台风影响期间石家庄秋季典型空气污染过程研究

利用PM2.5污染监测数据、气象资料和WRF模式,研究了2013年10月2日至10日石家庄地区秋季一次典型的空气污染过程,结果表明,PM2.5质量浓度的上升和下降阶段与相继出现的台风"菲特"和"丹娜丝"输送气流及其背景场有关,本次污染过程同时受台风系统背景场、副热带高压系统和大陆高压系统协同控制.石家庄PM2.5质量浓度演变分为上升、下降、再上升和下降4个阶段,浓度曲线呈现双峰特征,分别对应台风"菲特"加强、减弱、台风"丹娜丝"加强和减弱阶段.污染过程中,PM2.5日均质量浓度最高值是425μg·m-3,导致这一现象的原因是由于台风"菲特"和"丹娜丝"系统外围东南暖湿气流进入石家庄地区,高空1000、1800和2600 m处出现逆温层,下沉气流最大风速是0.2 m·s-1,覆盖并影响石家庄地区,形成稳定的大气条件,利于PM2.5污染物持续积累,造成石家庄地区PM2.5浓度达到峰值并出现重污染事件.     

2014年10月中国东部持续重污染天气成因分析

2014年10月5─13日中国东部发生了大范围、长时间的(雾)霾及重污染天气. 采用AQI数据分析此次大气重污染过程的时、空演变特征,并应用NCEP(美国国家环境预报中心)再分析资料以及地面、小球探空数据,分析了主要天气型演变、边界层及上空的风场、气象条件特征,以研究此次秋季重污染天气的气象成因和形成过程. 结果表明:①华北、东北是此次污染最为严重的地区,其域内各城市持续数日的污染演变可分为AQI显著上升、持续高值、下降3个阶段. ②在AQI上升阶段(10月6—8日),受大陆高压控制,东部地区出现较弱地方风场和偏南风输送风场,风速在0～2 m/s,相对湿度在22%～86%,3 000 m逆温显著利于污染物积累. ③在持续污染阶段(10月8—11日),海上高压滞留,再加上台风“凤凰”北上阻挡大陆高压影响,使东部地区出现持续4 d的偏南风、偏东风弱风场,风速在1～4 m/s,相对湿度为57%～96%,造成严重污染. ④在AQI下降阶段(10月11—12日),后续大陆高压南下,前部冷锋利于污染物清除,风速达到6 m/s,是AQI降低的主要天气背景场. 因此,持续出现的稳定天气形势是导致此次中国东部重污染天气的主要气象原因.      

Low-temperature CO oxidation over Au-doped 13X-type zeolite catalysts: preparation and catalytic activity

Au-supported 13X-type zeolite (Au/13X) was synthesized using a common deposition–precipitation (DP) method with a solution of sodium carbonate as a precipitate agent. Further testing was conducted to test for catalytic oxidation of CO. A study was conducted on the effects of different preparation conditions (i.e., chloroauric acid concentration, solution temperature, pH of solution, and calcinations temperature) on Au/13X for CO oxidation. In respect to the catalytic activity, the relationship between different the preparation conditions and gold particles in 13X zeolite was analyzed using X-ray diffraction, TEM and XPS. The activity of Au/13X catalysts in CO oxidation was dependent on the chloroauric acid concentration. From XRD results, a higher chloroauric acid concentration induced larger gold nanoparticles, which resulted in lower catalytic activity. Results revealed that higher temperatures induced higher Au loading, homogeneous deposit, and smaller gold clusters on the support of 13X, resulting in higher CO activity. Furthermore, a pH of 5 or 6 generated greater amounts of Au loading and smaller Au particles on 13X than at a pH of 8 or 9. This may be a result of an effective exchange between Au(OH)2Cl2- and Au(OH)₃Cl^- on specific surface sites of zeolite under the pH’s 5 and 6. The sample calcined at 300°C showed the highest activity, which may be due to the sample’s calcined at 200°C inability to decompose completely to metallic gold while the sample calcined at 400°C had larger particles of gold deposited on the support. It can be concluded from this study that Au/13X prepared from a gold solution with an initial chloroauric acid solution concentration of 1.5 × 10^-3 mol·L^-1 gold solution pH of 6, solution temperature of around 90°C, and a calcination temperature of 300°C provides optimum catalytic activity for CO oxidation.     

生物反应器填埋场产甲烷规律的模拟研究

生物反应器填埋场是一种新型的垃圾卫生填埋场,可以加速填埋场的稳定及甲烷的产生.通过模拟试验探讨了生物反应器填埋场在不同操作条件下的产甲烷情况及COD、pH值的变化趋势.试验证明较高的回灌频率有助于垃圾降解、产甲烷速率的升高及渗滤液中COD浓度的降低;污泥接种起缓冲作用,使垃圾的降解及产气速率更趋向平稳;甲烷的产生与COD的降低是同步进行的,因此可以通过COD的变化趋势来判断产甲烷情况.研究建立了反映垃圾含水率影响填埋场产甲烷的数学模型,该模型具有简便、直观、准确等优点.     

