Water contamination by emerging organic pollutants is calling for advanced methods of remediation such as iron-activated sulfite-based advanced oxidation. Sulfate radical, SO4??, and hydroxyl radical, ?OH, are the primary reactive intermediates formed in the Fe(III)/sulfite system, yet the possible involvement of Fe(IV) produced from Fe(II) and persulfates is unclear. Here we explored the role of Fe(IV) in the Fe(III)/sulfite system by methyl phenyl sulfoxide (PMSO) probe assay, electron paramagnetic resonance spectra analysis, alcohol scavenging experiment, and kinetic simulation. Results show that PMSO is partially transformed into methyl phenyl sulfone (PMSO2), thus evidencing Fe(IV) formation. The remaining degradation of PMSO is due to SO4?? and ?OH. The contribution of Fe(IV) versus free radicals is progressively promoted when the Fe(III)-sulfite reaction proceeds, with an upper limit of 80–90%. The contribution of Fe(IV) versus free radicals increases with Fe(III) and sulfite dosages, and decreases with increasing pH. Overall, our findings demonstrate the involvement of Fe(IV) in the Fe-catalyzed sulfite auto-oxidation process.
The Clean Air Act identifies 189 hazardous air pollutants (HAPs), or "air toxics," associated with a wide range of adverse human health effects. The U.S. Environmental Protection Agency has conducted a modeling study with the Assessment System for Population Exposure Nationwide (ASPEN) to gain a greater understanding of the spatial distribution of concentrations of these HAPs resulting from contributions of multiple emission sources. The study estimates year 1990 long-term outdoor concentrations of 148 air toxics for each census tract in the continental United States, utilizing a Gaussian air dispersion modeling approach. Ratios of median national modeled concentrations to estimated emissions indicate that emission totals without consideration of emission source type can be a misleading indicator of air quality. The results also indicate priorities for improvements in modeling methodology and emissions identification. Model performance evaluation suggests a tendency for underprediction of observed concentrations, which is likely due, at least in part, to a number of limitations of the Gaussian modeling formulation. Emissions estimates for HAPs have a high degree of uncertainty and contribute to discrepancies between modeled and monitored concentration estimates. The model's ranking of concentrations among monitoring sites is reasonably good for most of the gaseous HAPs evaluated, with ranking accuracy ranging from 66 to 100%. 相似文献
The aim of this study was to survey the response of the microbial community to crude oil and the diversity of alkane hydroxylase (alkB) genes in soil samples from the Qinghai-Tibet Plateau (QTP). The enrichment cultures and clone libraries were used. Finally, 53 isolates and 94 alkB sequences were obtained from 10 pristine soil samples after enrichment at 10 °C with crude oil as sole carbon source. The isolates fell into the phyla Proteobacteria, Actinobacteria, and Bacteroidetes, with the dominance of Pseudomonas and Acinetobacter. The composition of degraders was different from polar habitats where Acinetobacter sp. is not a predominant responder of alkane degradative microbial communities. Phylogenetic analysis showed that the alkB genes from isolates and enrichment communities formed eight clusters and mainly related with alkB genes of Pseudomonas, Rhodococcus, and Acinetobacter. The alkB gene diversity in the QTP was lower than marine environments and polar soil samples. In particular, a total of 10 isolates exhibiting vigorous growth with crude oil could detect no crude oil degradation-related gene sequences, such as alkB, P450, almA, ndoB, and xylE genes. The Shannon-Wiener index of the alkB clone libraries from the QTP ranged from 1.00 to 2.24 which is similar with polar pristine soil samples but lower than that of contaminated soils. These results indicated that the Pseudomonas, Acinetobacter, and Rhodococcus genera are the candidate for in situ bioremediation, and the environment of QTP may be still relatively uncontaminated by crude oil. 相似文献