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海藻酸盐影响淡水螺对 C 标记的少层石墨烯的团聚状态和摄取:对石墨烯在水生系统中环境归宿的启示。

Alginate affects agglomeration state and uptake of C-labeled few-layer graphene by freshwater snails: Implications for the environmental fate of graphene in aquatic systems.

机构信息

State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210093, China.

Beijing Normal University, School of Environment, State Key Lab Water Environmental Simulation, Beijing 100875, China.

出版信息

Environ Pollut. 2018 Mar;234:513-522. doi: 10.1016/j.envpol.2017.11.087. Epub 2017 Dec 21.

Abstract

Understanding of the interaction of graphene with natural polysaccharides (e.g., alginate) is crucial to elucidate its environmental fate. We investigated the impact of alginate on the agglomeration and stability of C-labeled few-layer graphene (FLG) in varying concentrations of monovalent (NaCl) and divalent (CaCl) electrolytes. Enhanced agglomeration occurred at high CaCl concentrations (≥5 mM) due to the alginate gel networks formation in the presence of Ca. FLG enmeshed within extended alginate gel networks was observed under transmission electron microscope and atomic force microscope. However, background Na competition for binding sites with Ca at the alginate surfaces shielded the gelation of alginate. FLG was readily dispersed by alginate under environmentally relevant ionic strength conditions (i.e., <200 mM Na and <5 mM Ca). In comparison with the bare FLG, the slow sedimentation of the alginate-stabilized FLG (158 μg/L) caused continuous exposure of this nanomaterial to freshwater snails, which ingested 1.9 times more FLG through filter-feeding within 72 h. Moreover, surface modification of FLG by alginate significantly increased the whole-body and intestinal levels of FLG, but reduced the internalization of FLG to the intestinal epithelial cells. These findings indicate that alginate will act as a stabilizing agent controlling the transport of FLG in aqueous systems. This study also provides the first evidence that interaction of graphene with natural polysaccharides affected the uptake of FLG in the snails, which may alter the fate of FLG in aquatic environments.

摘要

理解石墨烯与天然多糖(如海藻酸盐)的相互作用对于阐明其环境归宿至关重要。我们研究了海藻酸盐对标记为 C 的少层石墨烯(FLG)在不同浓度的单价(NaCl)和二价(CaCl)电解质中聚集和稳定性的影响。由于在 Ca 的存在下形成了海藻酸盐凝胶网络,因此在高 CaCl 浓度(≥5 mM)下发生了增强的聚集。在透射电子显微镜和原子力显微镜下观察到 FLG 被扩展的海藻酸盐凝胶网络包裹。然而,由于海藻酸盐表面上 Ca 与 Na 对结合位点的竞争,背景 Na 屏蔽了海藻酸盐的凝胶化。在环境相关的离子强度条件下(即 <200 mM Na 和 <5 mM Ca),FLG 很容易被海藻酸盐分散。与裸 FLG 相比,海藻酸盐稳定的 FLG(158 μg/L)的缓慢沉降导致这种纳米材料持续暴露于淡水蜗牛中,在 72 h 内,这些蜗牛通过滤食摄入的 FLG 增加了 1.9 倍。此外,FLG 表面经海藻酸盐修饰后,显著增加了 FLG 的全身和肠道水平,但减少了 FLG 向肠上皮细胞内化的程度。这些发现表明,海藻酸盐将作为一种稳定剂,控制 FLG 在水相系统中的传输。本研究还首次证明了石墨烯与天然多糖的相互作用会影响 FLG 在蜗牛体内的摄取,这可能会改变 FLG 在水生环境中的归宿。

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