中国城市NOx排放的时空特征与驱动因素:基于空间分异视角

空气质量的改善是当前中国社会经济转型及实现绿色可持续发展的重要目标之一.基于中国268个城市2007-2016年的氮氧化物（Nitrogen Oxide Emissions，NO_x）排放量数据，首先利用自然正交函数（Empirical Orthogonal Function，EOF）分析了268个城市NO_x排放的时空演变特征，然后采用一种新的空间分异性分析方法"地理探测器"从空间异质性视角探讨了NO_x排放的社会经济驱动因素.结果表明：①EOF第一模态特征向量的高值出现在京津冀地区、山东半岛的淄博、潍坊、济宁和临沂，以及长三角的上海、无锡、南京、苏州和杭州；低值则集中在西南的云贵地区、东南的广东、福建及西北的宁夏.②年尺度上NO_x排放的时间系数变化大致呈现先降后升再降的非线性波动.③因子探测分析结果显示，民用汽车总量对NO_x排放分布的影响最大，其次是城市人口和工业总产值.不同风险因子的交互作用均大于单因子的作用，其中，城市人口与人均GDP因子之间的交互作用强度最大，工业总产值与民用汽车总量的交互作用强度次之，人均GDP与城市建设用地面积的交互作用强度排第3.④风险区探测结果显示，社会经济驱动因子中的城市人口、人均GDP、工业总产值、城市建设用地面积、全社会用电量和民用汽车总量均与NO_x排放呈正相关.京津冀、山东半岛和长三角等发达城市为NO_x排放的高风险区，是社会经济驱动因素的多个风险因子共同作用的结果.     

汽油无铅化的关联问题

在实施汽油无铅化的过程中，一个值得引起重视的问题是，要防止“污染替代”发生，即在消除铅污染的同时，防止另一些对环境和健康构成严重威胁的污染物被引入。该文在调研大量中外文献的基础上，综述了目前研究较多的苯、芳烃、烯烃、甲基叔丁基醚等汽油组成和汽油蒸气压对汽车排放正、负方面的影响，提出了制定汽油燃料环保标准，汽油无铅化和安装催化转化器同步进行等建议。     

The lead content and isotopic composition of british coals and their implications for past and present releases of lead to the UK environment

More than 60 coal samples, predominantly from the principal coalfields of England and Wales (25) and Scotland (30), were analysed for lead by AAS and for stable lead isotopes by ICPMS. While the average lead content of Scottish coal, 23.9mg kg^–1, was more than double that of coal from England and Wales, 11.0mg kg^–1, the corresponding mean ²⁰⁶Pb/²⁰⁷Pb ratios (± 1 s.d.) were nearly identical, at 1.181±0.011 and 1.184±0.006, respectively. In the light of the lead isotopic signatures of British coals and of both indigenous (²⁰⁶Pb/²⁰⁷Pb 1.17) and imported Australian (²⁰⁶Pb/²⁰⁷Pb 1.04) lead ores, an approach based on estimated lead emissions from these sources and the deconvolution of the historical lead and ²⁰⁶Pb/²⁰⁷Pb records preserved in lake sediments, peat bogs and archival herbage material indicates that coal combustion became an increasingly significant contributor to atmospheric lead deposition in the UK during the period 1830–1930, especially after the onset of Englands decline as a major location of lead mining and smelting in the late19th Century. Since 1930 and the introduction of leaded petrol, the atmospheric ²⁰⁶Pb/²⁰⁷Pb ratio in the UK has been strongly influenced by carexhaust emissions of comparatively ²⁰⁶Pbdepleted lead of predominantly Australian origin, counterbalanced to some extent by coalcombustion emissions of lead, although these have fallen dramatically since the mid1950s. Nevertheless, with the introduction and substantial uptake of unleaded petrol in the UK during the last decade, even the declining releases from coal, along with contributions from other sources, are continuing to affect the atmospheric lead content and ²⁰⁶Pb/²⁰⁷Pb ratio.     

