Laboratory for Waste Management, Paul Scherrer Institut, Villigen PSI, Switzerland.
Environ Sci Technol. 2013 Jul 2;47(13):6978-86. doi: 10.1021/es304270c. Epub 2013 Jan 11.
Extended X-ray absorption fine structure (EXAFS) and Mössbauer spectroscopy combined with macroscopic sorption experiments were employed to investigate the sorption mechanism of Fe(II) on an iron-free synthetic montmorillonite (Na-IFM). Batch sorption experiments were performed to measure the Fe(II) uptake on Na-IFM at trace concentrations as a function of pH and as a function of sorbate concentration at pH 6.2 and 6.7 under anoxic conditions (O2 < 0.1 ppm). A two-site protolysis nonelectrostatic surface complexation and cation exchange sorption model was used to quantitatively describe the uptake of Fe(II) on Na-IFM. Two types of clay surface binding sites were required to model the Fe(II) sorption, the so-called strong (≡S(S)OH) and weak (≡S(W)OH) sites. EXAFS data show spectroscopic differences between Fe sorbed at low and medium absorber concentrations that were chosen to be characteristic for sorption on strong and weak sites, respectively. Data analysis indicates that Fe is located in the continuity of the octahedral sheet at trans-symmetric sites. Mössbauer spectroscopy measurements confirmed that iron sorbed on the weak edge sites is predominantly present as Fe(II), whereas a significant part of surface-bound Fe(III) was produced on the strong sites (∼12% vs ∼37% Fe(III) species to total sorbed Fe).
扩展 X 射线吸收精细结构(EXAFS)和穆斯堡尔光谱学结合宏观吸附实验,用于研究 Fe(II)在无铁合成蒙脱石(Na-IFM)上的吸附机理。在无氧条件下(O2 < 0.1 ppm),进行了一系列批次吸附实验,以测量 pH 值和 pH 值为 6.2 和 6.7 时的吸附物浓度作为函数,在痕量浓度下测定 Na-IFM 上的 Fe(II)摄取量。采用双位点质子解吸非静电表面络合和阳离子交换吸附模型,定量描述 Fe(II)在 Na-IFM 上的摄取。为了模拟 Fe(II)的吸附,需要两种类型的粘土表面结合位点,即所谓的强(≡S(S)OH)和弱(≡S(W)OH)位点。EXAFS 数据显示,在选择的低和中吸收器浓度下吸附的 Fe 之间存在光谱差异,这分别是吸附在强和弱位点的特征。数据分析表明,Fe 位于对称的反位点处的八面体片的连续性中。穆斯堡尔光谱测量证实,吸附在弱边缘位上的铁主要以 Fe(II)的形式存在,而在强位上产生了相当一部分表面结合的 Fe(III)(∼12%与总吸附 Fe 的 Fe(III)物种相比,∼37%)。