U.S. Army Engineer Research and Development Center, Vicksburg, MS, 39180, USA.
U.S. Army Engineer Research and Development Center, Vicksburg, MS, 39180, USA.
Chemosphere. 2017 Jan;166:192-196. doi: 10.1016/j.chemosphere.2016.09.084. Epub 2016 Sep 30.
The mobility and fate of inorganic oxyanions in the environment can be greatly influenced by interactions with natural organic matter (NOM). There is increasing evidence that this interaction between two anionic species is facilitated by cationic bridges, but detailed mechanistic studies into this system are challenging due to the heterogeneous nature of NOM. This work examines the ability of cations (Fe, Cr, Al, or Ga) to form ternary complexes with Suwannee River humic acid (SRHA) and the oxyanions of As (As and As) and Se (Se and Se). Complexes were characterized by separating SRHA from unbound species using size exclusion chromatography coupled to ICP-MS to determine its metal content. Unlike Cr and Fe, the post-transition metal ions Al and Ga proved ineffective at forming ternary complexes with any of the oxyanions, although minor complexation was observed with Ga, suggesting that electrostatic interactions are not the primary driving force behind the stabilization of these ternary complexes. The results also show differences in the behavior of Fe and Cr that may indicate that the two cations stabilize the ternary complexes by different mechanisms.
无机含氧酸根在环境中的迁移和归宿会受到与天然有机物(NOM)相互作用的极大影响。越来越多的证据表明,两种阴离子物种之间的这种相互作用是通过阳离子桥来促进的,但由于 NOM 的异质性,对该体系进行详细的机理研究具有挑战性。这项工作研究了阳离子(Fe、Cr、Al 或 Ga)与苏万尼河腐殖酸(SRHA)以及 As(As 和 As)和 Se(Se 和 Se)的含氧阴离子形成三元配合物的能力。通过使用尺寸排阻色谱法结合电感耦合等离子体质谱法将 SRHA 与未结合的物质分离,从而对配合物进行了表征,以确定其金属含量。与 Cr 和 Fe 不同,后过渡金属离子 Al 和 Ga 与任何含氧阴离子形成三元配合物的效果都不佳,尽管 Ga 与配合物有轻微的络合作用,这表明静电相互作用不是稳定这些三元配合物的主要驱动力。研究结果还表明,Fe 和 Cr 的行为存在差异,这可能表明这两种阳离子通过不同的机制稳定三元配合物。