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The influence of Si(IV) on the reactivity of [ Fe(III)]/[ Fe(II)] couples for 2-nitrophenol reduction in gamma-Al2O3 suspensions

机译:Si(iv)对[Fe(III)] / [Fe(II)]对2-硝基苯酚还原的反应性的影响γ-Al2O3悬浮液中的影响

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摘要

In a natural environment, Fe(II) adsorbed onto the surfaces of natural particles to form various surface complex species can influence the transformation of contaminants. The reductive reactivity of the [ Fe(III)]/[ Fe(II)] couples are close correlated with the surrounding conditions. In this study, we investigated the effects of Si(IV) on the reductive reactivity of [ Fe(III)]/[ Fe(II)] couples adsorbed onto gamma -Al2O3. Experiments were conducted under different conditions to investigate the effects of Si(IV) on the reactivity of [ Fe(III)]/[ Fe(II)] couples for 2-nitrophenol (2-NP, selected as the model pollutant) reduction in gamma-Al2O3 suspensions. Kinetics results revealed that chemical adsorption is the rate limiting step in Fe(II) and Si(IV) adsorption processes and the reduction of 2-NP is an endothermic reaction. The linear correlations between the reduced peak oxidation potential (E-p) (versus SCE) and 2-NP reduction rate (ln k), and between the adsorbed Fe(II) density (rho Fe(II)) and ln k, illustrated that E-p and rho Fe(II) are two key factors in the inhibiting effects of Si(IV) on the reductive reactivity of Fe(III)/Fe(II) couples on gamma-Al2O3. The results of Fe K-edge X-ray absorption spectroscopy revealed that the increase of Si(IV) concentration resulted in the gradual change in the composition of the adsorbed Fe species from pure AlOFe+ (gamma-Al2O3 surface-bound Fe(II) species with higher reductive reactivity) to a mixture of AlOFe+ and SiOFe+ (SiO2 surface-bound Fe(II) species with lower reductive reactivity), leading to the decrease in rho Fe(II), the positive shift in E-p, the increase in activation energy (E-a), and consequently the decrease in the reduction rate (ln k) of 2-NP.
机译:在天然环境中,吸附在天然颗粒表面上以形成各种表面复合物物质的Fe(II)可以影响污染物的转化。 [Fe(III)] / [Fe(II)]夫妇与周围条件相关的还原反应性。在这项研究中,我们研究了Si(iv)对吸附在γ-al2O3上的[Fe(III)] / [Fe(II)]夫妻的还原性反应性的影响。在不同条件下进行实验,以研究Si(IV)对2-硝基苯酚(2-NP,作为模型污染物)的反应性的影响对[Fe(III)] / [Fe(II)]夫妇的影响Gamma-Al2O3悬浮液。动力学结果显示,化学吸附是Fe(II)和Si(IV)吸附过程的速率限制步骤,并且2-NP的还原是吸热反应。降低峰氧化电位(EP)(相对于SCE)和2-NP还原率(LN k)之间的线性相关性,以及吸附的Fe(II)密度(Rho Fe(II))和LN K,示出了该EP rho fe(ii)是Si(iv)对γ-Al2O3对Fe(III)/ Fe(II)夫妇的还原性反应性抑制作用的两个关键因素。 Fe K-Edge X射线吸收光谱的结果显示,Si(IV)浓度的增加导致来自纯铝+(γ-Al2O3表面结合Fe(II)物种的吸附Fe物种组合物的逐渐变化较高的还原反应性)以熟料+和SiOFE +(SiO 2表面结合的Fe(II)物种的混合物,导致Rho Fe(II)的降低,EP的正换档,激活能量的增加(EA),因此,2-NP的减少率(LN K)的降低。

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  • 来源
    《RSC Advances》 |2018年第14期|共8页
  • 作者单位

    Guangdong Inst Ecoenvironm Sci &

    Technol Guangdong Key Lab Integrated Agroenvironm Pollut Guangzhou 510650 Guangdong Peoples R China;

    Natl Taiwan Univ Dept Agr Chem Taipei 10617 Taiwan;

    Guangdong Inst Ecoenvironm Sci &

    Technol Guangdong Key Lab Integrated Agroenvironm Pollut Guangzhou 510650 Guangdong Peoples R China;

    Hunan Normal Univ Natl &

    Local Joint Engn Lab New Petrochem Mat &

    F Changsha 410081 Hunan Peoples R China;

    Guangdong Inst Ecoenvironm Sci &

    Technol Guangdong Key Lab Integrated Agroenvironm Pollut Guangzhou 510650 Guangdong Peoples R China;

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  • 正文语种 eng
  • 中图分类 化学;
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