Large outdoor chamber experiments and computer simulations: (I) Secondary organic aerosol formation from the oxidation of a mixture of d-limonene and α-pinene

This work merges kinetic models for α-pinene and d-limonene which were individually developed to predict secondary organic aerosol (SOA) formation from these compounds. Three major changes in the d-limonene and α-pinene combined mechanism were made. First, radical–radical reactions were integrated so that radicals formed from both individual mechanisms all reacted with each other. Second, all SOA model species from both compounds were used to calculate semi-volatile partitioning for new semi-volatiles formed in the gas phase. Third particle phase reactions for particle phase α-pinene and d-limonene aldehydes, carboxylic acids, etc. were integrated. Experiments with mixtures of α-pinene and d-limonene, nitric oxide (NO), nitrogen dioxide (NO₂), and diurnal natural sunlight were carried out in a dual 270 m³ outdoor Teflon film chamber located in Pittsboro, NC. The model closely simulated the behavior and timing for α-pinene, d-limonene, NO, NO₂, O₃ and SOA. Model sensitivities were tested with respect to effects of d-limonene/α-pinene ratios, initial hydrocarbon to NO_x (HC₀/NO_x) ratios, temperature, and light intensity. The results showed that SOA yield (Y_SOA) was very sensitive to initial d-limonene/α-pinene ratio and temperature. The model was also used to simulate remote atmospheric SOA conditions that hypothetically could result from diurnal emissions of α-pinene, d-limonene and NO_x. We observed that the volatility of the simulated SOA material on the aging aerosol decreased with time, and this was consistent with chamber observations. Of additional importance was that our simulation did not show a loss of SOA during the daytime and this was consistent with observed measurements.     

Global environmental cycling of γ-HCH and DDT in the 1980s – A study using a coupled atmosphere and ocean general circulation model

A coupled atmosphere–ocean general circulation model, ECHAM5-MPIOM, was used to study the multicompartmental cycling and long-range transport of persistent and semivolatile organics. Multiphase systems in air and ocean are covered by submodels for atmospheric aerosols, HAM, and marine biogeochemistry, HAMOCC5, respectively. The model, furthermore, encompasses 2D surface compartments, i.e. top soil, vegetation surfaces and sea-ice. The total environmental fate of γ-hexachlorocyclohexane (γ-HCH, lindane) and dichlorophenyltrichloroethane (DDT) in agriculture were studied.DDT is mostly present in the soils, the water-soluble γ-HCH in soils and ocean. DDT has the longest residence time in almost all compartments. Quasi-steady state with regard to substance accumulation is reached within a few years in air and vegetation surfaces. In seawater the partitioning to suspended and sinking particles contributes to the vertical transport of substances. On the global scale deep water formation is, however, found to be more efficient. Up to 30% of DDT but only less than 0.2% of γ-HCH in seawater are stored in particulate matter.On the time scale studied (1 decade) and on global scale substance transport in the environment is determined by the fast atmospheric circulation. The meridional transport mechanism, for both compounds, is significantly enhanced by multi-hopping. Net meridional transport in the ocean is effective only regionally, mostly by currents along the western boundaries of Africa and the Americas. The total environmental burdens of the substances experience a net northward migration from their source regions, which is more pronounced for DDT than for γ-HCH. Due to the application distribution, however, after 10 years of simulation 21% of the global environmental burden of γ-HCH and 12% of DDT have accumulated in the Arctic.     

