Zhu Xinzhe, Chen Daoyi, Wu Guozhong
Division of Ocean Science and Technology, Graduate School at Shenzhen, Tsinghua University, Shenzhen, 518055, China; School of Environment, Tsinghua University, Beijing, 100084, China.
Division of Ocean Science and Technology, Graduate School at Shenzhen, Tsinghua University, Shenzhen, 518055, China.
Chemosphere. 2016 Oct;160:62-70. doi: 10.1016/j.chemosphere.2016.06.041. Epub 2016 Jun 27.
This study aimed to provide insights into the diffusion and aggregation of asphaltenes in the Na-montmorillonite (MMT) interlayer with different water saturation, salinity, interlayer space and humic substances. The molecular configuration, density profile, diffusion coefficient and aggregation intensity were determined by molecular dynamic simulation, while the 3D topography and particle size of the aggregates were characterized by atomic force microscopy. Results indicated that the diffusivity of asphaltenes was up to 5-fold higher in the MMT interlayer filled with fresh water than with saline water (salinity: 35‰). However, salinity had little impact on the asphaltene aggregation. This study also showed a marked decrease in the mobility of asphaltenes with decrease in the pore water content and the interlayer space of MMT. This was more pronounced in the organo-MMT where the humic substances were present. The co-aggregation process resulted in the sequestration of asphaltenes in the hollow cone-shaped cavity of humic substances in the MMT interlayer, which decreased the asphaltene diffusion by up to one-order of magnitude and increased the asphaltene aggregation by about 33%. These findings have important ramifications for evaluating the fate and transport of heavy fractions of the residual oil in the contaminated soils.
本研究旨在深入了解在不同水饱和度、盐度、层间间距和腐殖质条件下,沥青质在钠蒙脱石(MMT)层间的扩散和聚集情况。通过分子动力学模拟确定分子构型、密度分布、扩散系数和聚集强度,同时利用原子力显微镜对聚集体的三维形貌和粒径进行表征。结果表明,与盐水(盐度:35‰)相比,充满淡水的MMT层间中沥青质的扩散率高出5倍。然而,盐度对沥青质聚集的影响较小。本研究还表明,随着孔隙水含量和MMT层间间距的减小,沥青质的迁移率显著降低。在存在腐殖质的有机蒙脱石中,这种情况更为明显。共聚集过程导致沥青质被隔离在MMT层间腐殖质的空心锥形空腔中,这使沥青质扩散降低了一个数量级,并使沥青质聚集增加了约33%。这些发现对于评估污染土壤中残留油重质组分的归宿和迁移具有重要意义。