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中国鄱阳湖洪水/干旱转变过程中沉积物中羟基自由基的爆发。

Burst of hydroxyl radicals in sediments derived by flooding/drought transformation process in Lake Poyang, China.

作者信息

Du Haiyan, Wang Hongxia, Chi Zhilai, Song Na, Wang Changhui, Xu Huacheng

机构信息

State Key Laboratory of Lake Science and Environment, Nanjing Institute of Geography and Limnology, Chinese Academy of Sciences, Nanjing 210008, China.

Department of Statistics, Nanjing Audit University, Nanjing 211815, China.

出版信息

Sci Total Environ. 2021 Jun 10;772:145059. doi: 10.1016/j.scitotenv.2021.145059. Epub 2021 Feb 4.

Abstract

Oxygenation of the reduced species has been regarded as the major source for hydroxyl radical (HO) generation in aquatic environments. Yet, the O-induced formation of HO in lake sediments during the flooding/drought transformation process remained largely unexplored. In this study, two types of sediments from Wucheng (WC) and Nanji (NJ) area in Lake Poyang, China, were collected, respectively, with the burst of HO derived by flooding/drought transformation process exploring via the incubation experiments. Results showed that no obvious HO can be detected for the two sediments during the flooding period, while the concentrations of HO increased rapidly for the flooding/drought transformation process due to the enhanced dissolved oxygen contents. The highest concentrations of HO in the surface sediment were 2.45 ± 0.19 μmol kg for WC sediment and 0.69 ± 0.25 μmol kg for NJ sediment, showing higher burst potential of HO for the former. The contents of Fe(II) in the surface sediments for WC area (589.3 ± 37.29 mg kg) were about two times higher than those for NJ area (308.4 ± 94.01 mg kg) during the flooding period. Oxygenation of the surface Fe(II) contributed significantly to the burst of HO in the flooding/drought transformation process. Moreover, the higher percentage of humic-like substances in WC sediment indicated that the dissolved humic fraction exhibited also important role in the HO formation due to electrons transfer under redox conditions. This study highlighted the importance of reactive reduced species in manipulating the burst of HO in lake sediment, which is essential for understanding the geochemical cycling of several major and trace elements as well as the behavior and fate of the contaminants in aquatic ecosystems.

摘要

还原态物质的氧化作用被认为是水生环境中羟基自由基(HO)产生的主要来源。然而,在洪水/干旱转变过程中,湖泊沉积物中由氧诱导形成HO的情况在很大程度上仍未得到探索。在本研究中,分别采集了中国鄱阳湖吴城(WC)和南矶(NJ)地区的两种沉积物,并通过孵化实验探索洪水/干旱转变过程中HO的爆发情况。结果表明,在洪水期,两种沉积物中均未检测到明显的HO,而在洪水/干旱转变过程中,由于溶解氧含量增加,HO浓度迅速上升。表层沉积物中HO的最高浓度,WC沉积物为2.45±0.19 μmol kg,NJ沉积物为0.69±0.25 μmol kg,表明前者HO的爆发潜力更高。洪水期WC地区表层沉积物中Fe(II)的含量(589.3±37.29 mg kg)约为NJ地区(308.4±94.01 mg kg)的两倍。表层Fe(II)的氧化作用对洪水/干旱转变过程中HO的爆发有显著贡献。此外,WC沉积物中类腐殖质物质的比例较高,这表明在氧化还原条件下,溶解的腐殖质部分由于电子转移在HO形成中也发挥了重要作用。本研究强调了活性还原态物质在控制湖泊沉积物中HO爆发方面的重要性,这对于理解几种主要和微量元素的地球化学循环以及水生生态系统中污染物的行为和归宿至关重要。

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