Fog Chemistry at an Urban Midwestern Site

This work investigates the oxidative aging of preformed secondary organic aerosol (SOA) derived from α-pinene ozonolysis (～100 ppb_v hydrocarbon [HC_x] with excess of O₃) within the University of California–Riverside Center for Environmental Research and Technology environmental chamber that occurs after introduction of additional hydroxyl (OH) and nitrate (NO₃) radicals. Simultaneous measurements of SOA volume concentration, hygroscopicity, particle density, and elemental chemical composition (C:O:H) reveal increased particle wall-loss-corrected SOA formation (1.5%, 7.5%, and 15.1%), increase in oxygen-to-carbon ratio (O/C; 15.6%, 8.7%, and 8.7%), and hydrophilicity (4.2%, 7.4%, and 1.4%) after addition of NO (ultraviolet [UV] on), H₂O₂ (UV on), and N₂O₅ (dark), respectively. The processing observed as an increase in O/C and hydrophilicity is attributed to OH and NO₃ reactions with first-generation vapor products and UV photolysis. The rate of increase in O/C appears to be only sufficient to achieve semivolatile oxygenated organic aerosol (SV-OOA) on a day time scale even at the raised chamber radical concentrations. The additional processing with UV irradiation without addition of NO, H₂O₂, or N₂O₅ is observed, adding 5.5% wall-loss-corrected volume. The photolysis-only processing is attributed to additional OH generated from photolysis of the nitrous acid (HONO) offgasing from chamber walls. This finding indicates that OH and NO₃ radicals can further alter the chemical composition of SOA from α-pinene ozonolysis, which is proved to consist of first-generation products.

Implications: Secondary organic aerosol (SOA) may undergo aging processes once formed in the atmosphere, thereby altering the physicochemical and toxic properties of aerosol. This study discusses SOA aging of a major biogenic volatile organic compound (VOC; α-pinene) after it initially forms SOA. Aging of the α-pinene ozonolysis system by OH (through NO or H₂O₂ injection), NO₃ (through N₂O₅ injection), and photolysis is observed. Although the reaction rate appears to be only sufficient to achieve semivolatile oxygenated organic aerosol (SV-OOA) level of oxygenation on a 1-day scale, it is important that SOA aging be considered in ambient air quality models. Aging in this study is attributed to further oxidation of gas-phase oxidation products of α-pinene ozonolysis.

Supplemental Materials: Supplemental materials are available for this paper. Go to the publisher's online edition of the Journal of the Air &; Waste Management Association for information on the referenced α-pinene ozonolysis reaction and chamber reactor temperature.     

Analysis of the relationship between ambient levels of O3, NO2 and NO as a function of NOx in the UK

Monitoring data from the UK Automatic Urban and Rural Network are used to investigate the relationships between ambient levels of ozone (O₃), nitric oxide (NO) and nitrogen dioxide (NO₂) as a function of NO_x, for levels ranging from those typical of UK rural sites to those observed at polluted urban kerbside sites. Particular emphasis is placed on establishing how the level of ‘oxidant’, OX (taken to be the sum of O₃ and NO₂) varies with the level of NO_x, and therefore to gain some insight into the atmospheric sources of OX, particularly at polluted urban locations. The analyses indicate that the level of OX at a given location is made up of NO_x-independent and NO_x-dependent contributions. The former is effectively a regional contribution which equates to the regional background O₃ level, whereas the latter is effectively a local contribution which correlates with the level of primary pollution. The local oxidant source has probable contributions from (i) direct NO₂ emissions, (ii) the thermal reaction of NO with O₂ at high NO_x, and (iii) common-source emission of species which promote NO to NO₂ conversion. The final category may include nitrous acid (HONO), which appears to be emitted directly in vehicle exhaust, and is potentially photolysed to generate HO_x radicals on a short timescale throughout the year at southern UK latitudes. The analyses also show that the local oxidant source has significant site-to-site variations, and possible reasons for these variations are discussed. Relationships between OX and NO_x, based on annual mean data, and fitted functions describing the relative contributions to OX made by NO₂ and O₃, are used to define expressions which describe the likely variation of annual mean NO₂ as a function of NO_x at 14 urban and suburban sites, and which can take account of possible changes in the regional background of O₃.     

