Heterogeneous Sorption of Radionuclides Predicted by Crystal Surface Nanoroughness,Environmental Science & Technology

当前位置： X-MOL 学术 › Environ. Sci. Technol. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Heterogeneous Sorption of Radionuclides Predicted by Crystal Surface Nanoroughness
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2021-11-23 , DOI: 10.1021/acs.est.1c04413
Tao Yuan ₁ , Stefan Schymura ₁ , Till Bollermann ₁ , Konrad Molodtsov ₁ , Paul Chekhonin ₁ , Moritz Schmidt ₁ , Thorsten Stumpf ₁ , Cornelius Fischer ₁

Affiliation

Reactive transport modeling (RTM) is an essential tool for the prediction of contaminants’ behavior in the bio- and geosphere. However, RTM of sorption reactions is constrained by the reactive surface site assessment. The reactive site density variability of the crystal surface nanotopography provides an “energetic landscape”, responsible for heterogeneous sorption efficiency, not covered in current RTM approaches. Here, we study the spatially heterogeneous sorption behavior of Eu(III), as an analogue to trivalent actinides, on a polycrystalline nanotopographic calcite surface and quantify the sorption efficiency as a function of surface nanoroughness. Based on experimental data from micro-focus time-resolved laser-induced luminescence spectroscopy (μTRLFS), vertical scanning interferometry, and electron back-scattering diffraction (EBSD), we parameterize a surface complexation model (SCM) using surface nanotopography data. The validation of the quantitatively predicted spatial sorption heterogeneity suggests that retention reactions can be considerably influenced by nanotopographic surface features. Our study presents a way to implement heterogeneous surface reactivity into a SCM for enhanced prediction of radionuclide retention.

中文翻译：

晶体表面纳米粗糙度预测放射性核素的异质吸附

反应迁移模型 (RTM) 是预测生物圈和地圈中污染物行为的重要工具。然而，吸附反应的 RTM 受到反应性表面位点评估的限制。晶体表面纳米形貌的反应位点密度变化提供了一个“能量景观”，负责异质吸附效率，目前的 RTM 方法没有涵盖。在这里，我们研究了作为三价锕系元素类似物的 Eu(III) 在多晶纳米地形方解石表面上的空间异质吸附行为，并将吸附效率量化为表面纳米粗糙度的函数。基于微焦点时间分辨激光诱导发光光谱 (μTRLFS)、垂直扫描干涉测量和电子背散射衍射 (EBSD) 的实验数据，我们使用表面纳米形貌数据参数化表面复合模型（SCM）。定量预测的空间吸附异质性的验证表明，纳米形貌表面特征会显着影响保留反应。我们的研究提出了一种将异质表面反应性实施到 SCM 中的方法，以增强对放射性核素保留的预测。

更新日期：2021-12-07

点击分享查看原文

点击收藏

阅读更多本刊最新论文本刊介绍/投稿指南11