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批量和 EXAFS 技术研究腐殖酸对镍(II)在钙蒙脱石上吸附的影响。

Effect of humic acid on nickel(II) sorption to Ca-montmorillonite by batch and EXAFS techniques study.

机构信息

Key Laboratory of Novel Thin Film Solar Cells, Institute of Plasma Physics, Chinese Academy of Sciences, P.O. Box 1126, Hefei, 230031, PR China.

出版信息

Dalton Trans. 2012 Sep 21;41(35):10803-10. doi: 10.1039/c2dt31057k. Epub 2012 Aug 2.

Abstract

The influence of humic acid (HA) on Ni(II) sorption to Ca-montmorillonite was examined by using a combination of batch sorption experiments and extended X-ray absorption fine structure (EXAFS) spectroscopy technique. The sorption of Ni(II) on HA-montmorillonite hybrids is strongly dependent on pH and temperature. At low pH, the sorption of Ni(II) is mainly dominated by Ni-HA-montmorillonite and outer-sphere surface complexation. The EXAFS results indicate that the first coordination shell of Ni(II) consists of ∼6 O atoms at the interatomic distances of ∼2.04 Å in an octahedral structure. At high pH, binary Ni-montmorillonite surface complexation is the dominant sorption mechanism. EXAFS analysis indicates the formation of mononuclear complexes located at the edges of Ca-montmorillonite platelets at pH 7.5, while a Ni-Al layered double hydroxide (LDH) phase at the Ca-montmorillonite surface formed with pH 8.5. At pH 10.0, the dissolved HA-Ni(II) complexation inhibits the precipitation of Ni hydroxide, and Ni-Al LDH phase forms. The rise of temperature increases the sorption capacity of Ni(II), and promotes Ni-Al LDH phase formation and the growth of crystallites. The results are important to evaluate the physicochemical behavior of Ni(II) in the natural environment.

摘要

采用批量吸附实验和扩展 X 射线吸收精细结构(EXAFS)光谱技术研究了腐殖酸(HA)对 Ca-蒙脱石中 Ni(II)吸附的影响。Ni(II)在 HA-蒙脱石杂化体上的吸附强烈依赖于 pH 值和温度。在低 pH 值下,Ni(II)的吸附主要由 Ni-HA-蒙脱石和外球表面络合作用控制。EXAFS 结果表明,Ni(II)的第一配体壳层由约 6 个 O 原子组成,在八面体结构中原子间距离约为 2.04 Å。在高 pH 值下,二元 Ni-蒙脱石表面络合是主要的吸附机制。EXAFS 分析表明,在 pH 7.5 时,单核配合物位于 Ca-蒙脱石片的边缘形成,而在 pH 8.5 时,在 Ca-蒙脱石表面形成 Ni-Al 层状双氢氧化物(LDH)相。在 pH 10.0 时,溶解的 HA-Ni(II)络合抑制了 Ni 氢氧化物的沉淀,形成了 Ni-Al LDH 相。温度的升高增加了 Ni(II)的吸附容量,促进了 Ni-Al LDH 相的形成和晶粒的生长。这些结果对于评估 Ni(II)在自然环境中的物理化学行为非常重要。

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