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柴油 soot 纳米颗粒在湿环境中的聚集动力学。

Aggregation Kinetics of Diesel Soot Nanoparticles in Wet Environments.

机构信息

Department of Environmental Sciences, Rutgers, The State University of New Jersey , 14 College Farm Road, New Brunswick, New Jersey 08901, United States.

出版信息

Environ Sci Technol. 2017 Feb 21;51(4):2077-2086. doi: 10.1021/acs.est.6b04575. Epub 2017 Jan 31.

Abstract

Soot produced during incomplete combustion consists mainly of carbonaceous nanoparticles (NPs) with severe adverse environmental and health effects, and its environmental fate and transport are largely controlled by aggregation. In this study, we examined the aggregation behavior for diesel soot NPs under aqueous condition in an effort to elucidate the fundamental processes that govern soot particle-particle interactions in wet environments such as rain droplets or surface aquatic systems. The influence of electrolytes and aqueous pH on colloidal stability of these NPs was investigated by measuring their aggregation kinetics in different aqueous solution chemistries. The results showed that the NPs had negatively charged surfaces and exhibited both reaction- and diffusion-limited aggregation regimes with rates depended upon solution chemistry. The aggregation kinetics data were in good agreement with the classic Derjaguin-Landau-Verwey-Overbeek (DLVO) theory. The critical coagulation concentrations (CCC) were quantified and the Hamaker constant was derived for the soot (1.4 × 10 J) using the colloidal chemistry approach. The study indicated that, depending upon local aqueous chemistry, single soot NPs could remain stable against self-aggregation in typical freshwater environments and in neutral cloud droplets but are likely to aggregate under salty (e.g., estuaries) or acidic (e.g., acid rain droplets) aquatic conditions or both.

摘要

在不完全燃烧过程中产生的烟尘主要由碳质纳米颗粒(NPs)组成,对环境和健康有严重的不利影响,其环境归宿和传输在很大程度上受团聚作用控制。本研究考察了水相条件下柴油机烟尘 NPs 的团聚行为,旨在阐明控制在雨滴或地表水生系统等潮湿环境中烟尘颗粒-颗粒相互作用的基本过程。通过测量不同水相化学条件下的团聚动力学,研究了电解质和水相 pH 值对这些 NPs 胶体稳定性的影响。结果表明,NPs 带负电荷,表现出反应和扩散限制的团聚区,其速率取决于溶液化学。团聚动力学数据与经典的德加古林-朗道-维韦-奥弗贝克(DLVO)理论吻合较好。采用胶体化学方法,通过量化临界聚沉浓度(CCC)并推导出烟尘的哈马克常数(1.4×10 J),对其进行了定量研究。研究表明,根据局部水相化学,单个烟尘 NPs 在典型淡水环境和中性云滴中可能稳定,不会发生自团聚,但在咸水(如河口)或酸性(如酸雨滴)水生条件下或两者皆有时,很可能发生团聚。

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