Institute for Nuclear Waste Disposal (INE), Karlsruhe Institute of Technology (KIT), Karlsruhe, Germany.
Environ Sci Technol. 2012 Sep 4;46(17):9378-87. doi: 10.1021/es301969m. Epub 2012 Aug 23.
The spatial deposition of polystyrene latex colloids (d = 1 μm) at rough mineral and rock surfaces was investigated quantitatively as a function of Eu(III) concentration. Granodiorite samples from Grimsel test site (GTS), Switzerland, were used as collector surfaces for sorption experiments. At a scan area of 300 × 300 μm(2), the surface roughness (rms roughness, Rq) range was 100-2000 nm, including roughness contribution from asperities of several tens of nanometers in height to the sample topography. Although, an increase in both roughness and [Eu(III)] resulted in enhanced colloid deposition on granodiorite surfaces, surface roughness governs colloid deposition mainly at low Eu(III) concentrations (≤5 × 10(-7) M). Highest deposition efficiency on granodiorite has been found at walls of intergranular pores at surface sections with roughness Rq = 500-2000 nm. An about 2 orders of magnitude lower colloid deposition has been observed at granodiorite sections with low surface roughness (Rq < 500 nm), such as large and smooth feldspar or quartz crystal surface sections as well as intragranular pores. The site-specific deposition of colloids at intergranular pores is induced by small scale protrusions (mean height = 0.5 ± 0.3 μm). These protrusions diminish locally the overall DLVO interaction energy at the interface. The protrusions prevent further rolling over the surface by increasing the hydrodynamic drag required for detachment. Moreover, colloid sorption is favored at surface sections with high density of small protrusions (density (D) = 2.6 ± 0.55 μm(-1), asperity diameter (φ) = 0.6 ± 0.2 μm, height (h) = 0.4 ± 0.1 μm) in contrast to surface sections with larger asperities and lower asperity density (D = 1.2 ± 0.6 μm(-1), φ = 1.4 ± 0.4 μm, h = 0.6 ± 0.2 μm). The study elucidates the importance to include surface roughness parameters into predictive colloid-borne contaminant migration calculations.
作为功能函数,研究了在粗糙矿物和岩石表面上的聚苯乙烯乳胶胶体(d = 1 μm)的空间沉积,使用瑞士 Grimsel 试验场(GTS)的花岗闪长岩样品作为吸附实验的集收表面。在 300×300 μm2 的扫描面积上,表面粗糙度(均方根粗糙度,Rq)范围为 100-2000 nm,包括了样品形貌中几十纳米高度的凸起的粗糙度贡献。尽管,粗糙度和[Eu(III)]的增加都导致胶体在花岗闪长岩表面上的沉积增强,但表面粗糙度主要在低 Eu(III)浓度(≤5×10-7 M)下控制胶体的沉积。在表面粗糙度 Rq = 500-2000 nm 的范围内,在颗粒间孔隙的壁上发现了对花岗闪长岩最高的沉积效率。在表面粗糙度较低(Rq < 500 nm)的花岗闪长岩部分,如大而光滑的长石或石英晶体表面部分以及颗粒内孔隙,胶体的沉积要低大约 2 个数量级。胶体在颗粒间孔隙中的位置特异性沉积是由小尺度的凸起(平均高度 = 0.5 ± 0.3 μm)引起的。这些凸起局部地减小了界面处的总 DLVO 相互作用能。凸起通过增加用于脱离的水动力阻力来阻止胶体在表面上进一步滚动。此外,胶体的吸附在具有高密度小凸起的表面部分(密度(D)= 2.6 ± 0.55 μm-1,凸起直径(φ)= 0.6 ± 0.2 μm,高度(h)= 0.4 ± 0.1 μm)比在具有较大凸起和较低凸起密度的表面部分(D = 1.2 ± 0.6 μm-1,φ = 1.4 ± 0.4 μm,h = 0.6 ± 0.2 μm)更为有利。该研究阐明了在预测胶体携带污染物迁移计算中纳入表面粗糙度参数的重要性。