Lyles School of Civil Engineering, Purdue University, West Lafayette, Indiana, USA.
Department of Chemical, Biochemical and Environmental Engineering, University of Maryland Baltimore County, Baltimore, MD, USA.
Environ Sci Process Impacts. 2020 Sep 23;22(9):1852-1864. doi: 10.1039/d0em00219d.
Carbonyl sulfide (COS) and carbon disulfide (CS2) are important atmospheric gases that are formed from organic sulfur precursors present in natural waters when exposed to sunlight. However, it remains unclear how specific water constituents, such as dissolved organic matter (DOM), affect COS and CS2 formation. To better understand the role of DOM, irradiation experiments were conducted in O2-free synthetic waters containing four different DOM isolates, acquired from freshwater to open ocean sources, and the sulfur-based amino acid, cysteine (CYS). CYS is a known natural precursor of COS and CS2. Results indicated that COS formation did not vary strongly with DOM type, although small impacts were observed on the kinetic patterns. COS formation also increased with increasing CYS concentration but decreased with increasing DOM concentration. Quenching experiments indicated that ˙OH was not involved in the rate-limiting step of COS formation, whereas excited triplet states of DOM (3CDOM*) were plausibly involved, although the quenching agents used to remove 3CDOM* may have reacted with the CYS-derived intermediates as well. CS2 was not formed under any of the experimental conditions. Overall, DOM-containing synthetic waters had a limited to no effect towards forming COS and CS2, especially when compared to the higher concentrations formed in sunlit natural waters, as examined previously. The reasons behind this limited effect need to be explored further but may be due to the additional water quality constituents present in these natural waters. The findings of this study imply that multiple variables beyond DOM govern COS and CS2 photoproduction when moving from freshwaters to open ocean waters.
羰基硫 (COS) 和二硫化碳 (CS2) 是重要的大气气体,当暴露在阳光下时,它们由天然水中存在的有机硫前体形成。然而,目前尚不清楚特定的水成分,如溶解有机物 (DOM),如何影响 COS 和 CS2 的形成。为了更好地了解 DOM 的作用,在无氧的合成水中进行了辐照实验,这些水含有四种不同的 DOM 分离物,取自淡水到开阔海洋的来源,以及含硫的氨基酸半胱氨酸 (CYS)。CYS 是 COS 和 CS2 的已知天然前体。结果表明,COS 的形成与 DOM 类型没有强烈的相关性,尽管在动力学模式上观察到了一些微小的影响。COS 的形成也随着 CYS 浓度的增加而增加,但随着 DOM 浓度的增加而减少。猝灭实验表明,˙OH 没有参与 COS 形成的限速步骤,而 DOM 的激发三重态 (3CDOM*) 可能参与其中,尽管用于去除 3CDOM*的猝灭剂可能也与 CYS 衍生的中间体反应。在任何实验条件下都没有形成 CS2。总的来说,含有 DOM 的合成水对 COS 和 CS2 的形成没有明显的影响,尤其是与之前研究过的阳光照射下天然水中形成的较高浓度相比。需要进一步探讨这种有限影响的原因,但可能是由于这些天然水中存在更多的水质成分。这项研究的结果表明,从淡水到开阔海洋,影响 COS 和 CS2 光生产的因素除了 DOM 之外还有很多。