Natural Science Foundation of China (No.U1232209, No.41175121, and No.21307137), the Presidential Foundation of Hefei Institutes of Physical Science, Chinese Academy of Sciences, China (No.YZJJ201302), and the Knowledge Innovation Foundation of the Chinese Academy of Sciences (No.KJCX2-YW-N24).
文摘In order to investigate the atmospheric oxidation processes and the formation of secondary organic aerosol (SOA), an indoor environmental reaction smog chamber are constructed and characterized. The system consists of the collapsible ~830 L FEP Teflon film main reactor, in which the atmospheric chemical reactions take place and the formation of SOA occurs under the simulated atmospheric conditions, and the diverse on-line gas- and particle-phase instrumentation, such as the proton transfer reaction mass spectrometer, the synchrotron radiation photoionization mass spectrometer, the aerosol laser time-of-flight mass spectrometer, and other traditional commercial instruments. The initial characterization experiments are described, concerning the temperature and ultraviolet light intensity, the reactivity of the pure air, the wall loss rates of gaseous compounds and particulate matter. And the initial evaluation experiments for SOA yields from the ozonolysis of α-pinene and for mass spectra of the products resulting from the photooxidation of OH initiated isoprene are also presented, which indicate the applicability of this facility on the studies of gas-phase chemical mechanisms as well as the formation of SOA expected in the atmosphere.
基金supported by the National Natural Science Foundation of China (No.21207145, 20937004)the Strategic Priority Research Program of the Chinese Academy of Sciences (No.XDB05050600)supported by the Special Co-construction Project of the Beijing Municipal Commission of Education
文摘As an important precursor of hydroxyl radical, nitrous acid (HONO) plays a key role in the chemistry of the lower atmosphere. Recent atmospheric measurements and model calculations show strong enhancement for HONO formation during daytime, while they are inconsistent with the known sources in the atmosphere, suggesting that current models are lacking important sources for HONO. In this article, heterogeneous photochemical reactions of nitric acid/nitrate anion and nitrogen oxide on various aerosols were reviewed and their potential contribution to HONO formation was also discussed. It is demonstrated that HONO can be formed by photochemical reaction on surfaces with deposited HNO3 , by photocatalytic reaction of NO2 on TiO2 or TiO2 -containing materials, and by photochemical reaction of NO2 on soot, humic acids or other photosensitized organic surfaces. Although significant uncertainties still exist in the exact mechanisms and the yield of HONO, these additional sources might explain daytime observations in the atmosphere.
基金supported by the National Natural Science Foundation of China(No.21337001,21377073)the Independent Innovation Foundation of Shandong University(IIFSDU)(No.2012JC030)
文摘In this article, the NO3 radical-initiated atmospheric oxidation degradation of DDT was theoretically investigated using molecular orbital theory calculations. All the calculations of intermediates, transition states and products were performed at the MPWB1K/6-311+G(3df,2p)//MPWB1K/6- 31+G(d,p) level of theory. Several energetically favorable reaction pathways were revealed. The formation mechanisms of secondary pollutants were presented and discussed. The rate constants were deduced over the temperature range of 273-333 K using canonical variational transition-state (CVT) theory with the small curvature tunneling (SCT) method. Our study shows that H abstraction from the alkyl group and NO3 addition to the Ca atom of the benzene ring are the dominant reaction pathways. The rate-temperature formula of the overall rate constants is k(T)(DDT+NO3) = (7.21 ~ 10-15)exp(-153.81/T) cm3/(mol.sec) over the possible atmospheric temperature range of 273-333 K. The atmospheric lifetime of DDT determined by NO3 radical is about 52.5 days, which indicates that it can be degraded in the gas phase within several months.
基金This study was supported by the National Key Research and Development Program of China(2018YFD0800703)Wuhan Science and Technology Project(2020020601012264)the Fundamental Research Funds for the Central Universities(2662018PY078).
文摘To explore the effect of biochar on alleviating plant drought stress after being applied to soil,we prepared biochar using rice straw as raw material according to different pyrolysis temperatures(400,600 and 800°C)and reaction atmosphere(CO_(2)and N_(2)).The effect of different pyrolysis conditions on the water retention performance of biochar was studied.The early high water-retaining biochar materials were selected and wheat seeds were selected for the verification experiment of returning to the field in pots.Biochar with high porosity(specific surface area and total pore volume)and more surface hydrophilic functional groups(mainly-OH and-COOH)can indeed improve soil water retention performance.It is mainly reflected in the increase in the dry weight and fresh weight of wheat and the soil moisture content in the treatment group with the addition of biochar water retention agent.Among them,the growth rates of fresh weight and dry weight of wheat in the C800 treatment group were 11.51%and 10.64%,and the soil moisture content increased by 1.89%.It is worth noting that the application of biochar cannot completely alleviate the impact of drought stress on plants,but it can reduce the amount of water irrigation to a certain extent.Considering the quality of biochar,the biochar material(C800)prepared under the pyrolysis temperature of 800°C and the reaction atmosphere of CO_(2)has high water retention performance.
基金This work was financially supported by National key research and development program of China(No.2017YFB0602302)Beijing Municipal Science and Technology Project(No.Z181100005118006).
文摘During fluidized bed gasification,sulfur in coal will be released,which will lead to environmental pollution.The release behavior of sulfur in fluidized bed gasification has not been fully studied,although fluidized bed gasification technology has a promising prospect.Thus the release behaviors of sulfur during fluidized bed gasification were investigated comprehensively through two aspects:temperature and reaction atmosphere.During air gasification,the main gaseous sulfur is H_(2)S,followed by COS,and the yield of SO_(2)and CS_(2)is low.With the increase of temperature,both of the released sulfur and the percentage of inorganic sulfur in gas phase increase.Under the same working condition,the distributions of sulfur forms in gasification residues are analogous.Organic sulfur is the dominate sulfur forms in the gasification residues.Sulfate in residues increases while organic sulfur decreases with increasing temperature.Among three reaction atmospheres(CO_(2)/steam/air)studied,the yield of H_(2)S is the most among the above four kinds of gaseous sulfur.The percentage of H_(2)S in gaseous sulfur(H_(2)S/Sg)is the highest in the process of steam gasification,while most sulfur is released during air gasification.The sequencing of H_(2)/CO is the same as that of H_(2)S/Sg,while the trend of sulfur release rate is consistent with that of carbon conversion rate.The distributions of sulfur species in the fly ash of CO_(2)gasification and steam gasification are similar,while the sulfate content in the fly ash of air gasification is the highest.