A distributed feedback laser with a wavelength of 2.8μm was used to measure the species produced by water vapor glow discharge.Only the absorption spectra of OH radicals and transient H2O molecules were observed usin...A distributed feedback laser with a wavelength of 2.8μm was used to measure the species produced by water vapor glow discharge.Only the absorption spectra of OH radicals and transient H2O molecules were observed using concentration modulation(CM)spectroscopy.The intensities and orientations of the absorption peaks change with the demodulation phase,but the direction of one absorption peak of H2O is always opposite to the other peaks.The different spectral orientations of OH and H2O reflect the increase or the decrease of the number of particles in the energy levels.If more transient species can be detected in the discharge process,the dynamics of excitation,ionization,and decomposition of H2O can be better studied.This study shows that the demodulation phase relationship of CM spectrum can be used to study the population change of molecular energy levels.展开更多
Photolysis rate (J1) and reaction rate constants (kl) for the biacetyl (butane-2,3-dione) were evaluated in aqueous phase using a continuous photolysis system with a conventional Xe-Hg arc lamp as a light source...Photolysis rate (J1) and reaction rate constants (kl) for the biacetyl (butane-2,3-dione) were evaluated in aqueous phase using a continuous photolysis system with a conventional Xe-Hg arc lamp as a light source. The OH radicals was generated by H2OE/UV process and biacetyl (CH3C(O)C(O)CH3) concentrations were monitored using 2,4-DNPH derivatization method. 2,3-butanedione molecule is widely present in the atmosphere, it have been detected in hydrometeors (fogs, rain, and clouds) and at a significant yield (up to 10μmolar). The measurements were performed at 294 K and with free pH values. Our results lead to the following obtained values: J1= 3×10^-4 S^-1 and k1 = (6.17±0.95)×10^8 M^-1·s^-1.The uncertainty listed above is ±15%.展开更多
Plasma produced many active species such as OH radical and H radical. As well known, OH radical plays an important role in degrading complex pollutants. This study aims to measure the production of OH radicals and eva...Plasma produced many active species such as OH radical and H radical. As well known, OH radical plays an important role in degrading complex pollutants. This study aims to measure the production of OH radicals and evaluate important parameters that have influent in degradation process of waste water contains ammonia in circulated system and analyze the level of energy consumptions are resulted by this research. The production of OH radical was detected by formation of hydrogen peroxide which was resulted by recombination reaction between OH radicals during plasma electrolysis process. From the measured concentration of hydrogen peroxide, obtained concentration of OH radical is 2,020 ppm. The depth of anode, applied voltage and ammonia initial concentration have affected ammonia degradation percentage and energy consumption level. The highest result for ammonia degradation percentage is 63.2% which gets from applied voltage 700 V, with depth of anode 1 cm, initial concentration of ammonia 100 ppm, and lowest energy consumption of 110 KJ/mmol.展开更多
An experimental study of thermal DeNOx process with different additives was performed in an electricityheated tubular flow reactor,showing that CO is less effective to lower the optimum temperature than H2 and CH4. Th...An experimental study of thermal DeNOx process with different additives was performed in an electricityheated tubular flow reactor,showing that CO is less effective to lower the optimum temperature than H2 and CH4. The maximum NO reduction is lowered with H2 added,while it is hardly affected by CO or CH4.The temperature window is widened appreciably with CH4 added,while it is narrowed slightly by H2 or CO.The disadvantage of CH4 is that it causes CO emission due to its incomplete oxidation,and the maximum conversion of CH4 to CO is more than 50%.In general,the calculation using a detailed chemical kinetic model predicts most of the process features reasonably well.The analysis on reaction mechanism shows that the effects of these additives on NO reduction are achieved principally by promoting the production of·OH radical.展开更多
Biodiesel is a kind of clean and renewable energy. The effect of ethanol addition on the flame characteristics of waste oil biodiesel is studied by using OH-PLIF technique from the perspective of OH radical evolution....Biodiesel is a kind of clean and renewable energy. The effect of ethanol addition on the flame characteristics of waste oil biodiesel is studied by using OH-PLIF technique from the perspective of OH radical evolution. Ethanol addition leads to the appearance of diffusion flame reaction interface ahead of schedule and shortens the diffusion flame height. The experimental results show a linear correlation between the flame height and the fuel flow rate for a given fuel and oxidant. The same conclusion is drawn from the theoretical analysis of the approximate model. In addition. ethanol addition makes the average OH signal intensity of flame at different fuel flow rate tend to be consistent and the fuel flow rate enlarge where the flame field shows the strongest oxidation performance. Average OH signal intensity begins to weaken at larger fuel flow rate, which indicates that fuel flow rate of fuels blended with ethanol can change in larger range and does not significantly affect the uniformity of combustion.展开更多
