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在饱和多孔介质中对工程纳米多孔颗粒运移的原位测量。

In-situ measurements of engineered nanoporous particle transport in saturated porous media.

机构信息

Pacific Northwest National Laboratory, Richland, Washington 99354, USA.

出版信息

Environ Sci Technol. 2010 Nov 1;44(21):8190-5. doi: 10.1021/es1015586.

Abstract

Engineered nanoporous particles have become an important class of nanostructured materials that have been increasingly applied in energy, biomedical, and environmental researches and industries. The internal pore surfaces in the particles can be chemically functionalized for environmental applications to sequestrate metals and radionuclide contaminants from groundwater. The fate and transport of the nanoporous particles in subsurface environments, however, have not been studied. Here we present a scanning optical fiber fluorescence profiler that can be used to in situ monitor the transport of fluorescent particles in column systems. Engineered nanoporous silicate particles (ENSPs) that were covalently bounded with fluorescence-emitting, and uranium-chelating ligands in the intraparticle pore domains were synthesized and used as an example to investigate nanoporous particle transport and to demonstrate the application of the developed in situ measurement profiler. The profiler detected an "irreversible" or slowly detached fraction of ENSPs in a sand collector even under thermodynamically unfavorable conditions for particle attachment. Further, the in situ measurement system detected the spatial variability of ENSPs transport that deviated from one-dimensional, homogeneous assumption, which is typically used to model particle transport in column systems. Generally, however, both measured and model-calculated results indicated that the transport of ENSPs was consistent with that of nonporous colloidal particles subjected to coupled reversible attachment/detachment and straining processes. The developed system can also be applied to detect other fluorescent nanostructured or colloidal particles in porous media.

摘要

工程纳米多孔颗粒已经成为一类重要的纳米结构材料,在能源、生物医学和环境研究和工业中得到了越来越广泛的应用。颗粒内部的孔表面可以进行化学功能化,用于环境应用,以从地下水中螯合金属和放射性核素污染物。然而,纳米多孔颗粒在地下环境中的命运和传输尚未得到研究。在这里,我们提出了一种扫描光纤荧光轮廓仪,可用于原位监测柱系统中荧光颗粒的传输。合成了共价结合在颗粒内孔域中具有荧光发射和铀螯合配体的工程纳米多孔硅酸盐颗粒(ENSPs),并将其用作研究纳米多孔颗粒传输的示例,并展示了开发的原位测量轮廓仪的应用。该轮廓仪在热力学上不利于颗粒附着的条件下,在砂集器中检测到 ENSPs 的“不可逆”或缓慢脱落部分。此外,原位测量系统检测到 ENSPs 传输的空间变异性偏离了一维、均匀的假设,这通常用于模拟柱系统中的颗粒传输。然而,一般来说,测量结果和模型计算结果都表明,ENSPs 的传输与受可逆附着/脱落和应变过程耦合的无孔胶体颗粒的传输一致。开发的系统还可用于检测多孔介质中的其他荧光纳米结构或胶体颗粒。

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