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痕量金属的存在对水溶液中过氧化氢氧化Sb(III)的影响。

The effect of the presence of trace metals on the oxidation of Sb(III) by hydrogen peroxide in aqueous solution.

作者信息

Elleouet Catherine, Quentel François, Madec Christian-Louis, Filella Montserrat

机构信息

Laboratoire de Chimie Analytique, UMR-CNRS 6521, Université de Bretagne Occidentale, 6, avenue V. Le Gorgeu, C.S. 93837, 29238, Brest Cedex 3, France.

出版信息

J Environ Monit. 2005 Dec;7(12):1220-5. doi: 10.1039/b509802e. Epub 2005 Oct 13.

Abstract

Despite its importance for understanding the behaviour of antimony in the environment, the oxidation kinetics of Sb(III) with natural oxidants is still not well understood. We have studied the oxidation of Sb(III) by hydrogen peroxide on a time scale of hours in the presence of some trace metals, Cu(II), Mn(II), Zn(II) and Pb(II), under pH and concentration conditions close to natural ones. The effects that these trace metals have on Sb(iii) oxidation by hydrogen peroxide vary. Zn(II) had no catalytic effect at all, but Cu(II), Mn(II) and Pb(II) did, though their effects were not uniform. Cu(II) significantly accelerated the reaction, which remained first-order with respect to Sb(III) at any Cu(II) concentration tested. Pb(II) and Mn(II) also enhanced the reaction rates, but the apparent order of the reaction with respect to Sb(III) changed to two. The trace metal effect observed was concentration dependent for Pb(II). The addition of the hydroxyl radical scavenger 2-propanol suggests that the trace metal catalytic effect observed involves the action of hydroxyl radicals, but that they are not responsible for the oxidation of Sb(III) by H2O2 in the absence of trace metals. The fact that Sb(III) can be oxidized by hydroxyl radicals present in water, even if it is not capable of producing them, has important environmental implications because hydroxyl radicals are known to be abundant in many natural waters such as seawater, humic-rich surface waters or rainwater.

摘要

尽管了解锑在环境中的行为具有重要意义,但Sb(III)与天然氧化剂的氧化动力学仍未得到很好的理解。我们研究了在接近自然的pH值和浓度条件下,在一些痕量金属Cu(II)、Mn(II)、Zn(II)和Pb(II)存在的情况下,过氧化氢在数小时的时间尺度上对Sb(III)的氧化作用。这些痕量金属对过氧化氢氧化Sb(III)的影响各不相同。Zn(II)根本没有催化作用,但Cu(II)、Mn(II)和Pb(II)有催化作用,不过它们的作用并不一致。Cu(II)显著加速了反应,在任何测试的Cu(II)浓度下,反应对Sb(III)仍保持一级反应。Pb(II)和Mn(II)也提高了反应速率,但反应对Sb(III)的表观级数变为二级。观察到的痕量金属效应与Pb(II)的浓度有关。加入羟基自由基清除剂2-丙醇表明,观察到的痕量金属催化效应涉及羟基自由基的作用,但在没有痕量金属的情况下,它们并不是H2O2氧化Sb(III)的原因。即使水中的Sb(III)自身不能产生羟基自由基,但它能被水中存在的羟基自由基氧化,这一事实具有重要的环境意义,因为已知在许多天然水体中,如海水、富含腐殖质的地表水或雨水中,羟基自由基含量丰富。

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