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重新审视溶解硅酸盐在含铁矿物催化过氧化氢过程中的作用。

Revisiting the Role of Dissolved Silicate in Catalyzing the Hydrogen Peroxide Process with Iron-Bearing Minerals.

作者信息

Qiu Yicheng, Sun Lingkai, Cui Jiaxin, Li Zijun, Zeng Xiang, Liu Yuxiao, Alshawabkeh Akram N, Mao Xuhui

机构信息

School of Resources and Environmental Science, Wuhan University, Wuhan 430079, China.

Changjiang Survey, Planning, Design and Research Co., Ltd., Wuhan 430010, China.

出版信息

ACS ES T Water. 2023 Oct 13;3(10):3200-3205. doi: 10.1021/acsestwater.2c00557. Epub 2023 Jun 21.

Abstract

Injecting HO into aquifers is a widely used chemical oxidation (ISCO) technology for groundwater remediation. Dissolved silicate was reported to decrease the reactivity of iron (Ⅲ)-bearing minerals toward HO. In this study, the effect of naturally occurring levels of dissolved silicate (≤1 mM) on the catalyzing hydrogen peroxide (CHP) with Fe(II) minerals is revaluated, and new observations that contradict with previous studies are reported. Specifically, dissolved silicate enhanced the CHP process by Fe(II) minerals. In the presence of Fe(II) minerals, siderite and ferrous oxide (FeO), which had a stronger dissolution tendency than Fe(III) minerals, dissolved silicate could prevent the dissolved iron species from precipitation through a coordinating effect, therefore reinforcing the homogeneous CHP process and the degradation of 2,4-dichlorophenol. The solution pH decreased due to the generation of degradation intermediates, and the solution acidification in turn promoted further dissolution of Fe(II) minerals. FeO particles exhibited the strongest silicate adsorption among the minerals, therefore a higher initial silicate concentration of 1 mM was needed to observe the enhancing effect. This study redefines the role of dissolved silicate on CHP process and provides clues to the design of efficient HO-based ISCO system for the remediation of groundwater.

摘要

向含水层中注入羟基自由基(HO)是一种广泛应用于地下水修复的化学氧化(ISCO)技术。据报道,溶解态硅酸盐会降低含铁(Ⅲ)矿物对HO的反应活性。在本研究中,重新评估了天然存在水平的溶解态硅酸盐(≤1 mM)对铁(Ⅱ)矿物催化过氧化氢(CHP)的影响,并报告了与先前研究相矛盾的新观察结果。具体而言,溶解态硅酸盐增强了铁(Ⅱ)矿物的CHP过程。在存在铁(Ⅱ)矿物、菱铁矿和氧化亚铁(FeO)(其溶解倾向比铁(Ⅲ)矿物更强)的情况下,溶解态硅酸盐可通过配位作用防止溶解态铁物种沉淀,从而加强均相CHP过程以及2,4-二氯苯酚的降解。由于降解中间体的生成,溶液pH值降低,而溶液酸化反过来又促进了铁(Ⅱ)矿物的进一步溶解。在这些矿物中,FeO颗粒对硅酸盐的吸附最强因此需要1 mM的较高初始硅酸盐浓度才能观察到增强效果。本研究重新定义了溶解态硅酸盐在CHP过程中的作用,并为设计高效的基于HO的ISCO系统用于地下水修复提供了线索。

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