南宁市灰霾天气与空气污染物关系分析

根据2010年6月1日至2011年5月31日南宁市的环境监测数据和气象数据,分析南宁市灰霾天气特征,然后通过SPSS软件分析灰霾天气与能见度、颗粒物(PM2.5、PM10)浓度、气态污染物浓度和空气污染指数的关系,探讨南宁市灰霾天气与空气污染物的关系。结果发现,南宁市灰霾天气主要分布在秋、冬两季,PM2.5是直接造成南宁市灰霾天气的主要因子,PM10、SO2、NO2、CO和O3对灰霾天气的发生也有一定影响。PM2.5与PM10相关性最显著,与SO2、NO2相关性较显著,与CO相关性显著,与O3相关性不显著。     

Emission inventories of primary particles and pollutant gases for China

Detailed high-resolution emission inventories of primary particles(PM2.5,BC and OC) and pollutant gases(SO2,NOx,NH3,CO and VOCs) for China in 2007 were constructed on the basis of the latest fuel consumption data,mostly at the county level,and from socio-economic statistics and data on fossil and biomass fuels obtained from government agencies.New emission factors reflecting local features were also used.The calculated emissions were 13.212 Mt PM2.5,1.4 Mt BC,2.946 Mt OC,31.584 Mt SO2,23.248 Mt NOx,16.017 Mt NH3,164.856 Mt CO and 35.464 Mt VOCs.The national and regional emissions were gridded with 0.5°× 0.5° resolution for use in air quality models.Larger emissions were found in eastern and central China than in western China.The emissions estimated here are roughly equal to those obtained in previous studies,but with different contributions from because of seasonal changes in residential heating and biomass combustion.Finally,uncertainties in inventories were analyzed.     

Change of NO<Subscript>2</Subscript> column density over Beijing from satellite measurement during the Beijing 2008 Olympic Games

The effect of the air quality ensuring measures for the Beijing 2008 Olympic Games in reducing air pollution during the game period is assessed using the tropospheric NO₂ column density retrieved from Ozone Monitoring Instrument onboard AURA satellite. The basic method of the assessment is the comparison of the NO₂ column densities during the game period with that during the corresponding period of 2005−2007 for the Beijing area, and the comparison among Beijing and neighbouring cities Tianjin and Tangshan, which are of similar situation in air pollution of NO₂ in recent years. The images of tropospheric NO₂ column densities over Northern China during the Beijing 2008 Olympic Games show the remarkable effect of the air quality ensuring measures in reducing NO₂ pollution: the tropospheric NO₂ column density in Beijing is much lower than that in Tianjin and Tangshan, while there were very similar values in the three large cities during the same period of the last three years. About 40% reduction in tropospheric NO₂ column density over the Beijing area is obtained from the assessment during July to August, 2008, a key period of air quality ensuring measures for the Beijing 2008 Olympic Games.     

燃煤电厂锅炉PM2.5现场实测与排放特征研究

采用自设固定源PM_2.5稀释采集系统对陕西省关中地区多个燃煤电厂烟气中的颗粒物开展了现场实测与样品化学源组分分析。结果表明：4个燃煤电厂PM_2.5、PM₁₀占颗粒物比重差异较大（PM_2.5占比范围为6.92%~54.34%,PM₁₀占比范围为36.36%~73.02%）;4个燃煤电厂数浓度水平最高值（2.0×10⁴~4.0×10⁵个/cm³）差异较大,相差约1个数量级;燃煤电厂PM_2.5小粒径段颗粒物质量浓度占比大多较低,但其对PM_2.5数浓度贡献却很大（最小值>95%）,大粒径段颗粒物则相反;煤粉炉PM₁/PM_2.5较大,占比范围为35.29%~51.35%,循环流化床锅炉PM₁/PM_2.5较小,占比范围为16.62%~21.47%;SO₄^2-是燃煤电厂PM_2.5中最丰富的离子成分,各电厂SO₄^2-占总离子浓度比重范围为50.02~65.52%,Na⁺和Ca²⁺位于第2或第3位;各燃煤电厂主要检出无机元素是Si、Al、Ca、Na、Fe、Na等地壳元素;燃煤电厂PM_2.5、PM₁₀和颗粒物的排放因子范围分别为0.001~0.028 kg/t、0.002~0.086 kg/t、0.003~0.236 kg/t;除尘设施组合越复杂先进,排放因子就可能越小。     