Photocatalytic reduction of Cr(VI) by TiO2 suspension has been studied with the purpose of removing the toxic and carcinogenic Cr(VI) ions from water. The photocatalytic reduction was carried out in batch reactor,...Photocatalytic reduction of Cr(VI) by TiO2 suspension has been studied with the purpose of removing the toxic and carcinogenic Cr(VI) ions from water. The photocatalytic reduction was carried out in batch reactor, in which the influences of the presence ofmalonic and oxalic acids as well as of iron and lead ions on the degree of the reduction have been systematically evaluated. The results of the research indicated that the presence of malonic and oxalic acids with increasing concentration can improve the photoreduction. The increase in the Cr(V1) photoreduction is due to OH radical capturing by the organic acids so that it prevents the recombination of the OH radical and the free electron, and therefore can provide enough electron supply for Cr(VI) photoreduction. The effectiveness of Cr(VI) photoreduction is also enhanced by the addition of increasing concentration of both Fe(Ⅲ) and Pb(Ⅱ) ions through synergic effect. It is also found that the degree of the photopreduction is strongly influenced by solution acidity and the most effective Cr(VI) photoreduction is obtained at lower pH than 5, either in the absence or presence of the organic acids and the heavy metal ions.展开更多
The aim of this work was to study the influence of effluent organic matter (EfOM) on micropollutants removal by ozone and UV/H2O2. To perform the experiments, deionized water and municipal secondary effluents (SE)...The aim of this work was to study the influence of effluent organic matter (EfOM) on micropollutants removal by ozone and UV/H2O2. To perform the experiments, deionized water and municipal secondary effluents (SE) were artificially contaminated with atrazine (ATZ) and treated by the two proposed methods. ATZ concentration, COD and TOC were recorded along the reaction time and used to evaluate EfOM effect on the system efficiency. Results demonstrate that the presence of EfOM can significantly reduce the micropollutant removal rate due to competition of EfOM components to react with radicals and/or molecular ozone. The hydroxyl radical scavenging caused by EfOM was quantified as well as the contribution of molecular ozone and .OH radicals during the ozonation of SE. EfOM components promoted higher inhibition of ATZ oxidation by hydroxyl radicals than by molecular ozone.展开更多
The multi-stages humidifier semi-dry flue gas cleaning technology, the CRS plasma flue gas cleaning technology and oxidative additive flue gas cleaning technology were investigated for multi-pollutants removal. The se...The multi-stages humidifier semi-dry flue gas cleaning technology, the CRS plasma flue gas cleaning technology and oxidative additive flue gas cleaning technology were investigated for multi-pollutants removal. The semi-dry flue gas cleaning technology using multi-stages humidifier and additive can improve oxidation and absorption, and it can achieve high multi-pollutants removal efficiency. The CRS discharge can produce many OH radicals that promote NO oxidation. Combining NaOH absorption can achieve high deSO2 and deNO, efficiencies. It is fit for the reconstruction of primary wet flue gas desulfurization (WFGD). In addition, using NaClO2 as additive in the absorbent of WFGD can obtain very high removal efficiency of SO2 and NOx.展开更多
Nitrous acid (HONO), as a primary precursor of OH radicals, has been considered one of the most important nitrogencontaining species in the atmosphere. Up to 30% of primary OH radical production is attributed to the...Nitrous acid (HONO), as a primary precursor of OH radicals, has been considered one of the most important nitrogencontaining species in the atmosphere. Up to 30% of primary OH radical production is attributed to the photolysis of HONO. However, the major HONO formation mechanisms are still under discussion. During the Campaigns of Air Quality Research in Beijing and Surrounding Region (CAREBeijing2006) campaign, comprehensive measurements were carried out in the megacity Beijing, where the chemical budget of HONO was fully constrained. The average diurnal HONO concentration varied from 0.33 to 1.2 ppbv. The net OH production rate from HONO, Pon(HONO)net, was on average (from 05:00 to 19:00) 7.1 × 10^6 molecule/(cm^3 s), 2.7 times higher than from 03 photolysis. This production rate demonstrates the important role of HONO in the atmospheric chemistry of megacity Beijing. An unknown HONO source (Punknown) with an average of 7.3 × 10^6 molecule/(cm^3 s) was derived from the budget analysis during daytime. Punknown provided four times more HONO than the reaction of NO with OH did. The diurnal variation of Punknown showed an apparent photo-enhanced feature with a maximum around 12:00, which was consistent with previous studies at forest and rural sites. Laboratory studies proposed new mechanisms to recruit NO2 and J(NO2) in order to explain a photo-enhancement of of Puknown. In this study, these mechanisms were validated against the observation-constraint Punknown. The reaction of exited NO2 accounted for only 6% of Puknown, and Punk poorly correlated with [NO2] (R = 0.26) and J(NO2)[NO2] (R = 0.35). These results challenged the role of NO2 as a major precursor of the missing HONO source.展开更多
基金the National Natural Science Foundation of China(No.61625501,No.61427816)the Open Fund of the State Key Laboratory of High Field Laser Physics(SIOM)the Open Fund of the State Key Laboratory of Precision Spectroscopy。
文摘A distributed feedback laser with a wavelength of 2.8μm was used to measure the species produced by water vapor glow discharge.Only the absorption spectra of OH radicals and transient H2O molecules were observed using concentration modulation(CM)spectroscopy.The intensities and orientations of the absorption peaks change with the demodulation phase,but the direction of one absorption peak of H2O is always opposite to the other peaks.The different spectral orientations of OH and H2O reflect the increase or the decrease of the number of particles in the energy levels.If more transient species can be detected in the discharge process,the dynamics of excitation,ionization,and decomposition of H2O can be better studied.This study shows that the demodulation phase relationship of CM spectrum can be used to study the population change of molecular energy levels.
