Yao Youru, Ma Kang, Li Shiyin, Zhang Yong, Zhang Zhiming, Fang Fengman, Lin Yuesheng, Yin Li, Sun Lian, Zhang Chonghong
Key Laboratory of Earth Surface Processes and Regional Response in the Yangtze-Huaihe River Basin, School of Geography and Tourism, Anhui Normal University, Wuhu, Anhui Province, 241002, China.
School of Environment, Nanjing Normal University, Nanjing, 210023, China.
J Environ Manage. 2023 Oct 27;349:119425. doi: 10.1016/j.jenvman.2023.119425.
The phenomenon of algal blooms resulting from lake eutrophication has the potential to increase the concentration of dissolved organic matter (DOM) and consequently influence the environmental behaviour of arsenic (As). In the subtropical region, the interplay between DOM, Fe/Mn and As becomes complex as Fe/Mn-rich substances from soils and sediments enter eutrophic lakes. The mechanisms by which DOM-Fe/Mn interactions affect the transformation of As species remain uncertain. Therefore, the Chaohu Lake Basin was selected as a representative case study site to investigate the levels of DOM, As, Fe and Mn in the water and to establish their associations. In addition, the interaction mechanism between DOM-Fe/Mn and As was investigated by elucidating the transformation behaviour of DOM-Fe/Mn on As species in a controlled laboratory environment. The results showed that in cases where the coexistence of Fe and Mn concentrations was relatively low (e.g. Fe < ∼0.5 mg/L and Mn < ∼0.6 mg/L), the concentration of As in water would increase proportionally with the simultaneous increase of both Fe and Mn concentrations (As < 5 μg/L). However, when the concentration of either Fe or Mn reached 10 mg/L, the proportion of As complexed by DOM increased significantly, reaching 99.73% and 99.66%, respectively. In the configuration of a metallic bridge, the elements Fe and Mn act as connectors between negatively charged DOM and As, thereby increasing the adsorption capacity of DOM for As. The alcohol and alkene functional groups present on the DOM-Fe/Mn surface show a preference for binding with free species of As in aqueous environments. In addition, the reductive groups on the surface of DOM not only directly convert As(V) to As(III), but also facilitate the reduction of Fe(III) to Fe(II), resulting in the indirect conversion of As(V) to As(III). Thus, this study provides a comprehensive understanding of the transport and transformation processes of arsenic in subtropical eutrophic lakes.
湖泊富营养化导致的藻华现象有可能增加溶解有机物(DOM)的浓度,进而影响砷(As)的环境行为。在亚热带地区,由于来自土壤和沉积物的富含铁/锰的物质进入富营养化湖泊,DOM、铁/锰和砷之间的相互作用变得复杂。DOM-铁/锰相互作用影响砷形态转化的机制仍不确定。因此,选择巢湖流域作为典型案例研究地点,以调查水中DOM、砷、铁和锰的含量,并确定它们之间的关联。此外,通过在可控实验室环境中阐明DOM-铁/锰对砷形态的转化行为,研究了DOM-铁/锰与砷之间的相互作用机制。结果表明,在铁和锰浓度共存相对较低的情况下(例如铁<0.5mg/L且锰<0.6mg/L),水中砷的浓度会随着铁和锰浓度的同时增加而成比例增加(砷<5μg/L)。然而,当铁或锰的浓度达到10mg/L时,DOM络合的砷的比例显著增加,分别达到99.73%和99.66%。在金属桥构型中,铁和锰元素充当带负电荷的DOM与砷之间的连接体,从而提高DOM对砷的吸附能力。DOM-铁/锰表面存在的醇和烯烃官能团表现出在水环境中优先与游离态砷结合的倾向。此外,DOM表面的还原基团不仅直接将As(V)转化为As(III),还促进Fe(III)还原为Fe(II),导致As(V)间接转化为As(III)。因此,本研究全面了解了亚热带富营养化湖泊中砷的迁移和转化过程。