An in-situ DRIFTS study in the reaction between NO x and soot on BaAl2O4

The interactions between NO, O2 and their mixture on BaAl2O4, as well as the reaction of NOx with soot in the presence of O2, have been investigated using Diffuse Reflectance Infrared Fourier Transform Spectroscopy （DRIFTS）. NO adsorption produces only nitrites species in the absence of O2. NO2 adsorption produces nitrates species besides nitrites species. The produced nitrites will further react with O2, Osurf^-. and Olattice^2- to form nitrates. The reaction of NOx with soot begins with the reaction of nitrates with soot oxygenated complex （C（O））, which is regarded as the key and rate determining step. A reaction pathway is proposed for the catalyzed reaction of NOx with soot in the presence of O2.     

The impact of HS radicals on the measured rate constant of H<Subscript>2</Subscript>S with OH radicals

The rate constant for the reaction of OH radicals and hydrogen sulfide (H₂S) was studied in different bath gases (including N₂, air, O₂ and He) by using relative technique at 298 K. The small difference of the measured rate constants between N₂ and those with the presence of O₂ suggested possible influence of HS self reaction. Further experiments with NO_x presence for scavenging HS demonstrated this assumption. The rate constant of (5.48±0.12) ×10^–12 cm³ molecule^–1 s^–1 obtained with 4.09 ×10^–4 mol m₃ NO presence may be accurate for estimating the atmospheric lifetime of H2S. The results provided circumstantial evidence that the rapid reaction of HS with N₂O is suspected.     

氧化吸收法同步脱除燃烧烟气中SO2，NOx和CO2的化学热力学及其评价

湿化学法同步脱除烟气中气态污染物是燃烧源大气污染控制的重要方法之一,为探究采用不同氧化吸收策略同时脱除燃烧烟气中SO_2,NO_x和CO_2的可行性,基于化学热力学原理,分析了9种联合氧化吸收策略的性能,具体的氧化吸收策略包括:H_2O_2-NH_3·H_2O,H_2O_2-MDEA,H_2O_2-NaOH,O3-NH_3·H_2O,O3-MDEA,O3-NaOH,NaClO_2-NH_3·H_2O,NaClO_2-MDEA和NaClO_2-NaOH,并提出新的动态加权法对其性能进行综合评价。结果表明:上述所有策略均具有SO_2,NO_x和CO_2捕获的可行性。O3-NaOH,NaClO_2-MDEA和NaOH做吸收剂的氧化吸收溶液分别对单一脱硫、脱硝和脱碳效果最好。当综合考虑同步脱除SO_2,NO_x和CO_2时,NaClO_2-MDEA优于其他策略,其结果可为燃烧烟气中的气体污染物的联合脱除提供参考。     

SNOX法催化脱除模拟烟气中NO○x及SO2实验研究

为了实际考察SNOX方法的工艺条件对烟气中NO○x及SO2的催化脱除效果,针对NO○x的催化还原反应,采用浸渍法制备CuO/γ-Al2O3催化剂,考察了反应温度、空间速度、n(NH3)/n(NO○x)、SO2浓度对NO○x转化率的影响;针对SO2催化氧化反应,采用筛选出的V2O5催化剂,实验考察了反应温度、空间速度、n(O2)/n(SO2)对SO2转化率的影响.以实验研究成果为依据,进行了反应动力学计算.研究结果表明,在实验确定的最佳工艺条件下,NO○x还原率可达87.5%,经两级氧化SO2的转化率达94.3%.     

Pollution plumes observed by aircraft over North China during the IPAC-NC field campaign

Strong pollution emissions from large urban and industrial centres in eastern China are thought to greatly impact regional air quality and global atmospheric chemistry.In this study,we investigate extensive pollution plumes over North China,observed by aircraft during the IPAC-NC(Influence of Pollution on Aerosols and Cloud Microphysics in North China)field campaign in spring 2006.Several pollution plumes were encountered,characterized by sharp and strong increases of SO2and NOx(NO plus NO2)as well as remarkable O3variability.During a flight performed downwind of the megacity Tianjin on 9 April,O3was found to be depleted at NOx>15 ppbv and enhanced at NOx mixing ratios of 6–7 ppbv.Our analysis indicates that the plumes had recently been released by industrial plants,and partly mixed with urban emissions,giving rise to the large-scale transport of air pollution and substantial degradation of air quality.     

