Department of Civil and Environmental Engineering, Syracuse University, 151 Link Hall, Syracuse, New York 13244, United States.
Environ Sci Technol. 2020 Sep 1;54(17):10654-10667. doi: 10.1021/acs.est.0c02811. Epub 2020 Aug 18.
The Adirondack Mountain region of New York, a historical hotspot for atmospheric sulfur and nitrogen deposition, features abundant lakes that are experiencing browning associated with recovery from acidification. Yet, much remains unknown about the photoreactivity of Adirondack lake waters. We quantified the apparent quantum yields (Φ) of photochemically produced reactive intermediates (RIs), such as excited triplet states of dissolved organic matter (DOM*), singlet oxygen (O), and hydroxyl radicals (OH), for surface waters collected from 16 representative Adirondack lakes. Φ and Φ for native Adirondack lake waters fell within ranges reported for whole waters and DOM isolates from various sources, while Φ were substantially lower than those measured for other aquatic samples. Orthogonal partial least squares and multiple linear regression analyses identified the spectral slope coefficient from 290 to 400 nm () as the most effective predictor of Φ among measured water chemistry parameters and bulk DOM properties. Φ also exhibited divergent responses to controlled pH adjustment and aluminum or iron addition simulating hypothetical scenarios relevant to past and future water chemistry conditions of Adirondack lakes. This study highlights the need for continued research on changes in photoreactivity of acid-impacted aquatic ecosystems in response to browning and subsequent impacts on photochemical processes.
纽约州阿迪朗达克山脉地区是大气硫和氮沉积的历史热点地区,拥有丰富的湖泊,这些湖泊正在从酸化中恢复,因而出现了水色变深的现象。然而,对于阿迪朗达克湖水的光反应性,人们仍知之甚少。我们量化了从 16 个具有代表性的阿迪朗达克湖采集的表层水中光化学产生的反应性中间体(RI)的表观量子产率(Φ),如溶解有机物(DOM*)的激发三重态、单线态氧(O)和羟基自由基(OH)。Φ和Φ的范围与从各种来源采集的整个湖水和 DOM 分离物的报告值相吻合,而Φ值明显低于其他水生样本的测量值。正交偏最小二乘法和多元线性回归分析确定了从 290 到 400nm 的光谱斜率系数()是在所测量的水质参数和总体 DOM 特性中预测Φ的最有效指标。Φ对控制 pH 值调整和铝或铁添加的反应也存在差异,这模拟了与阿迪朗达克湖过去和未来水质条件相关的假设情况。本研究强调了需要继续研究酸化水生生态系统的光反应性变化,以应对水色变深现象以及对光化学过程的后续影响。