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胶体 α-Al2O3 铕(III)与腐殖质相互作用的宏观和光谱研究。

Colloidal α-Al2O3 Europium(III) and humic substances interactions: a macroscopic and spectroscopic study.

机构信息

Laboratoire de Géochimie des Eaux, Université Paris Diderot , IPGP UMR CNRS 7154, 75025 Paris, Cedex 13, France.

出版信息

Environ Sci Technol. 2011 Apr 15;45(8):3224-30. doi: 10.1021/es102592a. Epub 2010 Nov 19.

DOI:10.1021/es102592a
PMID:21090573
Abstract

Eu(III) sorption onto α-Al(2)O(3) in the presence of purified Aldrich humic acid (PAHA) is studied by batch experiments and time-resolved laser-induced luminescence spectroscopy of Eu(III). Experiments are conducted at varying pH, at 0.1 mol/L NaClO(4), 10(-6) mol/L Eu(III), 1 g/L α-Al(2)O(3) and 28 mg/L PAHA, which assured a complete Eu(III)-PAHA complexation. Adsorption of Eu(III) presents the expected pH-edge at 7, which is modified by addition of PAHA. Presence of Eu(III) slightly increases PAHA sorption throughout the pH range. The evolutions of luminescence spectra and decay times of the binary systems, that is, Eu(III)/α-Al(2)O(3) and Eu(III)/PAHA, indicate a progressive surface- and humic-complexation with increasing pH. The typical biexponential luminescence decay in Eu(III)/PAHA system is also recorded; the fastest deactivation depending barely on pH. In ternary Eu(III)/PAHA/α-Al(2)O(3) system, the existence of a luminescence biexponential decay for all pH means that Eu(III) is always in the direct neighborhood of the humic substance. Below pH 7, the spectra of the ternary system (Eu(III)/PAHA/α-Al(2)O(3)) are not different from the ones of Eu(III)/PAHA system, implying the same complex symmetry. Nevertheless, the increase of luminescence decay time points to a change in PAHA conformation onto the surface.

摘要

在 0.1 mol/L NaClO4、10(-6) mol/L Eu(III)、1 g/L α-Al2O3 和 28 mg/L PAHA 的条件下,通过批实验和时间分辨激光诱导发光光谱法研究了 Eu(III)在纯化的 Aldrich 腐殖酸 (PAHA)存在下对 α-Al2O3 的吸附。实验在不同 pH 值下进行,这保证了 Eu(III)-PAHA 络合物的完全形成。Eu(III)的吸附在 pH 值为 7 时呈现出预期的 pH 边缘,而 PAHA 的加入则改变了这一边缘。PAHA 的存在略微增加了整个 pH 范围内的 PAHA 吸附。二元体系(Eu(III)/α-Al2O3 和 Eu(III)/PAHA)的荧光光谱和衰减时间的演变表明,随着 pH 值的增加,表面和腐殖质络合逐渐增加。还记录了 Eu(III)/PAHA 体系中典型的双指数荧光衰减;最快的失活几乎与 pH 值无关。在三元 Eu(III)/PAHA/α-Al2O3 体系中,所有 pH 值下都存在双指数荧光衰减,这意味着 Eu(III)始终处于腐殖质物质的直接邻近处。在 pH 值低于 7 时,三元体系(Eu(III)/PAHA/α-Al2O3)的光谱与 Eu(III)/PAHA 体系的光谱没有区别,这意味着相同的络合对称性。然而,荧光衰减时间的增加表明 PAHA 在表面上的构象发生了变化。

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