化学强化剂提高生物膜填料塔烟气同时脱硫脱氮性能的实验研究

对采用外加化学强化剂提高生物膜填料塔烟气同时脱硫脱氮的性能进行实验研究.结果表明,当按最优化学强化剂添加量添加硝酸镧0.25+硝酸铈0.25 mg/L、硫酸镁0.5 g/L、乙酸钠0.3 g/L时,生物膜填料塔的NOx净化效率可达61.78%,脱硫率为100%.进一步的长时间连续运行实验结果表明,在对SO2的净化效率达到100%的同时,按添加最优化学强化剂条件实验操作的生物膜填料塔的NOx净化效率明显高于对比空白实验的NOx净化效率,其NOx净化效率的平均值提高了14.78%.实验为研究形成提高生物法烟气同时脱硫脱氮性能(尤其对提高烟气脱氮效率)的新型化学强化技术方法奠定了基础.     

Characterization of PM2.5/PM2.5-10 and source tracking in the juncture belt between urban and rural areas of Beijing

Coarse （PM2.5-10） and fine （PM2.5） atmospheric particulate samples were collected in summer and winter during 2005-2007 in the juncture belt between urban and rural areas of Beijing. Elements, ions, organic/elemental carbon （OC/EC） and polynuclear aromatic hydrocarbons （PAHs） were determined to obtain some latest information about the particulate pollution in the juncture belt of Beijing. Particulate matter levels at this site were high as compared with the levels at other sampling sites in Beijing. Pollution elements, secondary ions and PAHs were enriched in fine particles rather than in coarse particles. An obvious seasonal variation of the chemical composition of PM was observed. Source apportionment results showed that secondary components were the largest mass contributor of PM2.5, accounting for 28%; whereas soil-related sources were the largest contributor of PM2.5-10, explaining about 49% of the total mass. The abnormal levels of soil heavy metals at the electronic waste disassembly site in the upwind villages suggested the potential impact of such activities to the environment.     

Second organic aerosol formation by irradiation of α-pinene-NO<Subscript>x</Subscript>-H<Subscript>2</Subscript>O in an indoor smog chamber for atmospheric chemistry and physics

Ozone（O3） and secondary organic aerosol （SOA） are considered to be the most serious secondary air pollutants of concern in most metropolitan areas, as well as for Beijing. In this study, 03 and SOA formation potential of α-pinene, the most abundant biogenic VOCs, is investigated at Tsinghua Indoor Chamber Facility. The experiments were conducted under atmospheric relevant HCs/NOx ratios in both presence and absence of ammonia sulfate seed aerosol. A Scanning Mobility Particle Sizer system （3936, TSI） and a Condensation Particle Counter （3010, TSI） were used to study the SOA formation and a gas chromatograph （GC） equipped with a DB-5 column and a flame ionization detector （FID） was used to measure α-pinene simultaneously. The results show that the presence of ammonia sulfate seed aerosol did not change the formation trend of 03, but significantly contribute to SOA formation. A strong linear relationship （r^2 = 0.90） between SOA yield enhancement （△Y＊） and surface concentration of seed aerosol （PM1, s）has been found, denoting that the PMi, s is the control factor for SOA yield enhancement. And the possible reason for the enhancement is acid-catalyzed heterogeneous reactions.     

柴油机SCR尿素喷射方式研究

鉴于柴油机选择性催化还原系统尿素喷射特性与氮氧（NO_x）转化效率密切相关,本文搭建SCR系统小样试验台,NO和NH₃作为主要试验用气,研究了不同氨氮比和不同温度条件下V₂O₅-WO₃/TiO₂催化剂的氨存储、氨泄漏以及NO_x转化效率的影响.结果表明:氨氮比越大,氨存储量的建立时间越短,NO_x转化效率的提升就越快;氨氮比为0.22时,15 s内NO_x转化效率从0增大到4.3%;当氨氮比为0.30时,15 s内NO_x转化效率从0增大到8.7%;随着氨氮比的增大氨泄漏会提前出现;氨氮比先大后小的喷射方法有利于改善NO_x转化效率.采用氨氮比先大后小的喷射方法,进行ETC标准循环测试,NO_x比排放从8.26 g/（kW·h）减少到1.91 g/（kW·h）,NH₃泄漏均值为5×10-6,峰值为18×10-6,满足国V排放法规要求.      