Comparative studies of the Fe–UV, H2O2–UV, TiO2–UV/vis systems for the decolorization of a textile dye X-3B in water

The degradation of a common textile dye, Reactive-brilliant red X-3B, by several advanced oxidation technologies was studied in an air-saturated aqueous solution. The dye was resistant to the UV illumination (wavelength λ  320 nm), but was decolorized when one of Fe³⁺, H₂O₂ and TiO₂ components was present. The decolorization rate was observed to be quite different for each system, and the relative order evaluated under comparable conditions followed the order of Fe²⁺–H₂O₂–UV  Fe²⁺–H₂O₂ > Fe³⁺–H₂O₂–UV > Fe³⁺–H₂O₂ > Fe³⁺–TiO₂–UV > TiO₂–UV > Fe³⁺–UV > TiO₂–visible light (λ  450 nm) > H₂O₂–UV > Fe²⁺–UV. The mechanism for each process is discussed, and linked together for understanding the observed differences in reactivity.     

An important pathway for ozonolysis of alpha-pinene and beta-pinene in aqueous phase and its atmospheric implications

The aqueous ozonolysis of α-pinene and β-pinene was conducted under simulated tropospheric conditions at different pHs and temperatures. Three kinds of products, peroxides, carbonyl compounds, and organic acids, were well characterized, and the detection of these products provides effective evidence for understanding the atmospheric aqueous reaction pathway. We have two interesting findings: (1) the unexpected formation of methacrolein (MACR), with a yield of ～40%, in the α-pinene–O₃ aqueous reaction indicates a potentially new SOA formation pathway, because MACR is one of the important precursors of SOA; and (2) the surprisingly high yields of H₂O₂, ～60% for the α-pinene–O₃ reaction and ～100% for the β-pinene–O₃ reaction, indicates that H₂O₂ can be a significant contributor to the origin and transformation of oxidants in the atmosphere, especially in the humid regions. Moreover, we have determined the rate constant for aqueous reaction between MACR and H₂O₂ in pH 2 to 7 and obtained its upper limit as 0.13 M L^?1 s^?1. A mechanism concerning the formation of the species mentioned above is proposed, and it differs from that in the gas-phase reaction. We suggest that water plays a key role in the mechanism, by participating in the reactions as a direct reactant and by removing the excess energy of intermediates formed in the reactions.     

微波辐射Bi2O3/沸石-H2O2体系降解废水中的硝基苯

研究了微波辐射下，以负载于沸石上的三氧化二铋为催化剂，以双氧水为氧化剂的催化氧化体系处理硝基苯工艺。通过单因素实验法，从反应催化剂负载量、pH、双氧水用量、微波功率、反应时间、催化剂用量等方面初步考察了硝基苯在该体系中的催化氧化效果。在氧化铋负载量3%（质量比），pH=2，2 mL 30%双氧水，火力为中火，催化剂投加量为0.7 g，反应2 min，对降解过程所得的中间产物和终产物进行了分析。结果表明，该体系对硝基苯的去除率能够达到99.2%，COD去除率为73.91%。     

Biogeochemistry of two types of permeable reactive barriers, organic carbon and iron-bearing organic carbon for mine drainage treatment: Column experiments

