Heterogeneous uptake of gaseous hydrogen peroxide on mineral dust

The heterogeneous uptake processes of hydrogen peroxide on Arizona test dust and two types of authentic Chinese mineral dusts, i.e., Inner Mongolia desert dust and Xinjiang calciferous dust, were investigated using a Knudsen cell reactor coupled with a quadrupole mass spectrometer. The uptake coefficients were measured as a function of the initial concentration of H_2O_2 from 2.6 × 10~(11) to 1.2 × 10~(12)molecules/cm~3, and the temperature dependence of the uptake coefficients was investigated over a range from 253 to 313 K. The concentration of H_2O_2 showed little effect on the uptake coefficients of these heterogeneous processes. As a function of temperature, the initial uptake coefficients decrease with increasing temperature, whereas the steady state uptake coefficients of Arizona test dust and Inner Mongolia desert dust increase with increasing temperature. Implications for the understanding of the uptake processes onto mineral dust samples were also discussed.     

Heterogeneous uptake of nitrogen dioxide on Chinese mineral dust

Mineral dust is one of the major aerosols in the atmosphere. To assess its impact on trace atmospheric gases, in this work we present a laboratory study of the effect of temperature on the heterogeneous reaction of NO₂ on the surface of ambient Chinese dust over the temperature range from 258 to 313 K. The results suggest that nitrogen dioxide could mainly be adsorbed on these types of Chinese mineral dust reversibly with little temperature dependence. Similar to a previous study on NO₂ uptake on mineral aerosols, the uptake coefficients are mainly on the order of 10^− 6 for the Chinese dust, when BET areas are taken into account. HONO was observed as a product, and its formation and decomposition on Chinese mineral dust during the uptake processes were also studied. The complete dataset from this study was compiled with previous literature determinations. Atmospheric implications of the heterogeneous reaction between NO₂ and mineral dust are also discussed, in an effort to understand this important heterogeneous process.     

A case study of Asian dust storm particles: Chemical composition, reactivity to SO2 and hygroscopic properties

Mineral dust comprises a great fraction of the global aerosol loading, but remains the largest uncertainty in predictions of the future climate due to its complexity in composition and physico-chemical properties. In this work, a case study characterizing Asian dust storm particles was conducted by multiple analysis methods, including SEM-EDS, XPS, FT-IR, BET, TPD/mass and Knudsen cell/mass. The morphology, elemental fraction, source distribution, true uptake coefficient for SO₂, and hygroscopic behavior were studied. The major components of Asian dust storm particles are aluminosilicate, SiO₂ and CaCO₃, with organic compounds and inorganic nitrate coated on the surface. It has a low reactivity towards SO₂ with a true uptake coefficient, 5.767×10^-6, which limits the conversion of SO₂ to sulfate during dust storm periods. The low reactivity also means that the heterogeneous reactions of SO₂ in both dry and humid air conditions have little effect on the hygroscopic behavior of the dust particles.     

火电项目环境影响评价中污染控制水平分析

针对国家投资体制改革后我国火电迅猛发展的现象,以内蒙古地区作为研究对象,从2004年内蒙古地区拟建的36个火电项目的环境影响报告书中取得有关资料,分析了这些项目的环境影响控制情况,并对内蒙古地区火电发展的区域环境影响进行讨论.结果表明:即使内蒙古地区拟建项目全部建成投产,在火电装机容量增加33.68×106 kW的情况下,SO₂排放量仅增加0.8×104 t/a;通过对城市中水、矿井疏干水的使用,节约新鲜水用量超过1×108 t/a,环境影响评价中对火电项目的SO2总量控制和节约用水控制效果较好.但是内蒙古地区拟建电厂区域累积用水总量很大,将加剧该地区水资源不足问题,而内蒙古地区作为我国能源输出地,需寻求可持续发展道路.建议加快开展规划环境影响评价,并考虑循环经济发展模式.      

