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新鲜、老化和焚烧生物固体中银纳米颗粒的转化。

Transformation of silver nanoparticles in fresh, aged, and incinerated biosolids.

机构信息

United States Environmental Protection Agency, Office of Research and Development, National Risk Management Research Laboratory, 26 West Martin Luther King Drive, Cincinnati, OH 45268, USA.

出版信息

Water Res. 2013 Aug 1;47(12):3878-86. doi: 10.1016/j.watres.2012.12.041. Epub 2013 Mar 21.

Abstract

The purpose of this research was to assess the chemical transformation of silver nanoparticles (AgNPs) in aged, fresh, and incinerated biosolids in order to provide information for AgNP life cycle analyses. Silver nanoparticles were introduced to the influent of a pilot-scale wastewater (WW) treatment system consisting of a primary clarifier (PC), aeration basin, and secondary clarifier. The partitioning of the AgNPs between the aqueous and solid phases in the system was monitored. Less than 3% of the total AgNPs introduced into the PC were measured at the overflow of the PC. Biosolids were collected from the pilot-scale system for silver analyses, including Ag concentration and speciation. Additionally, biosolids were collected from a publically owned treatment works (POTW). The POTW biosolids were spiked with AgNPs, AgNO3, and Ag2S. One set of the spiked POTW biosolids was aged for one month, and another set was analyzed within 24 h via X-ray absorption spectroscopy (XAS) and scanning electron microscopy/energy dispersive X-ray spectroscopy (SEM-EDX) in order to determine Ag chemical speciation and elemental associations. Replicates of the aged and 24-h samples were also incinerated at 850 °C for 4 h. The residual ash was analyzed by XAS and SEM-EDX. The results show that AgNPs are converted to Ag-sulfur (as sulfide and sulfhydryl) species in fresh and aged biosolids, which is in agreement with other studies on AgNPs in biosolids. Results from linear combination fitting of the XAS data for incinerated biosolids show that a significant proportion of the spiked silver (30-50%) is converted to elemental Ag in the incineration process. In addition to elemental Ag, the results suggest the presence of additional Ag-S complexes such as Ag2SO4 (up to 25%), and silver associated with sulfhydryl groups (26-50%) in the incinerated biosolids. Incinerated biosolids spiked with AgNO3 and Ag2S exhibited similar transformations. These transformations of AgNPs should be accounted for in life-cycle analyses of AgNPs and in management decisions regarding the disposal of incinerated biosolids.

摘要

本研究旨在评估老化、新鲜和焚烧生物固体中银纳米粒子 (AgNP) 的化学转化,以为 AgNP 生命周期分析提供信息。将银纳米粒子引入由初沉池 (PC)、曝气池和二沉池组成的中试规模废水 (WW) 处理系统的进水。监测系统中银纳米粒子在水相与固相之间的分配。在 PC 的溢流中仅检测到引入 PC 的总 AgNP 的不到 3%。从中试规模系统中收集生物固体以进行银分析,包括 Ag 浓度和形态。此外,还从公共污水处理厂 (POTW) 中收集生物固体。将 AgNP、AgNO3 和 Ag2S 加入到 POTW 生物固体中。一组加标 POTW 生物固体经过一个月老化,另一组在 24 小时内通过 X 射线吸收光谱 (XAS) 和扫描电子显微镜/能量色散 X 射线光谱 (SEM-EDX) 进行分析,以确定 Ag 化学形态和元素结合。老化和 24 小时样品的重复也在 850°C 下燃烧 4 小时。用 XAS 和 SEM-EDX 分析残余灰分。结果表明,AgNP 在新鲜和老化的生物固体中转化为 Ag-硫(硫化物和巯基)物种,这与其他关于生物固体中 AgNP 的研究一致。用 XAS 数据进行线性组合拟合的结果表明,在焚烧过程中,大部分加标银(30-50%)转化为元素银。除了元素银之外,结果还表明存在其他 Ag-S 配合物,如 Ag2SO4(高达 25%),以及与巯基结合的银(26-50%)在焚烧生物固体中。用 AgNO3 和 Ag2S 加标的焚烧生物固体表现出类似的转化。在 AgNP 的生命周期分析以及焚烧生物固体处置的管理决策中,应考虑这些 AgNP 的转化。

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