Identifying source information after river chemical spill occurrences is critical for emergency responses. However, the inverse uncertainty characteristics of this kind of pollution source inversion problem have not yet been clearly elucidated. To fill this gap, stochastic analysis approaches, including a regional sensitivity analysis method, identifiability plot and perturbation methods, were employed to conduct an empirical investigation on generic inverse uncertainty characteristics under a well-accepted uncertainty analysis framework. Case studies based on field tracer experiments and synthetic numerical tracer experiments revealed several new rules. For example, the release load can be most easily inverted, and the source location is responsible for the largest uncertainty among the source parameters. The diffusion and convection processes are more sensitive than the dilution and pollutant attenuation processes to the optimization of objective functions in terms of structural uncertainty. The differences among the different objective functions are smaller for instantaneous release than for continuous release cases. Small monitoring errors affect the inversion results only slightly, which can be ignored in practice. Interestingly, the estimated values of the release location and time negatively deviate from the real values, and the extent is positively correlated with the relative size of the mixing zone to the objective river reach. These new findings improve decision making in emergency responses to sudden water pollution and guide the monitoring network design.
Atmospheric oxidizing capacity (AOC) is an essential driving force of troposphere chemistry and self-cleaning, but the definition of AOC and its quantitative representation remain uncertain. Driven by national demand for air pollution control in recent years, Chinese scholars have carried out studies on theories of atmospheric chemistry and have made considerable progress in AOC research. This paper will give a brief review of these developments. First, AOC indexes were established that represent apparent atmospheric oxidizing ability (AOIe) and potential atmospheric oxidizing ability (AOIp) based on aspects of macrothermodynamics and microdynamics, respectively. A closed study refined the quantitative contributions of heterogeneous chemistry to AOC in Beijing, and these AOC methods were further applied in Beijing-Tianjin-Hebei and key areas across the country. In addition, the detection of ground or vertical profiles for atmospheric OH·, HO2·, NO3· radicals and reservoir molecules can now be obtained with domestic instruments in diverse environments. Moreover, laboratory smoke chamber simulations revealed heterogeneous processes involving reactions of O3 and NO2, which are typical oxidants in the surface/interface atmosphere, and the evolutionary and budgetary implications of atmospheric oxidants reacting under multispecies, multiphase and multi-interface conditions were obtained. Finally, based on the GRAPES-CUACE adjoint model improved by Chinese scholars, simulations of key substances affecting atmospheric oxidation and secondary organic and inorganic aerosol formation have been optimized. Normalized numerical simulations of AOIe and AOIp were performed, and regional coordination of AOC was adjusted. An optimized plan for controlling O3 and PM2.5 was analyzed by scenario simulation. 相似文献
The atmospheric chemical mechanism is an essential component of airshed models used for investigating the chemical behaviors and impacts of species. Since the first tropospheric chemical mechanism was proposed in the 1960s, various mechanisms including Master Chemical Mechanism (MCM), Carbon Bond Mechanism (CBM), Statewide Air Pollution Research Center (SAPRC) and Regional Atmospheric Chemistry Mechanism (RACM) have been developed for different research purposes. This work summarizes the development and applications of these mechanisms, introduces their compositions and lumping methods, and compares the ways the mechanisms treat radicals with box model simulations. CBM can reproduce urban pollution events with relatively low cost compared to SAPRC and RACM, whereas the chemical behaviors of radicals and the photochemical production of ozone are described in detail in RACM. The photolysis rates of some oxygenated compounds are low in SAPRC07, which may result in underestimation of radical levels. As an explicit chemical mechanism, MCM describes the chemical processes of primary pollutants and their oxidation products in detail. MCM can be used to investigate certain chemical processes; however, due to its large size, it is rarely used in regional model simulations. A box model case study showed that the chemical behavior of OH and HO2 radicals and the production of ozone were well described by all mechanisms. CBM and SAPRC underestimated the radical levels for different chemical treatments, leading to low ozone production values in both cases. MCM and RACM are widely used in box model studies, while CBM and SAPRC are often selected in regional simulations. 相似文献
