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Fe(II) interaction with cement phases: Method development, wet chemical studies and X-ray absorption spectroscopy
Journal of Colloid and Interface Science ( IF 9.9 ) Pub Date : 2020-11-25 , DOI: 10.1016/j.jcis.2020.11.085
A Mancini 1 , E Wieland 2 , G Geng 3 , B Lothenbach 4 , B Wehrli 5 , R Dähn 2
Affiliation  

Fe(II) interaction with cement phases was studied by means of co-precipitation and sorption experiments in combination with X-ray absorption fine structure (XAFS) spectroscopy. Oxidation of Fe(II) was fast in alkaline conditions and therefore, a methodology was developed which allowed Fe(II) to be stabilised in the sorption experiments and to prepare samples for spectroscopy. X-ray diffraction (XRD) of the co-precipitation samples showed uptake of a small portion of Fe(II) by calcium-silicate-hydrates (C-S-H) in the interlayer indicated by an increase in the interlayer spacing. Fe(II) incorporation by AFm phases was not indicated. Wet chemical experiments using 55Fe radiotracer revealed linear sorption of Fe(II) irrespective of the Ca/Si ratio of C-S-H and equilibrium pH. The Kd values for Fe(II) sorption on C-S-H are more than three orders of magnitude lower as compared to Fe(III), while they are comparable to those of other bivalent metal cations. XAFS spectroscopy showed Fe(II) binding by C-S-H in an octahedral coordination environment. The large number of neighbouring atoms rules out the formation of a single surface-bound Fe(II) species. Instead the data suggest presence of Fe(II) in a structurally bound entity. The data from XRD and XAFS spectroscopy suggests the presence of both surface- and interlayer-bound Fe(II) species.



中文翻译:

Fe(II) 与水泥相的相互作用:方法开发、湿化学研究和 X 射线吸收光谱

通过共沉淀和吸附实验结合 X 射线吸收精细结构 (XAFS) 光谱,研究了 Fe(II) 与水泥相的相互作用。Fe(II) 在碱性条件下的氧化速度很快,因此,开发了一种方法,使 Fe(II) 在吸附实验中稳定并制备用于光谱的样品。共沉淀样品的 X 射线衍射 (XRD) 显示,夹层中的硅酸钙水合物 (CSH) 吸收了一小部分 Fe(II),这表明夹层间距的增加。没有表明 AFm 相掺入 Fe(II)。使用55 Fe 放射性示踪剂的湿化学实验揭示了 Fe(II) 的线性吸附,而与 CSH 的 Ca/Si 比和平衡 pH 值无关。在K d与 Fe(III) 相比,CSH 上的 Fe(II) 吸附值低三个数量级以上,而它们与其他二价金属阳离子的吸附值相当。XAFS 光谱显示 CSH 在八面体配位环境中结合 Fe(II)。大量相邻原子排除了单一表面结合 Fe(II) 物质的形成。相反,数据表明在结构结合的实体中存在 Fe(II)。来自 XRD 和 XAFS 光谱的数据表明存在表面和层间结合的 Fe(II) 物质。

更新日期:2020-11-25
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