School of Civil and Environmental Engineering, Georgia Institute of Technology , Atlanta, Georgia 30332, United States.
Environ Sci Technol. 2011 Oct 1;45(19):8368-76. doi: 10.1021/es201696e. Epub 2011 Sep 8.
Our previous study demonstrated that many commercial activated carbon (AC) particles may catalyze transformation of secondary amines to yield trace levels of N-nitrosamines under ambient aerobic conditions. Because of the widespread usage of AC materials in numerous analytical and environmental applications, it is imperative to understand the reaction mechanism responsible for formation of nitrosamine on the surface of ACs to minimize their occurrence in water treatment systems and during analytical methods employing ACs. The study results show that the AC-catalyzed nitrosamine formation requires both atmospheric oxygen and nitrogen. AC's surface reactive sites react with molecular oxygen to form reactive oxygen species (ROS), which facilitate fixation of molecular nitrogen on the carbon surfaces to generate reactive nitrogen species (RNS) likely nitrous oxide and hydroxylamine that can react with adsorbed amines to form nitrosamines. AC's properties play a crucial role as more nitrosamine formation is associated with carbon surfaces with higher surface area, more surface defects, reduced surface properties, higher O(2) uptake capacity, and higher carbonyl group content. This study is a first of its kind on the nitrosamine formation mechanism involving nitrogen fixation on AC surfaces, and the information will be useful for minimization of nitrosamines in AC-based processes.
我们之前的研究表明,在环境有氧条件下,许多商业活性炭(AC)颗粒可能会催化仲胺转化为痕量亚硝胺。由于活性炭材料在众多分析和环境应用中的广泛使用,了解其表面上形成亚硝胺的反应机制至关重要,以尽量减少其在水处理系统和使用活性炭的分析方法中的出现。研究结果表明,活性炭催化的亚硝胺形成需要大气中的氧气和氮气。活性炭表面的反应性位点与分子氧反应形成活性氧物种(ROS),促进氮气在碳表面上的固定,生成活性氮物种(RNS),可能是一氧化二氮和羟胺,它们可以与吸附的胺反应形成亚硝胺。活性炭的性质起着至关重要的作用,因为具有更高表面积、更多表面缺陷、降低的表面性质、更高的氧气吸收能力和更高的羰基含量的碳表面会导致更多的亚硝胺形成。本研究首次涉及到在活性炭表面上涉及氮气固定的亚硝胺形成机制,这些信息将有助于减少基于活性炭的工艺中的亚硝胺。