1995~2004年东亚沙尘气溶胶的模拟源汇分布及垂直结构

利用全球气溶胶模式GEM-AQ/EC的1995~2004年10年沙尘气溶胶模拟,探讨了东亚地区沙尘气溶胶源汇分布和垂直结构特征.结果表明,东亚大陆沙尘气溶胶源区主要集中在东亚的沙漠地区,有两大沙尘主要源区:覆盖蒙古国南部及中国内蒙中西部的沙漠地区和南疆的塔克拉玛干沙漠.东亚沙尘排放量春季最大,占全年排放总量的66.81%,四月份达15.29Mt,夏季下降,秋季小幅度回升,冬季最小;东亚沙尘排放量呈现明显的年际变化及增强的趋势.东亚沙尘沉降高值区与源区一致,源区及附近以干沉降为主,远距离传输到中国东北、长江以南及西太平洋包括日本、朝鲜半岛,湿沉降占主导地位;沙尘沉降具有季节变化,其趋势与东亚沙尘排放量的季节变化大致相同,且模拟的10年沉降量呈上升趋势.东亚沙漠地区排放的沙尘主导了东亚沙尘气溶胶的变化,最大的净沙尘汇区集中在紧邻净沙尘源区的黄土高原及华北平原西部.东亚地区春夏秋3个季节均是沙尘的净源区,而冬季强西风急流输入东亚以外的沙尘使东亚整体上为沙尘净接收区.东亚大陆大部分地区,沙尘垂直分布主要集中在对流层低层3km高度以下,在西太平洋地区包括日本、朝鲜半岛沙尘高值中心位于在对流层中层5km高度上下,在沙漠以北地区沙尘垂直廓线的高值出现在对流层中上层6~8km高度.     

Laboratory simulation of SO2 heterogeneous reactions on hematite surface under di erent SO2 concentrations

The variations of sulfate formation and optical coe cients during SO2 heterogeneous reactions on hematite surface under di erent SO2 concentrations were examined using in situ di use reflectance infrared Fourier transform spectroscopy (DRIFTS) and ion chromatograph (IC). Laboratory experiments revealed that within ambient SO2 of 0.51–18.6 ppmv, sulfate product, producing velocity, absorption and backward scattering coe cients showed an increasing trend with SO2 concentration. Under given SO2 concentration, the velocity of sulfate producing performed an evolution of initial increasing, midterm decreasing and final stabilizing. The reactive uptake and Brunauer-Emmett-Teller (BET) uptake coe cients of heterogeneous reactions rose with SO2 and exhibited high reactivities. Considering global warming, this result is important for the knowledge of heterogeneous reactions of SO2 on mineral particle surface in the atmosphere and the assessment of their impacts on radiative forcing.     

Heterogeneous reaction of SO2 on CaCO3 particles: Different impacts of NO2 and acetic acid on the sulfite and sulfate formation

Despite the heterogeneous reaction of sulfur dioxide (SO₂) on mineral dust particles significantly affects the atmospheric environment, the effect of acidic gases on the formation of sulfite and sulfate from this reaction is not particularly clear. In this work, using the in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) technique, we employed a mineral dust particle model (CaCO₃) combined with NO₂ and acetic acid to investigate their effects on the heterogeneous reaction of SO₂ on CaCO₃ particles. It was found that water vapor can promote the formation of sulfite and simulated radiation can facilitate the oxidation of sulfite to sulfate. The addition of NO₂ or acetic acid to the reaction system altered the production of sulfate and sulfite accordingly. There was a synergistic effect between NO₂ and SO₂ that promoted the oxidation of sulfite to sulfate, and a competitive effect between acetic acid and SO₂ that inhibited the formation of sulfite. Moreover, light and water vapor can also affect the heterogeneous reaction of SO₂ with the coexistence of multiple gases. These findings improve our understanding of the effects of organic and inorganic gases and environmental factors on the formation of sulfite and sulfate in heterogeneous reactions.     

Dry deposition of PM10 over the Yellow Sea during Asian dust events from 2001 to 2007

Dry deposition velocities and fluxes of PM10during Asian dust events over the Yellow Sea from 2001 to 2007 were investigated using observation data in Qingdao, China and Jeju, Korea. The dry deposition velocities of PM10 during dust events over the Yellow Sea ranged from 0.19 to 8.17 cm/sec, with an average of 3.38 cm/sec. Dry deposition fluxes of PM10during dust events over the Yellow Sea were in the range of 68.5–2647.1 mg/(m2·day), with an average of 545.4 mg/(m2·day), which is 2–10 times higher than those reported by other studies for both dust and non-dust periods. It was estimated that 2.6 × 1011–48.7 × 1011g dust particles deposit to the Yellow Sea during dust events through dry deposition every year. Compared with the results in previous studies, it was found that the dry deposition of PM10over the Yellow Sea during dust events in the years with high frequency of dust could account for a large or overwhelming fraction of the annual total dry deposition. Backward air mass trajectory analysis showed that dust events influenced Jeju mainly originated from the desert regions located in Mongolia and Inner Mongolia, China. There were 119 backward trajectories influenced both Qingdao and Jeju during 15 dust events from 2001 to 2007, accounting for 61.3% of the total trajectories of 194, indicating that Qingdao and Jeju were usually on the same pathway of dust transport downwind from source areas.     