Permeable reactive barriers (PRBs) are an alternative technology to treat mine drainage containing sulfate and heavy metals. Two column experiments were conducted to assess the suitability of an organic carbon (OC) based reactive mixture and an Fe⁰-bearing organic carbon (FeOC) based reactive mixture, under controlled groundwater flow conditions. The organic carbon mixture contains about 30% (volume) organic carbon (composted leaf mulch) and 70% (volume) sand and gravel. The Fe⁰-bearing organic carbon mixture contains 10% (volume) zero-valent iron, 20% (volume) organic carbon, 10% (volume) limestone, and 60% (volume) sand and gravel. Simulated groundwater containing 380 ppm sulfate, 5 ppm As, and 0.5 ppm Sb was passed through the columns at flow rates of 64 (the OC column) and 62 (the FeOC column) ml d^− 1, which are equivalent to 0.79 (the OC column) and 0.78 (the FeOC column) pore volumes (PVs) per week or 0.046 m d^− 1 for both columns. The OC column showed an initial sulfate reduction rate of 0.4 µmol g (OC)^− 1 d^− 1 and exhausted its capacity to promote sulfate reduction after 30 PVs, or 9 months of flow. The FeOC column sustained a relatively constant sulfate reduction rate of 0.9 µmol g (OC)^− 1 d^− 1 for at least 65 PVs (17 months). In the FeOC column, the δ³⁴S values increase with the decreasing sulfate concentration. The δ³⁴S fractionation follows a Rayleigh fractionation model with an enrichment factor of 21.6‰. The performance decline of the OC column was caused by the depletion of substrate or electron donor. The cathodic production of H₂ by anaerobic corrosion of Fe probably sustained a higher level of SRB activity in the FeOC column. These results suggest that zero-valent iron can be used to provide an electron donor in sulfate reducing PRBs. A sharp increase in the δ¹³C value of the dissolved inorganic carbon and a decrease in the concentration of HCO₃⁻ indicate that hydrogenotrophic methanogenesis is occurring in the first 15 cm of the FeOC column.     

Biological elimination of H2S and NH3 from wastegases by biofilter packed with immobilized heterotrophic bacteria

Biotreatment of various ratios of H₂S and NH₃ gas mixtures was studied using the biofilters, packed with co-immobilized cells (Arthrobacter oxydans CH8 for NH₃ and Pseudomonas putida CH11 for H₂S). Extensive tests to determine removal characteristics, removal efficiency, removal kinetics, and pressure drops of the biofilters were performed. To estimate the largest allowable inlet concentration, a prediction model was also employed. Greater than 95% and 90% removal efficiencies were observed for NH₃ and H₂S, respectively, irrespective of the ratios of H₂S and NH₃ gas mixtures. The results showed that H₂S removal of the biofilter was significantly affected by high inlet concentrations of H₂S and NH₃. As high H₂S concentration was an inhibitory substrate for the growth of heterotrophic sulfur-oxidizing bacteria, the activity of H₂S oxidation was thus inhibited. In the case of high NH₃ concentration, the poor H₂S removal efficiency might be attributed to the acidification of the biofilter. The phenomenon was caused by acidic metabolite accumulation of NH₃. Through kinetic analysis, the presence of NH₃ did not hinder the NH₃ removal, but a high H₂S concentration would result in low removal efficiency. Conversely, H₂S of adequate concentrations would favor the removal of incoming NH₃. The results also indicated that maximum inlet concentrations (model-estimated) agreed well with the experimental values for space velocities of 50–150 h⁻¹. Hence, the results would be used as the guideline for the design and operation of biofilters.     

Evaluation of a detailed model of secondary organic aerosol formation from α-pinene against dark ozonolysis experiments

BOREAM, a detailed model for the gas-phase oxidation of α-pinene and its subsequent formation of Secondary Organic Aerosol (SOA), is tested against a large set of SOA yield measurements obtained in dark ozonolysis experiments. For the majority of experiments, modelled SOA yields are found to agree with measured yields to within a factor 2. However, the comparisons point to a general underestimation of modelled SOA yields at high temperatures (above 30 °C), reaching an order of magnitude or more in the worst cases, whereas modelled SOA yields are often overestimated at lower temperature (by a factor of about 2). Comparisons of results obtained using four different vapour pressure prediction methods indicate a strong sensitivity to the choice of the method, although the overestimated temperature dependence of the yields is found in all cases. Accounting for non-ideality of the aerosol mixture (based on an adapted UNIFAC method) has significant effects, especially at low yields. Our simulations show that the formation of oligomers through the gas-phase reactions of Stabilised Criegee Intermediates (SCI) with other molecular organic products could increase the SOA yield significantly only at very low relative humidity (below 1%). Further tests show that the agreement between model and measurements is improved when the ozonolysis mechanism includes additional production of non-volatile compounds.     