Monitoring of Hydrocarbon Emissions in a Petroleum Refinery

In a petroleum refinery the hydrocarbon emissions which are mostly fugitive in nature are emitted from process, offsites and periodic accidental releases such as: materials storage & handling, process, equipment leaks, solvent evaporation, combustion sources, waste treatment etc. In India, the monitoring of such emissions in a refinery are limited as also the standards are not set for its limit in ambient air. Hence there is an urgent need for generating a database for such emissions. Recently in India, MoEF/CPCB has set some guidelines under CREP rules for monitoring such emissions in a refinery. A detailed monitoring of the hydrocarbon emissions from different sources in a typical 10.5 MMTPA Indian refinery is undertaken during 1999–2001 and the results are presented. It is observed that the storage tank emissions alongwith process leaks form the major contributor towards fugitive hydrocarbon emissions.     

The Appalachian Mountains' Copper Basin and the concept of environmental susceptibility

The Copper Basin is located within the southern Appalachian Mountains primarily in extreme southeastern Tennessee, USA. It has long been known for its copper mining/smelting and associated chemical industry, as well as its severely injured environment. Virtually all previous commentary on the environmental degradation at this location have focused on human activities and their destructive impact. This article approaches the subject from a different angle, one that emphasizes the interaction between man and nature. The site's physical setting, industrial history, and environmental history are briefly reviewed. The theory then presented here is that certain of the Copper Basin's natural features made its environment unusually vulnerable to the negative impact of copper mining and smelting, especially as practiced around the turn of the century. These features are identified. This reasoning provides the basis for the concept of environmental susceptibility, which is defined and discussed. A few of its applications are mentioned. This study offers a new perspective on the Copper Basin, as well as insights for those whose work involves investigating the man/nature relationship—both past and present.     

Influence of cetane improvers on the air quality in an urban street canyon

The concentration distributions of NO_x, PM, HC and CO in an urban street canyon have been estimated using a two-dimensional air quality numerical model based on the k– turbulent model and the atmospheric convection diffusion equation when various cetane improvers were used in diesel fuels. A wind vortex can be found within the street canyon, and the pollutants emitted from the bottom of the street canyon tend to follow the course of the wind field, moving circularly. The addition of cetane improvers can improve the air quality in a street canyon, all of the pollutants were found to decrease with increasing centane number.     

Spatial variability of ammonium and nitrate in soils near a poultry farm

This paper assesses the distribution of ammonium (NH4+) and nitrate (NO3-) nitrogen deposition in native bushland soil adjacent to an open ventilated poultry farm. The farm is located in Thirlmere 150 km south west of Sydney, Australia. A total of 104 geographically referenced soil cores were obtained from the study area. Soil pH, electrical conductivity (EC), NH4(+) - and NO3(-)-nitrogen concentrations were analysed for variable trends at three depths, i.e. 0-30, 30-60, and 60-90 cm. Significantly higher concentrations of the two nitrogen forms and EC were observed nearer to the farm in the surface soil samples (0-30 cm). The distribution of NH4+, NO3- and EC were all correlated in surface samples throughout the study area. There was no indication of NH4+ and NO3- leaching within soil profile sampled and it appears that weeds and native vegetation had utilised the accumulated nitrogen. The level of N deposition adjacent to the poultry farm decreased downwind due to dispersion of plume and to the buffering effects from the bushland.     

An Estimate of Biogenic Emissions of Volatile Organic Compounds during Summertime in China (7 pp)

Background and Aim An accurate estimation of biogenic emissions of VOC (volatile organic compounds) is necessary for better understanding a series of current environmental problems such as summertime smong and global climate change. However, very limited studies have been reported on such emissions in China. The aim of this paper is to present an estimate of biogenic VOC emissions during summertime in China, and discuss its uncertainties and potential areas for further investigations. Materials and Methods This study was mainly based on field data and related research available so far in China and abroad, including distributions of land use and vegetations, biomass densities and emission potentials. VOC were grouped into isoprene, monoterpenes and other VOC (OVOC). Emission potentials of forests were determined for 22 genera or species, and then assigned to 33 forest ecosystems. The NCEP/NCAR reanalysis database was used as standard environmental conditions. A typical summertime of July 1999 was chosen for detailed calculations. Results and Discussion The biogenic VOC emissions in China in July were estimated to be 2.3×10¹²gC, with 42% as isoprene, 19% as monoterpenes and 39% as OVOC. About 77.3% of the emissions are generated-from forests and woodlands. The averaged emission intensity was 4.11 mgC m⁻² hr⁻¹ for forests and 1.12 mgC m⁻² hr⁻¹ for all types of vegetations in China during the summertime. The uncertainty in the results arose from both the data and the assumptions used in the extrapolations. Generally, uncertainty in the field measurements is relatively small. A large part of the uncertainty mainly comes from the taxonomic method to assign emission potentials to unmeasured species, while the ARGR method serves to estimate leaf biomass and the emission algorithms to describe light and temperature dependence. Conclusions This study describes a picture of the biogenic VOC emissions during summertime in China. Due to the uneven spatial and temporal distributions, biogenic VOC emissions may play an important role in the tropospheric chemistry during summertime. Recommendations and Perspectives Further investigations are needed to reduce uncertainties involved in the related factors such as emission potentials, leaf biomass, species distribution as well as the mechanisms of the emission activities. Besides ground measurements, attention should also be placed on other techniques such as remotesensing and dynamic modeling. These new approaches, combined with ground measurements as basic database for calibration and evaluation, can hopefully provide more comprehensive information in the research of this field. Submission Editor: Prof. Dr. Gerhard Lammel (lammel@recetox.muni.cz)     

