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Uniform Mesoporous Amorphous Cobalt-Inherent Silicon Oxide as a Highly Active Heterogeneous Catalyst in the Activation of Peroxymonosulfate for Rapid Oxidation of 2,4-Dichlorophenol: The Important Role of Inherent Cobalt in the Catalytic Mechanism.均匀介孔非晶态钴负载氧化硅作为一种高活性多相催化剂用于活化过一硫酸盐快速氧化2,4-二氯苯酚:负载钴在催化机理中的重要作用
ACS Appl Mater Interfaces. 2020 Dec 23;12(51):57190-57206. doi: 10.1021/acsami.0c20341. Epub 2020 Dec 8.
2
Concentration-Dependent Enhancing Effect of Dissolved Silicate on the Oxidative Degradation of Sulfamethazine by Zero-Valent Iron under Aerobic Conditions.溶解态硅酸钠对有氧条件下零价铁氧化降解磺胺甲恶唑的浓度依赖性增强作用。
Environ Sci Technol. 2020 Jan 21;54(2):1242-1249. doi: 10.1021/acs.est.9b05904. Epub 2019 Dec 27.
3
A novel discovery of a heterogeneous Fenton-like system based on natural siderite: A wide range of pH values from 3 to 9.一种基于天然菱铁矿的新型均相类 Fenton 体系的发现:pH 值范围从 3 到 9。
Sci Total Environ. 2020 Jan 1;698:134293. doi: 10.1016/j.scitotenv.2019.134293. Epub 2019 Sep 4.
4
Disilicate-Assisted Iron Electrolysis for Sequential Fenton-Oxidation and Coagulation of Aqueous Contaminants.用于水污染物连续芬顿氧化和混凝的二硅酸盐辅助铁电解
Environ Sci Technol. 2017 Jul 18;51(14):8077-8084. doi: 10.1021/acs.est.7b01184. Epub 2017 Jun 29.
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Enhanced heterogeneous photo-Fenton process modified by magnetite and EDDS: BPA degradation.由磁铁矿和乙二胺二琥珀酸改性的强化非均相光芬顿过程:双酚A的降解
Environ Sci Pollut Res Int. 2017 Apr;24(11):10421-10429. doi: 10.1007/s11356-017-8728-8. Epub 2017 Mar 9.
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In-situ chemical oxidation: Principle and applications of peroxide and persulfate treatments in wastewater systems.原位化学氧化:过氧化物和过硫酸盐处理在废水系统中的原理和应用。
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Development of KMnO(4)-releasing composites for in situ chemical oxidation of TCE-contaminated groundwater.用于 TCE 污染地下水原位化学氧化的 KMnO(4)释放复合材料的开发。
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9
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10
Inhibitory effect of dissolved silica on H₂O₂ decomposition by iron(III) and manganese(IV) oxides: implications for H₂O₂-based in situ chemical oxidation.溶解态硅对铁(III)和锰(IV)氧化物分解 H₂O₂的抑制作用:对基于 H₂O₂的原位化学氧化的影响。
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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.

DOI:10.1021/acsestwater.2c00557
PMID:39371348
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11452147/
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。