改性矿物吸附法和 O3氧化法对维生素 B12废水脱色处理简

采用改性矿物吸附法和O₃氧化法对某制药厂维生素B₁₂废水进行脱色处理。以废水色度去除率大于50%为目的，通过实验确定改性矿物吸附法和O₃氧化法处理维生素B₁₂废水的最佳工艺条件：废水的pH为3.00，有机化膨润土的投加量为5 g/L，PAC的投加量为6 g/L，投加有机化膨润土后搅拌时间为30 min时，废水的色度去除率可达到51.3%，处理成本为12.85元/t。O₃氧化法的最佳条件：废水的pH保持不变，O₃流量为5 g/h，反应时间为2 min，废水的色度去除率可达到68.8%，处理成本为0.96元/t。对比这2种方法，O₃氧化法处理该废水成本更低、效率更高，并且能提高废水的可生化性以便后续处理。     

Primary source attribution and analysis of α-pinene photooxidation products in Duke Forest,North Carolina

Samples of fine particulate organic matter were collected outside Durham, NC in the Duke Research Forest as part of the CELTIC study in July 2003. Particulate samples were collected on quartz filters using high volume air sampling equipment, and samples were analyzed for polar and non-polar organic species. Among compounds analyzed, oxidation products of α-pinene, namely pinic acid and pinonic acid, were identified in all samples. Pinic acid, being a dicarboxylic acid, has a low vapor pressure of the order of 10⁻⁸ Torr and is expected to contribute significantly to secondary organic aerosol (SOA) formation from the oxidation of α-pinene. Source contribution estimates from primary organic aerosol emissions were computed using the organic species as molecular markers with the chemical mass balance (CMB) model. The unapportioned organic carbon (OC) was determined as the difference between measured OC and OC apportioned to primary sources. This unapportioned OC was then correlated with pinic and pinonic acid to get a better understanding of the role of monoterpene oxidation products to form SOA. A reasonably good fit between pinic acid concentrations and unapportioned OC levels is indicative of the contribution of α-pinene oxidation products to SOA formation in ambient atmosphere. The results are significant considering the role of monoterpene emissions to global atmospheric chemistry.     

Regression modelling of hourly NOx and NO2 concentrations in urban air in London

Based on hourly measurements of NO_x NO₂ and O₃ and meteorological data, an ordinary least squares (OLS) model and a first-order autocorrelation (AR) model were developed to analyse the regression and prediction of NO_x and NO₂ concentrations in London. Primary emissions and wind speed are the most important factors influencing NO_x concentrations; in addition to these two, reaction of NO with O₃ is also a major factor influencing NO₂ concentrations. The AR model resulted in high correlation coefficients (R > 0.95) for the NO_x and NO₂ regression based on a whole year's data, and is capable of predicting NO₂ (R = 0.83) and NO_x (R = 0.65) concentrations when the explanatory variables were available. The analysis of the structure of regression models by Principal Component Analysis (PCA) indicates that the regression models are stable. The results of the OLS model indicate that there was an exceptional NO₂ source, other than primary emission and reaction of NO with O₃, in the air pollution episode in London in December 1991.     

O3/H2O2处理嘧啶废水的研究

采用O3/H2O2法对嘧啶废水进行处理,考察了不同反应条件对嘧啶和COD去除率的影响,并对O3/H2O2降解嘧啶的反应机制和动力学进行了初步探讨.实验结果表明,在pH值为11,反应时间为70 min,O3流量为4g/h,H2O2投加量为50 mmol/L的条件下,废水的嘧啶和COD的去除率分别达到86.46%和74.9...     