Trend, seasonal and diurnal variations of atmospheric CO2 in Beijing

The concentration of atmospheric CO₂ in Beijing increased rapidly at a mean growth rate of 3.7% · a⁻¹ from 1993 to 1995. After displaying a peak of (409.7±25.9) μmol · mol⁻¹ in 1995, it decreased slowly. Both the almost stable anthropogenic CO₂ source and increasing biotic CO₂ sink contribute to the drop of CO₂ concentration from 1995 to 2000. The seasonal variation of CO₂ concentration exhibits a clear cycle with a maximum in winter, averaging (426.8±20.6) μmol · mol⁻¹, and a minimum in summer, averaging (369.1±6.1) μmol·mol⁻¹. The seasonal variation of CO₂ concentration is mainly controlled by phenology. The mean diurnal variation of atmospheric CO₂ concentration for a year in Beijing is highly clear: daily maximum CO₂ concentration usually occurs at night, but daily minimum CO₂ concentration does in the daytime, with a mean diurnal difference more than 34.7 μmol·mol⁻¹. It has been revealed that the interannual variations of atmospheric CO₂ concentration in winter and autumn regulated the interannual trend of atmospheric CO₂, whereas the interannual variation of CO₂ concentration in summer affected the general tendency of atmospheric CO₂ in a less degree.     

重庆涪陵大气污染物特征及其与气象要素的关系

利用重庆涪陵2010—2014年空气质量监测数据和同期的气象资料,分析了涪陵地区大气污染物的变化情况与气象要素的相关关系.结果表明:涪陵从2010到2014年空气质量有变好趋势,迎宾大道和兴华中路的空气质量总体较好,AQI指数优良天数分别占87%和85.6%,PM_(10)为涪陵首要污染物.PM_(10),SO_2质量浓度具有周期性变化特征,从1月至12月为先降低后升高的趋势,每年较冷的12月、1月、2月PM_(10)质量浓度值较高,较热的月份质量浓度值较低.NO_2质量浓度年际间变化幅度较小.PM_(10)与气温、降水量、相对湿度、平均风速具有负相关性,与气压具有正相关,即气温越高、降雨量越大、气压越低、风速越大,PM_(10)质量浓度越低.SO_2,NO_2与气温、气压、降水量均为负相关,与相对湿度正相关.不同月份大气污染物与气象要素的相关性存在较大差异.     

Preparation and characterization of LiAlxMn2-xO4 for a supercapacitor in aqueous electrolyte

LiAl_xMn_2—xO₄ (0≤x≤0.5) was synthesized by high temperature solid-state reaction. The structure and morphology of LiAl_xMn_2—xO₄ were investigated by X-ray diffraction and scanning electron microscopy (SEM). The results indicate that all samples show spinel phase. The polyhedral particles turn to club-shaped, then change to small spherical, and finally become agglomerates with increasing Al content. The supercapacitive performances of LiAl_xMn_2—xO₄ were studied by means of galvanostatic charge-discharge, cyclic voltammetry, and alternating current (AC) impedance in 2 mol·L⁻¹ (NH₄)₂SO₄ aqueous solution. The results show that LiAl_xMn_2—xO₄ represents rectangular shape performance in the potential range of 0-1 V. The capacity and cycle performance can be improved by doping Al. The composition of x=0.1 has the maximum special capacitance of 160 F·g⁻¹, which is 1.37 times that of LiMn₂O₄ electrode. The capacitance loss of LiAl_xMn_2—xO₄ with x=0.1 is only about 14% after 100 cycles.     