Temporal and spatial characteristics of PM2.5 transport fluxes of typical inland and coastal cities in China

Local pollution and the cross-boundary transmission of pollutants between cities have an inevitable impact on the atmosphere. Quantitative assessments of the contribution of transport to pollution in inland and coastal cities are necessary for the implementation of practical, regional, and joint emission control strategies. In this study, the Comprehensive Air Quality Model (CAMx), together with the Weather Research and Forecasting model (WRF), was used to simulate the contributions to pollution of different cities in 2016. The monthly inflow, outflow, and net flux from the ground to the extended layers served as the three main indicators for the analysis of the interactions of PM_2.5 transport between adjacent cities. Between inland and coastal cities, the magnitude of inflow and outflow are larger in the former than in the latter. The inflow flux in the inland cities (Beijing and Shijiazhuang) was 10.6 and 10.7 kt/day, respectively, while that in the coastal cities (Tianjin, Shanghai, Hefei, Nanjing, and Hangzhou) was 9.1, 3.3, 5.8, 4.4, and 3.7 kt/day, respectively. In terms of variation over the year, the strongest inflow in the BTH region occurred in April, followed by October, July, and January, while that in the coastal cities in YRD occurred in January, followed by October, April, and July. Therefore, based on the flux intensity calculations and the transport flux pathways, effective joint control measures can be provided with scientific support, and a better understanding of the evolutionary mechanism among inland and coastal cities can be acquired.     

Adsorption performance of CMK-3 and C-FDU-15 in NO removal at low temperature

CMK-3 and C-FDU-15 samples were synthesized using hard-templating and evaporationinduced self-assembly(EISA) methods,respectively.The pore structures of CMK-3 and CFDU-15 as well as commercial activated carbon were characterized by means of X-ray diffraction,field emission scanning electron microscopy,transmission electron microscopy,and N_2 adsorption–desorption.Adsorption of NO was investigated by means of thermogravimetric analysis,temperature-programmed desorption of NO + O_2,and in situ diffuse reflectance Fourier transform infrared spectroscopy.The results show that the CMK-3 and C-FDU-15 materials possessed ordered and uniform structures.The coadsorption capacity of NO and O_2 decreased in the sequence CMK-3(88.6 mg/g) C-FDU-15(71.7 mg/g) AC(25.3 mg/g).There were two main adsorption species on CMK-3 and CFDU-15:nitrite and nitrate.Nitrite is converted to nitrate easily.However,the adsorption species were more complex on AC,with nitrite being the main species.Moreover,CMK-3 and C-FDU-15 exhibit excellent regeneration efficiency compared with AC.The excellent NO adsorption performance of CMK-3 and C-FDU-15 was associated with their ordered mesoporous structures and high surface areas.The research provides more options for NO adsorption in the future.     

石家庄市冬季一次重污染过程分析与反馈效应研究

为深入探究高ρ（PM_2.5）地区重污染过程的发展变化规律,以石家庄市一次重污染过程（2017年1月13-20日）为例,结合空气质量监测数据、PM_2.5组分测试数据、气象观测资料,从重污染发展阶段（简称"P1阶段"）、维持阶段（简称"P2阶段"）和清除阶段（简称"P3阶段"）分析PM_2.5及其化学组分的变化特征、气象条件和高低空天气形势演变特征,并利用WRF-Chem模型定量研究重污染过程气溶胶反馈效应对典型气象要素的影响.结果表明:①此次重污染过程属于逐步累积增长、快速清除型,在P2阶段ρ（PM_2.5）平均值为241.0 μg/m3,最大值为367.5 μg/m3.②P1和P2阶段高低空大气环流配置稳定,大气边界层高度范围为620.6~712.2 m,风速范围为1.3~2.5 m/s,相对湿度范围为60%~80%.③P2阶段SOR（硫氧化率）和NOR（氮氧化率）均为0.3,ρ（SNA）（SNA为SO₄2-、NO₃-和NH₄+的统称）为128.8 μg/m3,占ρ（PM_2.5）的56.2%;OM[有机质,ρ（OM）=ρ（POA）+ρ（SOA）,其中,POA为一次有机气溶胶,SOA为二次有机气溶胶]是除SNA以外的第二大组分,在P1和P3阶段ρ（POA）大于ρ（SOA）,而在P2阶段ρ（SOA）与ρ（POA）相等,均为28.0 μg/m3,表明在重污染过程中二次污染严重;整个污染过程ρ（NO₃-）/ρ（SO₄2-）为1.0,表明石家庄市移动源和固定源对ρ（PM_2.5）贡献相当.④WRF-Chem模型模拟结果表明,太阳辐射量、温度和大气边界层高度受气溶胶反馈效应的影响在P2阶段的下降量分别为75.1 W/m2、2.7℃和109.9 m,比P1阶段分别高33.6%、91.4%和18.6%,比P3阶段分别高147.0%、305.3%和24.1%.研究显示,此次静稳天气下的重污染过程二次污染严重,气溶胶反馈效应整体使得太阳辐射量、温度和大气边界层高度均向不利于污染扩散的趋势发展,造成石家庄市的ρ（PM_2.5）进一步增加.      