Atmospheric lead and bromine in Germany: post-abatement levels,variabilities and trends

INTENTION, GOAL, SCOPE, BACKGROUND: Abatement measures since the 1970s have depleted lead and bromine levels in the atmosphere over large parts of Europe. Our knowledge of the atmospheric cycling of these elements while a several decade-long period of intensive mobilization reaches its end is incomplete. OBJECTIVE: We have characterized the trends in the atmospheric levels of Pb and Br and present-day temporal and spatial variabilities. METHODS: This was achieved by short-term (weeks) and long-term (years) measurements of particulate Pb and Br at various sites in Germany. Samples of atmospheric particulate matter were collected on filter membranes and analyzed by x-ray fluorescence. RESULTS AND DISCUSSION: Average Pb levels at rural and urban inland sites did not exceed concentrations in background aerosols, sampled at a Baltic Sea coastal site, by more than a factor of 3. Due to sea salt, bromide inland particulate Br levels are below those at a coastal site. There, non-sea salt Br, however, is significant as well. Urban Pb and Br levels are not necessarily higher than rural levels. The concentration levels have decreased in such a way that the previously common source, local vehicular traffic emissions, is no longer predominant. Regional rather than local sources have been increasingly determining the concentrations since the 1990s. This is more pronounced for Br than for Pb. We found indications for coal burning and long-range transport as significant Pb sources. For particulate Pb species, a range of ages (elapsed time since Pb emission) has been found. This range shows two maxima corresponding to characteristic times of 72 and 24 h. CONCLUSIONS: The (mean) atmospheric residence time of particulate Pb is longer than the residence time of Br, in particular in the wintertime. The chemical species contributing to atmospheric Pb should be addressed in future studies. RECOMMENDATION AND OUTLOOK: Clearly, despite effective abatement measures, atmospheric Pb will continue to be dominated by anthropogenic mobilization. The influence from long-range transport can be expected to decrease with the effectiveness of abatement programmes in neighbouring countries of the region.     

Source characterization and identification by real-time single particle mass spectrometry

A Real-Time Single Particle Mass Spectrometer, RSMS-3, was deployed to Wilmington, Delaware to study regional and local contributions to fine and ultra-fine urban particulate matter (PM). Approximately two-thirds of PM₁ consisted of internally mixed secondary aerosol. The remaining one-third was externally mixed including biomass burning (13%), fossil fuel combustion (7%) and various industrial sources (13%). In this last group, particle classes containing specific combinations of transition and/or heavy metals gave wind-rose plots consistent with specific point sources. For example, particles containing V and Ni were detected from different wind directions than those containing V and Fe. Samples from two industrial emission stacks, a steel manufacturing facility 10 km away and a coal-fired electrical power generation facility 5 km away, were analyzed and compared to the ambient data set. In each case, a direct correlation was found: a Pb–Zn–K–Na class for the steel manufacturing facility and an Fe–La/Ce class for the power generation facility. The ambient particle classes showed additional small signals from secondary components indicating atmospheric processing. Ambient particle classes containing only a subset of these elements, such as Zn only, Fe only and Pb–K only, were nonspecific, that is, the wind-rose plots were more diffuse and the particles could not be mapped to individual sources. The merits of stack sampling as an aid to interpreting single particle data sets are discussed.