基于DEA方法的我国大气污染治理效率评价

选取废气治理设施数、废气处理运行费用和工业二氧化硫、工业烟尘、工业粉尘去除量作为大气污染治理的投入与产出变量,运用超效率DEA模型,对我国各省份2004~2009年大气污染治理效率进行研究.结果表明,研究期内我国大气污染治理效率的省际格局基本不变,中部地区大气污染治理效率高于东部和西部地区;江西、内蒙古等省份大气污染治理效率相对较高,而北京、天津、四川、新疆等省份则相对较低;并据此提出了相应的大气污染治理投入的对策建议.     

基于CALIPSO对中国春季一次沙尘暴的研究

文章利用CALIPSO卫星观测资料,结合气溶胶模式模拟,分析了2013年入春以来发生的第1次强沙尘天气过程中的沙尘气溶胶垂直分布特征及输送特性.结果表明:此次沙尘事件有两个源区,南疆盆地(源区一),沙尘先后输送影响我国内蒙古西南部、甘肃、宁夏等地区.2月27日沙尘在甘肃西部河西走廊附近,沙尘气溶胶分布在2~5 km,退偏振比在0.1~0.5之间,色比在0.4~0.8之间;28日新疆地区沙尘气溶胶分布在4~12 km,退偏振比在0.3~0.5,色比在0.5~1.0之间.蒙古国西南部地区(源区二),沙尘先后影响我国内蒙古中西部地区、甘肃、山西北部、陕西北部、河北北部和东北西南部地区,2月28日内蒙古沙尘气溶胶分布在4~11 km,退偏振比在0.2~0.5之间,色比在0.5~1.2之间.     

大气环境中污染物的产生及治理技术的发展

摘要：本文论述了几种典型的大气污染物的种类及产生方式,并介绍了二氧化硫、氖氧化物、光化学烟雾、烟尘的处理技术方法和机理,对不同方法进行了比较,得出了最佳处理技术和方法。     

中国硫沉降数值模拟

采用致酸污染物长距离传输模型ATMOS,对我国2002年排放的SO₂所产生的S沉降分布进行了数值模拟研究.分别将模式输出的ρ(SO₂),SO₄2-湿沉降量与实际监测地面层的ρ(SO₂),降水中SO₄2-湿沉降量进行相关性分析;对我国总S沉降、地面层ρ(SO₂)分布,以及S干、湿沉降分布特点等模拟结果进行详细分析.在此基础上,得到模拟各网格的总S沉降数值,将其与相应的S沉降临界负荷值进行比较,获得95%保证率(RAINS-Asia)下我国1°×1°S沉降超临界负荷分布图.为控制我国的S沉降,对各省SO₂减排的形势进行分析,并提出具体要求.      

中国工业行业的生态效率

中国工业是资源消费和污染物排放的主要源头,解析工业各行业的生态效率可为中国产业结构调整和整体环境质量改善提供必要信息.在分析工业构成并构建工业系统与外部环境之间关系的基础上,选择能源消费和废水、固体废物、SO2、工业烟尘、粉尘等污染物的排放量作为研究的环境影响类别,界定了与这些环境影响相关的生态效率,估算了中国2007年的工业生态效率现状,结果为:能源效率615.5万元·ktce-1;废水和固废方面的生态效率分别为54.3万元·kt-1和1.9万元·t-1;工业SO2、烟尘和粉尘方面的生态效率分别为59.6、169.2和184.6万元·t-1.深入分析了39个工业部门的生态效率,结果表明,以上几种生态效率具有明显的行业不均衡性,表现为不同行业在不同类型生态效率中的工业排序明显不同;与此同时,对于同一种生态效率,不同工业行业的数值可相差几百倍到几万倍,表明通过优化工业结构将具有较大的提高工业生态效率的可能性.     

