Sustained activation of persulfate by slow release of Fe(II) from silica-coated nanosized zero-valent iron for in situ chemical oxidation

IF 11.4 1区环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Water Research Pub Date : 2023-11-01 DOI:10.1016/j.watres.2023.120715

Minjoo Song , Quoc Bien Nguyen , Cheolyong Kim , Inseong Hwang

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引用次数: 2

Abstract

Sustained activation of persulfate through the slow release of Fe(II) from silica-coated nanosized zero-valent iron (nZVI) particles (nZVI@SiO₂) was investigated. Slow release of Fe(II) prevented radical scavenging by excess Fe(II) and increased the radical yield, which improved the stoichiometric efficiency of phenol degradation. Sulfate and hydroxyl radicals were found to be the main oxidative species produced during phenol degradation and were found to make comparable contributions to oxidation. The nZVI@SiO₂ particle silica shell thickness controlled the release of Fe(II) and therefore the sustained activation of persulfate and was strongly affected by the synthesis conditions, including the [Si]/[Fe] ratio and silica supply rate. Optimal sustained phenol degradation was achieved when nZVI@SiO₂ particles were synthesized using a [Si]/[Fe] ratio of 0.5 and a tetraethyl orthosilicate supply rate of 0.5 mL/min, and this was attributed to the nZVI@SiO₂ particles giving an optimal Fe(II) release rate and therefore a high persulfate activation rate and a high phenol removal efficiency. Sustained persulfate activation induced by Fe(II) being slowly released was described well by single-stage first-order kinetics rather than two-stage first-order kinetics typical of unmodified nZVI/persulfate systems. Persulfate was found still to be activated by iron (oxyhydr)oxides minerals after the nZVI@SiO₂ particles had been exhausted but the persulfate sustained activation induced by the slow release of Fe(II) played a crucial role in determining the overall degradation efficiency. The results highlight the importance of the slow release of Fe(II) from nZVI-based materials for in situ chemical oxidation through sustained persulfate activation.

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通过从二氧化硅包覆的纳米零价铁中缓慢释放Fe（II）来持续活化过硫酸盐，用于原位化学氧化。

通过从二氧化硅包覆的纳米零价铁（nZVI）颗粒中缓慢释放Fe（II）来持续活化过硫酸盐(nZVI@SiO2)被调查。Fe（II）的缓慢释放阻止了过量的Fe（Ⅱ）对自由基的清除，并提高了自由基的产率，从而提高了苯酚降解的化学计量效率。硫酸盐和羟基自由基被发现是苯酚降解过程中产生的主要氧化物种，并且被发现对氧化有相当的贡献。这个nZVI@SiO2颗粒二氧化硅壳厚度控制了Fe（II）的释放，从而控制了过硫酸盐的持续活化，并受到合成条件的强烈影响，包括[Si]/[Fe]比和二氧化硅供应速率。当nZVI@SiO2使用[Si]/[Fe]比为0.5和正硅酸四乙酯供应速率为0.5mL/min合成颗粒，这归因于nZVI@SiO2颗粒提供最佳的Fe（II）释放速率，并因此提供高的过硫酸盐活化速率和高的苯酚去除效率。由缓慢释放的Fe（II）诱导的持续过硫酸盐活化通过单阶段一阶动力学而不是未改性的nZVI/过硫酸盐系统的典型的两阶段一阶动力来很好地描述。在nZVI@SiO2颗粒已经耗尽，但由Fe（II）的缓慢释放引起的过硫酸盐持续活化在决定整体降解效率方面起着至关重要的作用。研究结果强调了从基于nZVI的材料中缓慢释放Fe（II）对于通过持续的过硫酸盐活化进行原位化学氧化的重要性。

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来源期刊

Water Research 环境科学-工程：环境

CiteScore

20.80

自引率

9.40%

发文量

1307

审稿时长

38 days

期刊介绍： Water Research, along with its open access companion journal Water Research X, serves as a platform for publishing original research papers covering various aspects of the science and technology related to the anthropogenic water cycle, water quality, and its management worldwide. The audience targeted by the journal comprises biologists, chemical engineers, chemists, civil engineers, environmental engineers, limnologists, and microbiologists. The scope of the journal include: •Treatment processes for water and wastewaters (municipal, agricultural, industrial, and on-site treatment), including resource recovery and residuals management; •Urban hydrology including sewer systems, stormwater management, and green infrastructure; •Drinking water treatment and distribution; •Potable and non-potable water reuse; •Sanitation, public health, and risk assessment; •Anaerobic digestion, solid and hazardous waste management, including source characterization and the effects and control of leachates and gaseous emissions; •Contaminants (chemical, microbial, anthropogenic particles such as nanoparticles or microplastics) and related water quality sensing, monitoring, fate, and assessment; •Anthropogenic impacts on inland, tidal, coastal and urban waters, focusing on surface and ground waters, and point and non-point sources of pollution; •Environmental restoration, linked to surface water, groundwater and groundwater remediation; •Analysis of the interfaces between sediments and water, and between water and atmosphere, focusing specifically on anthropogenic impacts; •Mathematical modelling, systems analysis, machine learning, and beneficial use of big data related to the anthropogenic water cycle; •Socio-economic, policy, and regulations studies.