Contributions of biogenic volatile organic compounds to the formation of secondary organic aerosols over Mt. Tai,Central East China

To better understand the contribution of biogenic volatile organic compounds to the formation of secondary organic aerosol (SOA) in high mountain regions, ambient aerosols were collected at the summit of Mt. Tai (1534 m, a.s.l.), Central East China (CEC) during the Mount Tai Experiment 2006 campaign (MTX2006) in early summer. Biogenic SOA tracers for the oxidation of isoprene, α/β-pinene, and β-caryophyllene were measured using gas chromatography/mass spectrometry. Most of the biogenic SOA tracers did not show clear diurnal variations, suggesting that they are formed during long-range atmospheric transport or over relatively long time scales. Although isoprene- and α/β-pinene-derived SOA tracers did not correlate with levoglucosan (a biomass burning tracer), β-caryophyllinic acid showed a good correlation with levoglucosan, indicating that crop residue burning may be a source for this acid. Total concentrations of isoprene oxidation products are much higher than those of α/β-pinene and β-caryophyllene oxidation products. The averaged ratio of isoprene to α/β-pinene oxidation products (R_iso/pine) was 4.9 and 6.7 for the daytime and nighttime samples, respectively. These values are among the highest in the aerosols reported in different geographical regions, which may be due to the large isoprene fluxes and relatively high levels of oxidants such as OH in CEC. Using a tracer-based method, we estimated the concentrations of secondary organic carbon (SOC) derived from isoprene, α/β-pinene, and β-caryophyllene to be 0.42–3.1 μgC m^?3 (average 1.6 μgC m^?3) during the daytime and 0.11–4.2 μgC m^?3 (1.7 μgC m^?3) during the nighttime. These values correspond to 2.9–23% (10%) and 3.2–28% (9.8%) of the total OC concentrations, in which isoprene-derived SOC accounts for 58% and 63% of total SOC during the daytime and nighttime, respectively. This study suggests that isoprene is a more significant precursor for biogenic SOA than α/β-pinene and β-caryophyllene at high altitudes in CEC.     

铁氧化物复合氧化铝催化臭氧化过程中溴酸盐的生成控制简

以市售活性炭、硅藻土和氧化铝小球为载体，考察了负载铁基活性组分对催化臭氧化过程中溴酸盐的控制情况，其中，铁基复合氧化铝小球体现出更好的溴酸盐还原特性和催化剂稳定性，证实催化剂中铁氧化物是溴酸盐得到有效控制的主要活性组分。进一步考察了铁基复合氧化铝小球催化臭氧化处理实际原水过程中对溴酸盐的生成控制，以及反应过程中溶解性有机碳（DOC）的去除情况。结果表明，与单独臭氧化相比，该催化剂既能有效去除水中的溶解性有机物，又能明显抑制溴酸盐的生成，反应50 h，其活性并没有明显下降。催化剂失活主要归因于吸附位点数量的下降，可以通过负载铁氧化物来实现催化剂的再生。     

A kinetic mechanism for predicting secondary organic aerosol formation from toluene oxidation in the presence of NOx and natural sunlight

A kinetic mechanism to predict secondary organic aerosol (SOA) formation from the photo-oxidation of toluene was developed. Aerosol phase chemistry that includes nucleation, gas–particle partitioning and particle-phase reactions as well as the gas-phase chemistry of toluene and its degradation products were represented. The mechanism was evaluated against experimental data obtained from the University of North Carolina (UNC) 270 m³ dual outdoor aerosol smog chamber facility. The model adequately simulates the decay of toluene, the nitric oxide (NO) to nitrogen dioxide (NO₂) conversion and ozone formation. It also provides a reasonable prediction of SOA production under different conditions that range from 15 to 300 μg m⁻³. Speciation of simulated aerosol material shows that up to 70% of the aerosol mass comes from oligomers and polymers depending on initial reactant concentrations. The dominant particle-phase species predicted by the mechanism are glyoxal oligomers, ketene oligomers from the photolysis of the toluene OH reaction product 2-methyl-2,4-hexadienedial, organic nitrates, methyl nitro-phenol analogues, C7 organic peroxides, acylperoxy nitrates and for the low-concentration experiments, unsaturated hydroxy nitro acids.     