内蒙古乌达-乌斯太工业园环境单颗粒研究

2015年夏季在内蒙古乌达-乌斯太工业园布点采集了大气颗粒物核孔膜样品16件,采用扫描电镜（SEM-EDX）共表征了1600个单颗粒的形貌和化学组成,结果表明,研究区单颗粒主要为矿物颗粒、燃烧产生颗粒和含硫颗粒3大类,其中矿物颗粒不仅含有硅铝酸盐和碳酸盐这类常见颗粒,还有风化煤矸石和沙尘颗粒这两种特殊颗粒;燃烧产生颗粒不仅有通常的燃煤飞灰、烟尘集合体和絮状碳质颗粒,还有原煤尘颗粒.统计表明,烟尘聚合体、硅铝酸盐和沙尘这三者占颗粒物总数的64%,风化煤矸石尘和原煤尘主要呈现为可吸入颗粒（2.5~10μm）;烟尘聚合体和沙尘则主要为超细颗粒（<1.0μm）.总之,单颗粒分析揭示该典型煤炭工业园区大气颗粒物主要来源：园内燃煤排放和交通,上风向矿区煤炭生产和上风向沙漠自然活动.     

Heterogeneous uptake of NO2 on soils under variable temperature and relative humidity conditions

Heterogeneous reactions of nitrogen dioxide (NO₂) on soils collected from Dalian (S1) and Changsha (S2) were investigated over the relative humidity (RH) range of 5%-80% and temperature range of 278-328 K using a horizontal coated-wall flow tube. The initial uptake coefficients of NO₂ on S2 exhibited a decreasing trend from (10 ± 1.3) × 10^-8 to (3.1 ± 0.5) × 10^-8 with the relative humidity increasing from 5% to 80%. In the temperature effect studies, the initial uptake coefficients of S1 and S2 decreased from (10 ± 1.2) × 10^-8 to (3.8 ± 0.5) × 10^-8 and from (16 ± 2.2) × 10^-8 to (3.8 ± 0.4) × 10^-8 when temperature increased from 278 to 288 K for S1 and from 278 to 308 K for S2, respectively. As the temperature continued to increase, the initial uptake coefficients of S1 and S2 returned to (7.9 ± 1.1) × 10^-8 and (20 ± 3.1) × 10^-8 at 313 and 328 K, respectively. This study shows that relative humidity could influence the uptake kinetics of NO₂ on soil and temperature would impact the heterogeneous chemistry of NO₂.     

长治市沙尘天气污染特征及传输路径解析

以2018年3次沙尘天气为研究对象,分析了PM_2.5和PM₁₀浓度、水溶性离子组分、气象条件和气溶胶光学特征,研究了长治市沙尘天气的典型污染特征和传输路径.结果表明：长治市2018年共8d为受沙尘天气影响日,其中4月份最多（5d）,这与春季大气环流调整,冷暖空气活动频繁有关.沙尘污染发生前一般受西方或西北方冷空气影响,大气层结不稳定,大气环流转为经向环流,平均风速达4m/s以上;沙尘污染过程中PM_2.5/PM₁₀均低于0.3,环境空气中粗颗粒物占比较大,水溶性离子总浓度在PM_2.5中占比下降,Ca²⁺浓度为沙尘污染发生前的4倍以上.冬季沙尘为近地面扩散传输,春夏季沙尘为高空沉降传输,影响范围大,区域传输贡献明显.长治市沙尘重要潜在源区为蒙古国、哈萨克斯坦中部和新疆中北部的荒漠地区,传输路径主要为西北路径和正北路径,其中西北路径为哈萨克斯坦—新疆中北部—内蒙古西部—长治以及新疆中北部—内蒙古西部—长治两条路径,正北路径为蒙古国—内蒙古中部—山西北部—长治.     