文摘Photolysis rate (J1) and reaction rate constants (kl) for the biacetyl (butane-2,3-dione) were evaluated in aqueous phase using a continuous photolysis system with a conventional Xe-Hg arc lamp as a light source. The OH radicals was generated by H2OE/UV process and biacetyl (CH3C(O)C(O)CH3) concentrations were monitored using 2,4-DNPH derivatization method. 2,3-butanedione molecule is widely present in the atmosphere, it have been detected in hydrometeors (fogs, rain, and clouds) and at a significant yield (up to 10μmolar). The measurements were performed at 294 K and with free pH values. Our results lead to the following obtained values: J1= 3×10^-4 S^-1 and k1 = (6.17±0.95)×10^8 M^-1·s^-1.The uncertainty listed above is ±15%.
文摘Plasma produced many active species such as OH radical and H radical. As well known, OH radical plays an important role in degrading complex pollutants. This study aims to measure the production of OH radicals and evaluate important parameters that have influent in degradation process of waste water contains ammonia in circulated system and analyze the level of energy consumptions are resulted by this research. The production of OH radical was detected by formation of hydrogen peroxide which was resulted by recombination reaction between OH radicals during plasma electrolysis process. From the measured concentration of hydrogen peroxide, obtained concentration of OH radical is 2,020 ppm. The depth of anode, applied voltage and ammonia initial concentration have affected ammonia degradation percentage and energy consumption level. The highest result for ammonia degradation percentage is 63.2% which gets from applied voltage 700 V, with depth of anode 1 cm, initial concentration of ammonia 100 ppm, and lowest energy consumption of 110 KJ/mmol.
基金Supported by the State Key Development Program for Basic Research of China(2006CB200303) the National Natural Science Foundation of China (50706011) the National High Technology Research and Development Program of China(2007AA05Z337)
文摘An experimental study of thermal DeNOx process with different additives was performed in an electricityheated tubular flow reactor,showing that CO is less effective to lower the optimum temperature than H2 and CH4. The maximum NO reduction is lowered with H2 added,while it is hardly affected by CO or CH4.The temperature window is widened appreciably with CH4 added,while it is narrowed slightly by H2 or CO.The disadvantage of CH4 is that it causes CO emission due to its incomplete oxidation,and the maximum conversion of CH4 to CO is more than 50%.In general,the calculation using a detailed chemical kinetic model predicts most of the process features reasonably well.The analysis on reaction mechanism shows that the effects of these additives on NO reduction are achieved principally by promoting the production of·OH radical.
基金Project(51766007)supported by the National Natural Science Foundation of ChinaProject(U1602272)supported by the NSFC-Yunnan Joint Fund Project+1 种基金Project(2015FB128)supported by the Natural Science Fund Project in Yunnan Province,ChinaProject(CNMRCUTS1704)supported by the Research Fund from State Key Laboratory of Complex Nonferrous Metal Resources Clean Utilization,China
文摘Biodiesel is a kind of clean and renewable energy. The effect of ethanol addition on the flame characteristics of waste oil biodiesel is studied by using OH-PLIF technique from the perspective of OH radical evolution. Ethanol addition leads to the appearance of diffusion flame reaction interface ahead of schedule and shortens the diffusion flame height. The experimental results show a linear correlation between the flame height and the fuel flow rate for a given fuel and oxidant. The same conclusion is drawn from the theoretical analysis of the approximate model. In addition. ethanol addition makes the average OH signal intensity of flame at different fuel flow rate tend to be consistent and the fuel flow rate enlarge where the flame field shows the strongest oxidation performance. Average OH signal intensity begins to weaken at larger fuel flow rate, which indicates that fuel flow rate of fuels blended with ethanol can change in larger range and does not significantly affect the uniformity of combustion.
