纳米银在水-沉积物中的迁移机制研究
THE TRANSPORTATION OF SILVER NANOPARTICLES BETWEEN WATER AND SEDIMENTS
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摘要: 为研究纳米银(AgNPs)在水体中的迁移、水-沉积物中的分配及转化机制, 采用武汉东湖湖水及沉积物开展模拟实验, 以硝酸银(AgNO3)为参照, 研究了AgNPs和聚乙烯吡咯烷酮包裹纳米银Poly (vinylpyrrolidone)-coated silver nanoparticles(PVP-AgNPs)在上覆水中的沉降、在沉积物中的迁移和形态分布、以及扰动释放过程。结果表明, 上覆水银初始浓度均为75 mg/L的AgNO3、AgNPs及PVP-AgNPs在120h后分别为0.086、0.957和2.770 mg/L, 显示纳米银和硝酸银进入水体后120h内大部分沉入沉积物中, 且经过包裹的纳米银比未包裹的纳米银在水中停留时间稍长; 60d后三种银均主要分布在表层沉积物中, AgNO3体系银含量随深度的增加而逐渐降低, AgNPs和PVP-AgNPs体系银在2 cm以上随深度的增加而增高, 随后逐渐降低, 表明纳米银比硝酸银具有更强的迁移能力。此外, PVP-AgNPs在23 cm层中的银含量占总量的24.6%, 而AgNPs在同一层中含量仅为2.6%, 说明前者的迁移能力更强。在沉积物中, 硫化物和有机物是银的主要结合相。释放实验结果表明, 沉积物中纳米银的释放量远小于硝酸银的释放量, 表明纳米银一旦与沉积物结合就难以再次释放。以上实验结果为评价纳米银的生态安全提供了科学依据。Abstract: Silver nanoparticles (AgNPs), one of the most widely used and fastest developed nanomaterials, have gradually aroused people's concern. But the mechanisms of its transportation and transformation across water-sediments remain unknown. To reveal the water environmental behaviors of AgNPs, indoor simulation experiments using the water and sediments sampled from the East Lake of Wuhan were employed for AgNPs and Poly (vinylpyrrolidone)-coated silver nanoparticles (PVP-AgNPs) test, and silver nitrate (AgNO3) was used as a reference. The sedimentation curves, distribution patterns and different forms of silver in the sediments and the release curves were studied within 60 days. The results indicated that most of silver sank into the sediments after they were added into water for 120 hours. Specially, the Ag concentration in the overlying water dropped from the same initial concentration (75 mg/L) to 0.086 mg/L, 0.957 mg/L and 2.770 mg/L for AgNO3, AgNPs and PVP-AgNPs, respectively. After 60 days, all of the Ag species entered the sediments and stayed in the 5 cm top layers. The silver contents of AgNO3 system gradually decreased with increasing depth, while those of the AgNPs and PVP-AgNPs first increased, and then reduced gradually when reaching 2 cm depth. Furthermore, although 24.6% silver existed in 23 cm layer for PVP-AgNPs system, only 2.6% for AgNPs system were observed in the same layer. These distribution patterns indicated that the transport ability of nano-silver was stronger than that of AgNO3, and PVP-AgNPs was stronger than that of uncoated. Speciation analysis showed that silver was mainly combined by sulfides and organic matters in the sediments. The release experiment results showed that the release of nano-silver aggregated in the sediments was much difficult than that of AgNO3, suggesting that the adverse environmental effects of nano-silver would greatly depressed once they entered the real water environment. The above results provide scientific basis to evaluate the ecological security of nano-silver.