通过Mössbauer和Fe K-Edge X射线吸收光谱学对天然铁双碳酸盐的阴阳位占用
Daria V Boglaienko1, Micah P Prange2, C Heath Stanfield1
1Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United States.
自然的双碳酸盐表现出阴离子乱,其中铁 (Fe) 可以占据 (Ca) 的位置. 这项研究揭示了Ca层中显著的Fe存在,影响矿物质形成.
科学领域:
- 矿物学和结晶学研究.
- 地质化学和材料科学 材料科学
背景情况:
- 双碳酸盐具有酸盐类型的结构,具有交替的阴离子层.
- 完美有序的晶体在热力学上是稳定的,但自然形成会导致阴离子乱,例如抗体替代.
- 了解阴离子排序对于解释矿物质形成路径至关重要.
研究的目的:
- 为了研究自然存在的双碳酸盐样本中阴离子排序的程度.
- 检查铁 (Fe) 在A (Ca) 和B (Mg/Fe) 结晶学位点上的分布对结构秩序的影响.
主要方法:
- 使用了莫斯巴尔光谱,X射线衍射 (XRD),X射线吸收光谱 (XANES和EXAFS) 和能量分散式X射线光谱 (EDS).
- 采用密度函数理论 (DFT) 来解释实验数据并阐明阴离子乱的结构效应.
主要成果:
- 证明名义上由 (Ca) 占据的A位点可以容纳大量的铁 (Fe).
- 量化了阴离子乱的程度及其与晶体结构中Fe分布的相关性.
- 在自然的双碳酸盐中提供了动力捕获障碍的实验证据.
结论:
- 双碳酸盐中的A位点对Fe的适应性比之前所认为的要强.
- 阴离子障碍,特别是Ca位点的Fe替代,对理解矿物形成过程有着显著的影响.
- 综合实验和计算方法为复杂的矿物结构提供了强大的洞察力.
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