文摘Photocatalytic reduction of Cr(VI) by TiO2 suspension has been studied with the purpose of removing the toxic and carcinogenic Cr(VI) ions from water. The photocatalytic reduction was carried out in batch reactor, in which the influences of the presence ofmalonic and oxalic acids as well as of iron and lead ions on the degree of the reduction have been systematically evaluated. The results of the research indicated that the presence of malonic and oxalic acids with increasing concentration can improve the photoreduction. The increase in the Cr(V1) photoreduction is due to OH radical capturing by the organic acids so that it prevents the recombination of the OH radical and the free electron, and therefore can provide enough electron supply for Cr(VI) photoreduction. The effectiveness of Cr(VI) photoreduction is also enhanced by the addition of increasing concentration of both Fe(Ⅲ) and Pb(Ⅱ) ions through synergic effect. It is also found that the degree of the photopreduction is strongly influenced by solution acidity and the most effective Cr(VI) photoreduction is obtained at lower pH than 5, either in the absence or presence of the organic acids and the heavy metal ions.
文摘The aim of this work was to study the influence of effluent organic matter (EfOM) on micropollutants removal by ozone and UV/H2O2. To perform the experiments, deionized water and municipal secondary effluents (SE) were artificially contaminated with atrazine (ATZ) and treated by the two proposed methods. ATZ concentration, COD and TOC were recorded along the reaction time and used to evaluate EfOM effect on the system efficiency. Results demonstrate that the presence of EfOM can significantly reduce the micropollutant removal rate due to competition of EfOM components to react with radicals and/or molecular ozone. The hydroxyl radical scavenging caused by EfOM was quantified as well as the contribution of molecular ozone and .OH radicals during the ozonation of SE. EfOM components promoted higher inhibition of ATZ oxidation by hydroxyl radicals than by molecular ozone.
基金supported by NSF of Zhejiang (Y507079)EOP of Zhejiang (Y200702725)PSF of China (20080431325)
文摘The multi-stages humidifier semi-dry flue gas cleaning technology, the CRS plasma flue gas cleaning technology and oxidative additive flue gas cleaning technology were investigated for multi-pollutants removal. The semi-dry flue gas cleaning technology using multi-stages humidifier and additive can improve oxidation and absorption, and it can achieve high multi-pollutants removal efficiency. The CRS discharge can produce many OH radicals that promote NO oxidation. Combining NaOH absorption can achieve high deSO2 and deNO, efficiencies. It is fit for the reconstruction of primary wet flue gas desulfurization (WFGD). In addition, using NaClO2 as additive in the absorbent of WFGD can obtain very high removal efficiency of SO2 and NOx.
基金supported by the National Natural Science Foundation of China(21190052,40675072,41121004)the Ministry of Science and Technology of China(2002CB410801)the Beijing Council of Science and Technology(HB200504-6,HB200504-2)
文摘Nitrous acid (HONO), as a primary precursor of OH radicals, has been considered one of the most important nitrogencontaining species in the atmosphere. Up to 30% of primary OH radical production is attributed to the photolysis of HONO. However, the major HONO formation mechanisms are still under discussion. During the Campaigns of Air Quality Research in Beijing and Surrounding Region (CAREBeijing2006) campaign, comprehensive measurements were carried out in the megacity Beijing, where the chemical budget of HONO was fully constrained. The average diurnal HONO concentration varied from 0.33 to 1.2 ppbv. The net OH production rate from HONO, Pon(HONO)net, was on average (from 05:00 to 19:00) 7.1 × 10^6 molecule/(cm^3 s), 2.7 times higher than from 03 photolysis. This production rate demonstrates the important role of HONO in the atmospheric chemistry of megacity Beijing. An unknown HONO source (Punknown) with an average of 7.3 × 10^6 molecule/(cm^3 s) was derived from the budget analysis during daytime. Punknown provided four times more HONO than the reaction of NO with OH did. The diurnal variation of Punknown showed an apparent photo-enhanced feature with a maximum around 12:00, which was consistent with previous studies at forest and rural sites. Laboratory studies proposed new mechanisms to recruit NO2 and J(NO2) in order to explain a photo-enhancement of of Puknown. In this study, these mechanisms were validated against the observation-constraint Punknown. The reaction of exited NO2 accounted for only 6% of Puknown, and Punk poorly correlated with [NO2] (R = 0.26) and J(NO2)[NO2] (R = 0.35). These results challenged the role of NO2 as a major precursor of the missing HONO source.