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低氧化和高氧化柴油颗粒过滤器对遗传毒性废气成分的影响。

Impact of low- and high-oxidation diesel particulate filters on genotoxic exhaust constituents.

机构信息

Swiss Federal Laboratories for Materials Testing and Research, Uberlandstrasse 129, CH-8600 Dubendorf, Switzerland.

出版信息

Environ Sci Technol. 2010 Feb 1;44(3):1078-84. doi: 10.1021/es9019222.

Abstract

Diesel exhaust contains several genotoxic compounds that may or may not penetrate diesel particulate filters (DPFs). Furthermore, the DPF-supported combustion of soot and adsorbed compounds may lead to the formation of additional pollutants. Herein, we compare the impact of 14 different DPFs on emissions of known genotoxic compounds. During a four year period, these DPFs were tested on a heavy duty diesel engine, operated in the ISO 8178/4 C1 cycle. Integral samples, including gas-phase and particle-bound matter were taken. All DPFs were efficient wall-flow filters with solid particulate number filtration efficiencies eta > 98%. On the basis of their CO, NO, and NO(2) emission characteristics, two different filter families were distinguished. DPFs with high oxidation potential (hox, n = 8) converted CO and NO besides hydrocarbons, whereas low oxidation potential DPFs (lox, n = 6) did not support CO and NO oxidation but still converted hydrocarbons. Lox-DPFs reduced NO(2) from 1.0 +/- 0.3 (engine-out) to 0.42 +/- 0.11 g/kWh (eta = 0.59), whereas hox-DPFs induced a NO(2) formation up to 3.3 +/- 0.7 g/kWh (eta = -2.16). Emissions of genotoxic PAHs decreased for both filter families. Conversion efficiencies varied for individual PAHs and were lower for lox- (eta = 0.31-0.87) than for hox-DPFs (eta = 0.75-0.98). Certain nitro-PAHs were formed indicating that nitration is an important step along PAH oxidation. For example, 1-nitronaphthalene emissions increased from 11 to 17 to 21 microg/L without, with lox-, and hox-DPFs respectively, whereas 2-nitronaphthalene emissions decreased from 25 to 19 to 4.7 microg/L. In contrast to our expectations, the nitration potential of lox-DPFs was higher than the one of hox-DPFs, despite the intense NO(2) formation of the latter. The filters converted most genotoxic PAHs and nitro-PAHs and most soot particles, acting as carriers for these compounds. Hox-DPF exhaust remains oxidizing and therefore is expected to support atmospheric oxidation reactions, whereas lox-DPF exhaust is reducing and consuming oxidants such as ozone, when mixed with ambient air.

摘要

柴油机尾气中含有几种可能穿透柴油机颗粒过滤器(DPF)的遗传毒性化合物。此外,DPF 支持的烟尘和吸附化合物的燃烧可能导致额外污染物的形成。在此,我们比较了 14 种不同的 DPF 对已知遗传毒性化合物排放的影响。在四年期间,这些 DPF 被安装在一台重型柴油机上,在 ISO 8178/4 C1 循环中运行。采集了整体样品,包括气相和颗粒相物质。所有 DPF 都是高效的壁流式过滤器,固体颗粒数量过滤效率 η>98%。根据其 CO、NO 和 NO2 排放特性,区分了两种不同的过滤器家族。具有高氧化电位(hox,n=8)的 DPF 除了烃类之外还能转化 CO 和 NO,而低氧化电位 DPF(lox,n=6)不支持 CO 和 NO 氧化,但仍能转化烃类。lox-DPF 将 NO2 从 1.0±0.3(发动机排出)减少到 0.42±0.11g/kWh(η=0.59),而 hox-DPF 诱导形成的 NO2 高达 3.3±0.7g/kWh(η=-2.16)。两种过滤器家族的遗传毒性多环芳烃排放量均有所减少。个别多环芳烃的转化率因种类而异,lox-DPF(η=0.31-0.87)的转化率低于 hox-DPF(η=0.75-0.98)。某些硝基多环芳烃的形成表明硝化是多环芳烃氧化的重要步骤。例如,1-硝基萘的排放分别从 11μg/L 增加到 17μg/L 和 21μg/L,而 2-硝基萘的排放分别从 25μg/L 减少到 19μg/L 和 4.7μg/L,没有、有 lox-DPF 和 hox-DPF 的情况下。与我们的预期相反,尽管后者产生了强烈的 NO2,lox-DPF 的硝化潜力仍高于 hox-DPF。过滤器转化了大多数遗传毒性多环芳烃和硝基多环芳烃以及大部分烟尘颗粒,作为这些化合物的载体。hox-DPF 尾气仍然具有氧化性,因此预计会支持大气氧化反应,而 lox-DPF 尾气在与环境空气混合时是还原性的,会消耗氧化剂,如臭氧。

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