长治市沙尘天气污染特征及传输路径解析

以2018年3次沙尘天气为研究对象,分析了PM_2.5和PM₁₀浓度、水溶性离子组分、气象条件和气溶胶光学特征,研究了长治市沙尘天气的典型污染特征和传输路径.结果表明：长治市2018年共8d为受沙尘天气影响日,其中4月份最多（5d）,这与春季大气环流调整,冷暖空气活动频繁有关.沙尘污染发生前一般受西方或西北方冷空气影响,大气层结不稳定,大气环流转为经向环流,平均风速达4m/s以上;沙尘污染过程中PM_2.5/PM₁₀均低于0.3,环境空气中粗颗粒物占比较大,水溶性离子总浓度在PM_2.5中占比下降,Ca²⁺浓度为沙尘污染发生前的4倍以上.冬季沙尘为近地面扩散传输,春夏季沙尘为高空沉降传输,影响范围大,区域传输贡献明显.长治市沙尘重要潜在源区为蒙古国、哈萨克斯坦中部和新疆中北部的荒漠地区,传输路径主要为西北路径和正北路径,其中西北路径为哈萨克斯坦—新疆中北部—内蒙古西部—长治以及新疆中北部—内蒙古西部—长治两条路径,正北路径为蒙古国—内蒙古中部—山西北部—长治.     

Reactive uptake of NO2 on volcanic particles: A possible source of HONO in the atmosphere

The heterogeneous degradation of nitrogen dioxide (NO₂) on five samples of natural Icelandic volcanic particles has been investigated. Laboratory experiments were carried out under simulated atmospheric conditions using a coated wall flow tube (CWFT). The CWFT reactor was coupled to a blue light nitrogen oxides analyzer (NO_x analyzer), and a long path absorption photometer (LOPAP) to monitor in real time the concentrations of NO₂, NO and HONO, respectively. Under dark and ambient relative humidity conditions, the steady state uptake coefficients of NO₂ varied significantly between the volcanic samples probably due to differences in magma composition and morphological variation related with the density of surface OH groups. The irradiation of the surface with simulated sunlight enhanced the uptake coefficients by a factor of three indicating that photo-induced processes on the surface of the dust occur. Furthermore, the product yields of NO and HONO were determined under both dark and simulated sunlight conditions. The relative humidity was found to influence the distribution of gaseous products, promoting the formation of gaseous HONO. A detailed reaction mechanism is proposed that supports our experimental observations. Regarding the atmospheric implications, our results suggest that the NO₂ degradation on volcanic particles and the corresponding formation of HONO is expected to be significant during volcanic dust storms or after a volcanic eruption.     

垃圾焚烧中硫化合物对重金属Pb迁移分布影响

采用管式炉和模拟垃圾对垃圾焚烧中硫化合物(包括S、Na2S、Na2SO3、Na2SO4)、焚烧温度、重金属初始加入浓度以及焚烧停留时间对Pb迁移分布的影响进行了研究.使用ICP-AES分析技术(美国EPA消解方法)对重金属浓度进行测量.结果表明,垃圾焚烧中4种硫化合物的加入均使得Pb在底渣中的分布比例比未加入硫化合物时的分布比例降低.Pb在底渣中的分布比例随加入S和Na2S含量的增加而减少,相应地在飞灰中的分布随S和Na2S加入量的增加而增加,而Pb的迁移分布比例受Na2SO3和Na2SO4含量变化的影响不显著.温度的升高使得Pb向飞灰中的分布比例逐渐增加,整个试验温度范围内Pb在烟气中的分布均为0.初始浓度的增加也使Pb在底渣中的分布比例逐渐升高,飞灰中的分布比例逐渐下降.停留时间的增加会使得Pb在底渣中的分布比例降低,相应地在飞灰中的分布比例会增加.     

内蒙古草地生长季植被变化对气候因子的响应

基于MODIS NDVI数据,研究分析了2000-2010年内蒙古典型草原、草甸草原和荒漠草原生长季NDVI时空变化趋势,探讨不同类型草地生长季NDVI对温度、降水的响应。结果表明,内蒙古草地生长季NDVI整体年增长速率为0.735%,典型草原最为明显,年增长率达到1.063%;但是仍有31.807%的草地NDVI呈现下降趋势,其中典型草原、草甸草原和荒漠草原分别有8.664×10⁴、6.814×10⁴、2.841×10⁴ km²。除东北部草甸草原外,大部分草地生长季NDVI与降水量的相关性高于温度;草地生长季NDVI与温度和降水的相关系数均呈现出草甸草原>典型草原>荒漠草原的变化规律。内蒙古草地植被变化对温度和降水的响应具有滞后作用,且具有明显的经度地带性和纬度地带性特征,其滞后时间随着经度和纬度的增加逐渐减少。