Homogeneous and Heterogeneous (Fex, Cr1-x)(OH)3 Precipitation: Implications for Cr Sequestration

Homogeneous and Heterogeneous (Fex, Cr1-x)(OH)3 Precipitation: Implications for Cr Sequestration
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DOI:
10.1021/acs.est.5b04319
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发表时间:
2016-02-16
影响因子:
11.4
通讯作者:
Hu, Yandi
Hu, Yandi
中科院分区:
环境科学与生态学1区
文献类型:
--
作者:
Dai, Chong;Zuo, Xiaobing;Hu, Yandi

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(Fe,Cr)(OH)(3)纳米颗粒的形成决定了水溶液中Cr在许多水环境中的命运。使用小角X射线散射,在pH = 3.7 +/-0.2下,从含有0- 0.25mM Cr(III)的0.1mM Fe(III)溶液中定量溶液中和石英上的(Fe,Cr)(OH)(3)纳米颗粒的沉淀速率。Cr(III)/Fe(III)浓度比控制了(Fe-x,Cr 1-x)(OH)(3)沉淀的化学组成(x)、溶液相对于沉淀的过饱和度和石英表面电荷。因此,水溶液中Cr(III)/Fe(III)的比例通过不同的机制影响(Fe-x,Cr 1-x)(OH)(3)的均匀(在溶液中)和非均匀(在石英上)沉淀速率。还研究了沉淀物中Cr(III)的螯合机理。在具有高含水Cr(III)/Fe(III)比率的溶液中,发生Cr(III)在沉淀物上的表面富集,导致溶液中的颗粒生长较慢。从0-0.1 mM Cr(III)的溶液中,石英上的颗粒在1 h内从2 nm生长到4 nm。有趣的是,从0.25 mM Cr(III)的溶液中,在石英上形成了两种不同尺寸(2和6 nm)的颗粒,并且它们的尺寸在整个反应过程中保持不变。我们的研究为(Fe-x,Cr 1-x)(OH)(3)纳米颗粒的均匀和非均匀沉淀提供了新的见解,这有助于确定Cr在水环境中的归宿。
The formation of (Fe, Cr)(OH)(3) nanoparticles determines the fate of aqueous Cr in many aquatic environments. Using small-angle X-ray scattering, precipitation rates of (Fe, Cr)(OH)(3) nanoparticles in solution and on quartz were quantified from 0.1 mM Fe(III) solutions containing 0-0.25 mM Cr(III) at pH = 3.7 +/- 0.2. Concentration ratio of aqueous Cr(III)/Fe(III) controlled the chemical composition (x) of (Fe-x, Cr1-x)(OH)(3) precipitates, solutions' supersaturation with respect to precipitates, and the surface charge of quartz. Therefore, the aqueous Cr(III)/Fe(III) ratio affected homogeneous (in solution) and heterogeneous (on quartz) precipitation rates of (Fe-x, Cr1-x)(OH)(3) through different mechanisms. The sequestration mechanisms of Cr(III) in precipitates were also investigated. In solutions with high aqueous Cr(III)/Fe(III) ratios, surface enrichment of Cr(III) on the precipitates occurred, resulting in slower particle growth in solutions. From solutions with 0-0.1 mM Cr(III), the particles on quartz grew from 2 to 4 nm within 1 h. Interestingly, from solution with 0.25 mM Cr(III), particles of two distinct sizes (2 and 6 nm) formed on quartz, and their sizes remained unchanged throughout the reaction. Our study provided new insights on homogeneous and heterogeneous precipitation of (Fe-x, Cr1-x)(OH)(3) nanoparticles, which can help determine the fate of Cr in aquatic environments.