Using a bottom-up estimation method, a comprehensive, high-resolution emission inventory of gaseous and particulate atmospheric pollutants for multiple anthropogenic sectors with typical local sources has been developed for the Harbin-Changchun city agglomeration (HCA). The annual emissions for CO, NOx, SO2, NH3, VOCS, PM2.5, PM10, BC and OC during 2017 in the HCA were estimated to be 5.82 Tg, 0.70 Tg, 0.34 Tg, 0.75 Tg, 0.81Tg, 0.67 Tg, 1.59 Tg, 0.12 Tg and 0.26 Tg, respectively. For PM10 and SO2, the emissions from industry processes were the dominant contributors representing 54.7% and 49.5%, respectively, of the total emissions, while 95.3% and 44.5% of the total NH3 and NOx emissions, respectively, were from or associated with agricultural activities and transportation. Spatiotemporal distributions showed that most emissions (except NH3) occurred in November to March and were concentrated in the central cities of Changchun and Harbin and the surrounding cities. Open burning of straw made an important contribution to PM2.5 in the central regions of the northeastern plain during autumn and spring, while domestic coal combustion for heating purposes was significant with respect to SO2 and PM2.5 emissions during autumn and winter. Furthermore, based on Principal Component Analysis and Multivariable Linear Regression model, air temperature, relative humidity, electricity and energy consumption, and the urban and rural population were optimized to be representative indicators for rapidly assessing the magnitude of regional atmospheric pollutants in the HCA. Such indicators and equations were demonstrated to be useful for local atmospheric environment management. 相似文献
Understanding ozone (O3) formation regime is a prerequisite in formulating an effective O3 pollution control strategy. Photochemical indicator is a simple and direct method in identifying O3 formation regimes. Most used indicators are derived from observations, whereas the role of atmospheric oxidation is not in consideration, which is the core driver of O3 formation. Thus, it may impact accuracy in signaling O3 formation regimes. In this study, an advanced three-dimensional numerical modeling system was used to investigate the relationship between atmospheric oxidation and O3 formation regimes during a long-lasting O3 exceedance event in September 2017 over the Pearl River Delta (PRD) of China. We discovered a clear relationship between atmospheric oxidative capacity and O3 formation regime. Over eastern PRD, O3 formation was mainly in a NOx-limited regime when HO2/OH ratio was higher than 11, while in a VOC-limited regime when the ratio was lower than 9.5. Over central and western PRD, an HO2/OH ratio higher than 5 and lower than 2 was indicative of NOx-limited and VOC-limited regime, respectively. Physical contribution, including horizontal transport and vertical transport, may pose uncertainties on the indication of O3 formation regime by HO2/OH ratio. In comparison with other commonly used photochemical indicators, HO2/OH ratio had the best performance in differentiating O3 formation regimes. This study highlighted the necessities in using an atmospheric oxidative capacity-based indicator to infer O3 formation regime, and underscored the importance of characterizing behaviors of radicals to gain insight in atmospheric processes leading to O3 pollution over a photochemically active region. 相似文献
A concise modeling approach using long-term averaged meteorological data was developed to estimate site-specific concentrations of congeners of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) near a solid waste incinerator. This approach consists of calculation of atmospheric dispersion, dry and wet deposition of gaseous and particle-bound congeners, and non-steady-state concentrations in soil. The predictability of this approach was evaluated by comparison of calculated concentrations of congeners in soil with those measured at eight locations near a municipal solid waste incinerator (MSWI). The variation of these concentrations due to variability of meteorological parameters is small. A considerable number of mean values show good agreement with measured concentrations within a factor of three. The reasonable agreement between calculated and measured concentrations indicates that algorithms for the calculation of vapor-phase deposition and non-steady-state concentrations in soil must be included in the modeling approach for an accurate estimation of the concentrations of congeners of PCDD/Fs emitted from MSWIs to the atmosphere. For a detailed estimation of site-specific concentrations, it is important to specify the bulk density of soil in the evaluated area, together with meteorological parameters. 相似文献
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 NOx, 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 NOx, 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 NOx-independent and NOx-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 NOx, 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 HOx 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 NOx, 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 NOx at 14 urban and suburban sites, and which can take account of possible changes in the regional background of O3. 相似文献