Characterization of aircraft emissions and air quality impacts of an international airport

Beijing Capital International Airport(ZBAA) is the world's second busiest airport. In this study, the emissions of air pollutants from aircraft and other sources at ZBAA in 2015 were estimated using an improved method, which considered the mixing layer height calculated based on aircraft meteorological data relay(AMDAR), instead of using the height(915 m)recommended by ICAO. The yearly emissions of NO_x, CO, VOCs, SO_2, and PM_(2.5) at the airport were 8.76 × 10~3, 4.43 × 10~3, 5.43 × 10~2, 4.80 × 10~2, and 1.49 × 10~2 ton/year, respectively. The spatial–temporal distribution of aircraft emissions was systematically analyzed to understand the emission characteristics of aircraft. The results indicated that NOxwas mainly emitted during the take-off and climb phases, accounting for 20.5% and 55.5% of the total emissions. CO and HC were mainly emitted during the taxi phase, accounting for 91.6%and 92.2% of the total emissions. Because the mixing layer height was high in summer, the emissions of aircraft were at the highest level throughout the year. Based on the detailed emissions inventory, four seasons simulation using WRF-CMAQ model was performed over the domain surrounding the airport. The results indicated that the contribution to PM_(2.5) was relatively high in winter; the average impact was about 1.15 μg/m~3 within a radius of1 km around the airport. Meanwhile, the near surroundings and southwest areas of the airport are the most sensitive to PM_(2.5).     

Characteristics of ozone and ozone precursors (VOCs and NOx) around a petroleum refinery in Beijing, China

A field measurement campaign for ozone and ozone precursors(VOCs and NOx) was conducted in summer 2011 around a petroleum refinery in the Beijing rural region. Three observation sites were arranged, one at southwest of the refinery as the background, and two at northeast of the refinery as the downwind receptors. Monitoring data revealed the presence of serious surface O3 pollution with the characteristics of high average daily mean and maximum concentrations(64.0 and 145.4 ppbV in no-rain days, respectively) and multi-peak diurnal variation. For NOx, the average hourly concentrations of NO2 and NO were in the range of 20.5–46.1 and 1.8–6.4 ppbV, respectively. For VOC measurement, a total of 51 compounds were detected. Normally, TVOCs at the background site was only dozens of ppbC, while TVOCs at the downwind sites reached several hundreds of ppbC. By subtracting the VOC concentrations at background, chemical profiles of VOC emission from the refinery were obtained, mainly including alkanes(60.0% ± 4.3%), alkenes(21.1% ± 5.5%) and aromatics(18.9% ± 3.9%). Moreover, some differences in chemical profiles for the same measurement hours were observed between the downwind sites; the volume ratios of alkanes with low reactivity and those of alkenes with high reactivity respectively showed an increasing trend and a decreasing trend. Finally, based on temporal and spatial variations of VOC mixing ratios, their photochemical degradations and dispersion degradations were estimated to be 0.15–0.27 and 0.42–0.62, respectively, by the photochemical age calculation method, indicating stronger photochemical reactions around the refinery.     

Excellent performance of Cu-Mn/Ti-sepiolite catalysts for low-temperature CO oxidation

The Ti-modified sepiolite (Ti-Sep)-supported Mn-Cu mixed oxide (yMn5Cu/Ti-Sep) catalysts were synthesized using the co-precipitation method. The materials were characterized by the X-ray diffraction scanning electron microscope, N₂ adsorption-desorption, H₂-TPR, O₂-TPD, and XPS techniques, and their catalytic activities for CO oxidation were evaluated. It was found that the catalytic activities of yMn5Cu/Ti-Sep were higher than those of 5Cu/Ti-Sep and 30Mn/Ti-Sep, and the Mn/Cu molar ratio had a distinct influence on catalytic activity of the sample. Among the yMn5Cu/Ti- Sep samples, the 30Mn5Cu/Ti-Sep catalyst showed the best activity (which also outperformed the 30Mn5Cu/Sep catalyst), giving the highest reaction rate of 0.875 × 10^–3 mmol·g^–1·s^–1 and the lowest T _50% and T _100% of 56°C and 86°C, respectively. Moreover, the 30Mn5Cu/Ti-Sep possessed the best low-temperature reducibility, the lowest O₂ desorption temperature, and the highest surface Mn³⁺/Mn⁴⁺ atomic ratio. It is concluded that factors, such as the strong interaction between the copper or manganese oxides and the Ti-Sep support, good low-temperature reducibility, and good mobility of chemisorbed oxygen species, were responsible for the excellent catalytic activity of 30Mn5Cu/Ti-Sep.

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