Carbonyl products of the gas-phase reaction of ozone with 1-alkenes

Carbonyl products have been identified and their formation yields measured in experiments involving the gas-phase reaction of ozone with the 1-alkenes (RCH = CH 2) 3-methyl-l-butene (R = i-propyl), 4-methyl-l-pentene (R = i-butyl), 3-methyl-l-pentene (R= s-butyl), 3,3-dimethyl-l-butene (R = t-butyl) and styrene (R = C₆H₅) at ambient T and p = 1 atm of air. Sufficient cyclohexane was added to scavenge OH in order to minimize reactions of OH with the alkenes and with their carbonyl products. Formation yields (carbonyl formed/ozone reacted) of primary carbonyls were close to the value of 1.0 that is consistent with the mechanism: O₃ + RCH = CH₂ → α(HCHO + RCHOO) + (1 - α) (H₂COO + RCHO), where formaldehyde and RCHO are the primary carbonyls and H₂COO and RCHOO are the biradicals. Measured sums of the primary carbonyl formation yields were 1.006 ± 0.053 (1 S.D.) for formaldehyde + methylpropanal from3-methyl-l-butene(α = 0.494 ± 0.049), 1.025 ± 0.017 for formaldehyde + 2-methylbutanal from 3-methyl-l-pentene (α = 0.384 ± 0.013),1.147 ± 0.050 for formaldehyde + 3-methylbutanal from 4-methyl-l-pentene (α = 0.384 ± 0.020), 0.986 ± 0.014 for formaldehyde + 2,2-dimethylpropanal from 3,3-dimethyl-l-butene (α = 0.320 ± 0.012) and 0.980 ± 0.086 for formaldehyde + benzaldehyde from styrene (α = 0.347 ± 0.059). Carbonyls other than the primary carbonyls were identified; formation pathways are proposed that involve subsequent reactions of the monosubstituted biradicals RCHOO. Similarities and differences between branched-chain 1-alkenes and n-alkyl-substituted 1-alkenes are discussed.     

A new environmental chamber for evaluation of gas-phase chemical mechanisms and secondary aerosol formation

A new state-of-the-art indoor environmental chamber facility for the study of atmospheric processes leading to the formation of ozone and secondary organic aerosol (SOA) has been constructed and characterized. The chamber is designed for atmospheric chemical mechanism evaluation at low reactant concentrations under well-controlled environmental conditions. It consists of two collapsible 90 m³ FEP Teflon film reactors on pressure-controlled moveable frameworks inside a temperature-controlled enclosure flushed with purified air. Solar radiation is simulated with either a 200 kW Argon arc lamp or multiple blacklamps. Results of initial characterization experiments, all carried out at 300–305 K under dry conditions, concerning NO_x and formaldehyde offgasing, radical sources, particle loss rates, and background PM formation are described. Results of initial single organic–NO_x and simplified ambient surrogate–NO_x experiments to demonstrate the utility of the facility for mechanism evaluation under low NO_x conditions are summarized and compared with the predictions of the SAPRC-99 chemical mechanism. Overall, the results of the initial characterization and evaluation indicate that this new environmental chamber can provide high quality mechanism evaluation data for experiments with NO_x levels as low as 2 ppb, though the results indicate some problems with the gas-phase mechanism that need further study. Initial evaluation experiments for SOA formation, also carried out under dry conditions, indicate that the chamber can provide high quality secondary aerosol formation data at relatively low hydrocarbon concentrations.     

Co3O4/介孔分子筛催化剂对苯催化完全氧化的研究

分别以介孔分子筛MCM-41、MCM-48、SBA-15为载体，采用等体积浸渍法制备了氧化钴/介孔分子筛催化剂，利用N₂吸附、X射线衍射、程序升温还原等技术对催化剂进行了表征，考察了Co₃O₄的负载量及载体的孔结构对催化剂完全催化氧化苯的性能的影响。结果表明，Co₃O₄的负载量为20%时，催化剂的催化活性最好；载体的孔径和催化剂的可还原性能是影响催化活性的主要因素，催化剂活性顺序为Co₃O₄ /SBA-15> Co₃O₄ /MCM41> Co₃O₄ /MCM-48。