Ice core dust particulate by XPS-SEM/EDAX

The ice core dust particulate sampled from Mt. Xixabangma has been analyzed by means of X-ray photoelectron spectrometer (XPS) and scanning electron microscope with energy dispersion X-ray analysis (SEM/EDAX). The results show that the contents of SO ₄ ²⁻ and SO ₄ ²⁻ in the surface layer of the dust are significantly higher than those in the subsurface layer (with the exception of organic sulfide). This difference indicates that the surface SO_x has been captured and then chemically converted by the atmospheric dust particulate before its deposition with snow, which is obviously different from those inner layer sulfates and sulfites contained by dust itself. In addition, it has been determined by SEM/EDAX that the dust contains relatively high concentrations of transition metal elements such as Fe and Ti oxides which could function as photocatalysts to the conversion of SO_x adhered on the surface of the dust, and consequently accelerate the deposition of SO_x to snow. Our research also demonstrates that the adsorptive carrying and the catalytic performance of the dust to the atmospheric SO_x are most important causes of the positive correlation between SO ₄ ²⁻ and dust concentration records in ice cores.     

Organic acids: Differences in ice core records between Glacier 1, Tianshan, China and the polar areas

Formate (HCOO-), acetate (CH₃COO-), oxalate (C₂O₄^2-) and pyruvate ((CO)C₂O₄^2-) are detected in a 14.08-m-long ice core recovered in Glacier 1 at the Urumqi riverhead, Tianshan, China, which is a mid-latitude alpine glacier (43°06′N, 86°49′E). the mean concentrations for the four organic acids in recent four decades are (102.8±147.3), (392.3±390.8), (6.9±14.8) and (4.2±8.3) ng/g, respectively, with the ratio for HCOO^-/CH₃COO^- of 0.34 ± 0.43. They represent the major acid components, and originate mainly from anthropogenic emission in the nearby industrial cities. Compared with Greenland and Antarctica, Glacier 1 is much higher in carboxylic acids, which were not subjected to long distance transportation as well as complicated atmospheric reactions. The alpine glacier can be, therefore, useful to reconstructing human pollution scenario to the regional atmosphere.     

Effects of ambient air pollution on allergic rhinitis among preschool children in Changsha, China

Prevalence of allergic rhinitis has rapidly increased among Chinese children,but the reasons are unclear.Recent findings have suggested that exposure to outdoor air pollutants may increase the risk of allergic rhinitis,but the results were inconsistent.This study further investigated the effect of outdoor air pollutants on allergic rhinitis among preschool children.A standardized questionnaire on health,home and environmental factors was conducted for 4988 children aged 1–8 in the city of Changsha,and the concentrations of PM10(particle diameter 10 m),sulfur dioxide(SO2)and nitrogen dioxide(NO2)during 2006–2011 were acquired from the official web of Changsha Environmental Protection Agency.Results showed that the prevalence of children’s doctor diagnosed rhinitis was 8.4%(95%confidence interval[CI]7.0%–10.0%).It was found that the prevalence of rhinitis was not associated with site-specific background concentrations of air pollutants,but significantly positively correlated with age-related accumulative personal exposure of PM10,SO2and NO2.We conclude that age-related accumulative personal exposure to ambient air pollution may play an important role in the development of rhinitis.     

Selective catalytic reduction of NO x by hydrogen over modified Pd/TiO2-Al2O3 catalyst under lean-burn conditions

A series of Ni, Sn and Ca modified Pd/TiO2-Al2O3 catalysts were prepared by the incipient wetness impregnation method and their catalytic performance for the selective catalytic reduction of NOx by H2 was evaluated. The results showed that the NOx conversion and N2 selectivity were improved over Pd-Sn/TiO2-Al2O3 and Pd-Ni/TiO2- Al2O3 catalysts above 200 ℃. More importantly, the N2 selectivity and high-temperature activity of Pd-Sn/TiO2- Al2O3 catalyst was far superior to the single Pd/TiO2-Al2O3 catalyst. The optimal Sn loading was 2 wt.%. X-ray diffrac- tion （XRD） results showed that the interaction between Pd and Sn promotes the dispersion of Pd over TiO2-Al2O3. Temper- ature-programmed reduction （Ha-TPR） results demonstrated that the addition of Sn contributes to the formation of PdO and improving the redox property of Pd/TiOz-Al2O3. The addi- tives of Ni and Sn also facilitated the absorption of NOx and the oxidation of NO to NOa, which play important roles in the selective catalytic reduction of NOx by hydrogen.